ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides

(Exotic Radionuclides from Accelerator WAstefor Science and Technology)

Dorothea Schumann PSI Villigen Switzerland

Overview

The ideaThe ideaDescription of PSI accelerator facilitiesDescription of PSI accelerator facilitiesConcept of ERAWASTConcept of ERAWASTCopper beam dumpCopper beam dumpGraphite targetsGraphite targetsLead targetsLead targetsSeparation techniquesSeparation techniquesSummary and OutlookSummary and Outlook

Application of exotic long-lived isotopes for several purposesCollaboration between

bull Nuclide production facilitiesbull Basic physics researchNuclear Structurebull Laser Spectrometry (RIMS) bull Nuclear Astrophysics bull Accelerator Mass Spectrometry (AMS) bull Pharmaceutical chemistry

Workshop at PSI in Nov 2006 (30 participants from 12 countries)

bull Accelerator waste with high beam dose available at PSIbull 590 MeV protons produce several spallation products in shieldings beam

dump and targetsbull Accelerator waste contains considerable amounts of long-lived exotic

radionuclides

The idea

Chemical separation necessary

Activated parts

BX2-Target Beam dumpand shielding(Beam Control 71 MeV protons)

BMA-Target Beam dump and shielding(Pion therapy station 590 MeV protons)

Target E beam dump and shielding(590 MeV protons)

Lead and Zirkalloy from theSINQ facility

MaterialsCopperBerylliumTungstenAluminiumCast ironStainless steelGraphiteLeadConcrete

1 Existing accelerator waste materialCopper beam dump irradiated at the 590-MeV proton beam station at PSI dismounted about 15 years ago26Al 59Ni 53Mn 60Fe 44Ti or others can be separatedother irradiated materials like carbon (10Be) stainless steel or concrete are also available

2 Target material from the SINQ facilityTwo irradiated lead targets from the spallation source are available Heavier isotopes like 182Hf or several rare earth elements (eg 146Sm several Dy isotopes) can be obtained In principle targets from the SINQ will be available every second year

3 Special irradiationsThe SINQ facility offers the possibility to irradiate materials with 590 MeV protons at special positions Tended experiments for isotope production can be offered

Concept of ERAWAST

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Overview

The ideaThe ideaDescription of PSI accelerator facilitiesDescription of PSI accelerator facilitiesConcept of ERAWASTConcept of ERAWASTCopper beam dumpCopper beam dumpGraphite targetsGraphite targetsLead targetsLead targetsSeparation techniquesSeparation techniquesSummary and OutlookSummary and Outlook

Application of exotic long-lived isotopes for several purposesCollaboration between

bull Nuclide production facilitiesbull Basic physics researchNuclear Structurebull Laser Spectrometry (RIMS) bull Nuclear Astrophysics bull Accelerator Mass Spectrometry (AMS) bull Pharmaceutical chemistry

Workshop at PSI in Nov 2006 (30 participants from 12 countries)

bull Accelerator waste with high beam dose available at PSIbull 590 MeV protons produce several spallation products in shieldings beam

dump and targetsbull Accelerator waste contains considerable amounts of long-lived exotic

radionuclides

The idea

Chemical separation necessary

Activated parts

BX2-Target Beam dumpand shielding(Beam Control 71 MeV protons)

BMA-Target Beam dump and shielding(Pion therapy station 590 MeV protons)

Target E beam dump and shielding(590 MeV protons)

Lead and Zirkalloy from theSINQ facility

MaterialsCopperBerylliumTungstenAluminiumCast ironStainless steelGraphiteLeadConcrete

1 Existing accelerator waste materialCopper beam dump irradiated at the 590-MeV proton beam station at PSI dismounted about 15 years ago26Al 59Ni 53Mn 60Fe 44Ti or others can be separatedother irradiated materials like carbon (10Be) stainless steel or concrete are also available

2 Target material from the SINQ facilityTwo irradiated lead targets from the spallation source are available Heavier isotopes like 182Hf or several rare earth elements (eg 146Sm several Dy isotopes) can be obtained In principle targets from the SINQ will be available every second year

3 Special irradiationsThe SINQ facility offers the possibility to irradiate materials with 590 MeV protons at special positions Tended experiments for isotope production can be offered

Concept of ERAWAST

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Application of exotic long-lived isotopes for several purposesCollaboration between

bull Nuclide production facilitiesbull Basic physics researchNuclear Structurebull Laser Spectrometry (RIMS) bull Nuclear Astrophysics bull Accelerator Mass Spectrometry (AMS) bull Pharmaceutical chemistry

Workshop at PSI in Nov 2006 (30 participants from 12 countries)

bull Accelerator waste with high beam dose available at PSIbull 590 MeV protons produce several spallation products in shieldings beam

dump and targetsbull Accelerator waste contains considerable amounts of long-lived exotic

radionuclides

The idea

Chemical separation necessary

Activated parts

BX2-Target Beam dumpand shielding(Beam Control 71 MeV protons)

BMA-Target Beam dump and shielding(Pion therapy station 590 MeV protons)

Target E beam dump and shielding(590 MeV protons)

Lead and Zirkalloy from theSINQ facility

MaterialsCopperBerylliumTungstenAluminiumCast ironStainless steelGraphiteLeadConcrete

1 Existing accelerator waste materialCopper beam dump irradiated at the 590-MeV proton beam station at PSI dismounted about 15 years ago26Al 59Ni 53Mn 60Fe 44Ti or others can be separatedother irradiated materials like carbon (10Be) stainless steel or concrete are also available

2 Target material from the SINQ facilityTwo irradiated lead targets from the spallation source are available Heavier isotopes like 182Hf or several rare earth elements (eg 146Sm several Dy isotopes) can be obtained In principle targets from the SINQ will be available every second year

3 Special irradiationsThe SINQ facility offers the possibility to irradiate materials with 590 MeV protons at special positions Tended experiments for isotope production can be offered

Concept of ERAWAST

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Activated parts

BX2-Target Beam dumpand shielding(Beam Control 71 MeV protons)

BMA-Target Beam dump and shielding(Pion therapy station 590 MeV protons)

Target E beam dump and shielding(590 MeV protons)

Lead and Zirkalloy from theSINQ facility

MaterialsCopperBerylliumTungstenAluminiumCast ironStainless steelGraphiteLeadConcrete

1 Existing accelerator waste materialCopper beam dump irradiated at the 590-MeV proton beam station at PSI dismounted about 15 years ago26Al 59Ni 53Mn 60Fe 44Ti or others can be separatedother irradiated materials like carbon (10Be) stainless steel or concrete are also available

2 Target material from the SINQ facilityTwo irradiated lead targets from the spallation source are available Heavier isotopes like 182Hf or several rare earth elements (eg 146Sm several Dy isotopes) can be obtained In principle targets from the SINQ will be available every second year

3 Special irradiationsThe SINQ facility offers the possibility to irradiate materials with 590 MeV protons at special positions Tended experiments for isotope production can be offered

Concept of ERAWAST

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

1 Existing accelerator waste materialCopper beam dump irradiated at the 590-MeV proton beam station at PSI dismounted about 15 years ago26Al 59Ni 53Mn 60Fe 44Ti or others can be separatedother irradiated materials like carbon (10Be) stainless steel or concrete are also available

2 Target material from the SINQ facilityTwo irradiated lead targets from the spallation source are available Heavier isotopes like 182Hf or several rare earth elements (eg 146Sm several Dy isotopes) can be obtained In principle targets from the SINQ will be available every second year

3 Special irradiationsThe SINQ facility offers the possibility to irradiate materials with 590 MeV protons at special positions Tended experiments for isotope production can be offered

Concept of ERAWAST

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Characteristics of the copper beam dump

Beam stop from the former BMA stationOperated from 1980-1992 dismounted in 199301 Ah total beam dose (590 MeV protons)copper cylinder of ~ 10 kg diameter 80mmSample taking from several parts by drillingCharacterization of the radionuclide inventory including radial and depth distribution

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Sample

44Ti[kBqg]

36Cl[Bqg]

63Ni[kBqg]

55Fe[kBqg]

60Fe[Bqg]

26Al[Bqg]

110mAg[Bqg]

108mAg[Bqg]

59Ni[Bqg]

53Mn[Bqg]

60Co[kBqg]

C611 48 406 2203 2336 0154 121 177 2240

C612 054 049 1337 373 0016 198 252 857

C621 16160 341511 424503 140 389 6258 6900 499571

C622 02 030 2177 1086 248 135 129 06 1116

C631 7408 365667 441363 56 23 3727 4310 379696

C632 186 20060 25620 33 1 0453 919 6620 112 26918

C633 15 11097 15524 19 02 132 922 2620 117 12394

C634 06 18416 2570 05 003 092 169 759 6 6632

C635 04 035 7062 1547 056 106 466 49 4388

C641 7781 167763 265904 41 164 2770 3600 472560

C642 024 7991 1325 009 127 21 5055

C651 950 57641 115204 202 3 1170 1364 998 100919

C652 027 5456 1578 059 180 422 20 4150

C661 - 013 10057 2876 0012 375 393 4590

C662 - 008 2332 1278 00019 049 094 1698

C671 - 008 1702 3507 14 134 1486

C672 - 004 1188 2336 00013 185 086 911

C673 - 004 01 00012 386 172 1 561

C674 - 004 00009 018 103 05 61

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

30 45 45 45 90 33

50

20

1 2 3 4 6 7

350

370

Beam80

(measures in mm)

5

Schematic view of the beam dump

- Area of drilling Oslash 20mm

Drilling of appr 500g of copper from the inner part containing about 80 of activity

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Estimation of available radionuclides(no separation)

44Ti 100 MBq53Mn 500 kBq (1019 atoms)26Al 7 kBq (1017 atoms)60Fe (50 kBq ndash 1018 atoms)59Ni (60Co 5 GBq)

All these radionuclides can be provided without carrier but some of them contain other long-lived isotopes (55Fe63Ni)

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Graphite targets

Myon production station (target E)Up to 20 of the proton beamTypical operation time 1-3 yearsSource for 7Be and 10BeOther radionuclides 14C 3H impurities of 22Na 54Mn 5760Co

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Results for 710Be

SampleSample 1010BeBe[Bqg][Bqg]

ICPICP--MSMS

1010BeBe[Bqg][Bqg]AMSAMS

Total Total amount of amount of

atomsatoms

Total Total amount in amount in

μμgg

77BeBe[Bqg][Bqg]EOBEOB

1a 220 67middot1016 16 -

23middot1011

15middot1011

84middot1010

1i 95

2a 291 316 84middot1016 14

2i 7

3a 506 495 65middot1016 11

4a 2049 10middot1018 167

beam doses 4 ndash 11 Ah

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Lead targets from SINQLead targets from SINQ

Proton beam

Sample positions

2 Samples from target 4 2 years operation EOB 1999

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

500 1000 1500 20000

1x106

172Lu102mRh

173Lu

172Lu

207Bi

172Lu

207Bi

coun

ts

Energy [keV]

194Au

172Lu

60Co

102mRh

Analytics

1780 1800 1820 18400

200

400

600

800

1000

1200

1400

1600

coun

ts

Energy [keV]

26Al

44Ti (63y) 80kBqg 194Hg(520y) 20MBqg60Co (5y) 4MBqg 1723LuHf (1914y) 30MBqg207Bi (3155y) 30MBqg

1100 1200 1300 1400 15000

1x104

2x104

3x104

coun

ts

Energy [MeV]

60Co

44Sc

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Examples for separation60Fe for determination of half-life with carrier 1015 atoms collaboration with TUM)60Fe for neutron capture carrier-free 1016 atoms collaboration with FZK44Ti for TiSc generator (radiopharmaceutical use) carrier-free 1 MBq collaboration with University Mainz44Ti probably for studies of core collapse supernovae carrier-free 35 MBq (collaboration with Uni Edinburgh)26Al with carrier standard material for AMS 10 Bq collaboration with ETH Zuumlrich26Al carrier-free laser spectrometry (RIMS) 1013 atoms collaboration with Uni Mainz10Be carrier-free radioactive ion beam 5μg collaboration with UCL10Be carrier-free laser spectrometry 1013 atoms collaboration with GSI

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Special Problem60Fe (15106 y) rarr 60mCo (105 min) rarr 60Co (53 y) rarr 60Ni (stable) 60Fe no γ radiation low βminusenergy Measurement of the increase of the Co-daughter rarr very goodchemical separation from Co necessary

Dissolution of 38g Cu (beam dump) in 7 M HNODissolution of 38g Cu (beam dump) in 7 M HNO33

Evaporation to drynessEvaporation to drynessDissolution in 7 M HClDissolution in 7 M HCl+ 5 mg Fe+ 5 mg Fe3+3+ and 5 mg Coand 5 mg Co2+2+ as carrieras carrierExtraction with Methylisobutylketone (MIBK) Extraction with Methylisobutylketone (MIBK) Aqueous phase Ni Co Cu organic phase FeAqueous phase Ni Co Cu organic phase FeBack Extraction with 01 M HCl repetition of procedureBack Extraction with 01 M HCl repetition of procedureAdditional purification by precipitation of Fe(OH)Additional purification by precipitation of Fe(OH)33

Result Result ~ 10~ 101515 6060Fe atoms decontamination factor Fe atoms decontamination factor (Co) lt 10(Co) lt 10--77

Chemical separation of Chemical separation of 6060FeFe

β- γβ-γ

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Chemical separation of Chemical separation of 4444TiTibull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 44Ti and othersbull Carrier free required

Fe(OH)3+Ti(OH)4+60Co

Dissolution In 7 M HCl

DOWEX1x8Adsorption of FeElution of Ti

DOWEX1x8Adsorption of TiRinsing with 1 MHF (for removalof 60Co)Elution of Ti with1 M HNO3

Evaporation to drynessFuming with conc HFDissolution in 1 M HF

Result~ 45 MBq 44TiDecontaminationFactor 60Colt10-6

7 M HCl-solution +Fe3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(95)

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Chemical separation of Chemical separation of 2626AlAlbull Aliquot from the remaining solution of the

Fe-separation (500 ml 7 M HCl)bull Contains Cu 60Co 26Al and othersbull With carrier required

Al(OH)3+60Co

DOWEX50x8Adsorption of AlElution of Al with4 M Cl

Result~ 10 Bq 26Al=1014 atomsDecontaminationFactor 60Colt10-6

7 M HCl-solution +Al3+ + NH3

Cu(NH3)42+Co(NH3)4

2+(40-60)

+Co2+ + 5 M NaOH

Co(OH)2Al(OH)4

-

Al(OH)3

+HCl

Dissolution in 01M HNO3

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Chemical separation of Chemical separation of 1010BeBebull Graphite of Target E contains mainly 14C

3H 10Be (7Be - decayed)bull 10B as the stable isobaric isotope of 10Be has

to be separated nearly completelybull Carrier (stable 9Be) not suitable for

radioactive beam

N2

Ba(OH)2

14g graphite7Be as tracer

HNO3HClO4H2SO4

Fe(OH)3+Be(OH)2 Filtration+Fe3+ +NH3Dissolution

In 7 M HCl

DOWEX1x8Adsorption of FeElution of Be

DOWEX50x8Adsorption of BeRinsing with 01 MHNO3 (for removalof boron)Elution of Be with4 M HCl

Evaporation to drynessDissolution in 01 M HNO3

Result~ 16μg 10Be = 11018 atoms

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook

Summary and OutlookCu- and C-samples available Work on Pb-targets ongoing1015-17 atoms of several radionuclides (26Al 60Fe 44Ti) separated and availableUp to 1018 atoms of 10Be separated and availablePossibilities for other irradiation positions (SINQ beam dumps collimators)ESF-funded Research-Network-Program launchedNext step Automated system for stepwise separation of big amounts of radionuclides from copper and carbon in a hotcell or gloveboxDevelopment of a similar system for the lead targetsRoutine production facility

• ERAWAST ndash a New Production Route for Exotic Long-lived Radionuclides(Exotic Radionuclides from Accelerator WAste for Science
• Overview
• The idea
• Concept of ERAWAST
• Characteristics of the copper beam dump
• Estimation of available radionuclides(no separation)
• Graphite targets
• Results for 710Be
• Analytics
• Examples for separation
• Summary and Outlook