u.s. department of energy’s initiatives for proliferation prevention in russia: results of...

U.S. Department of Energy’s Initiatives for Proliferation Prevention in Russia:

Results of Radioactive Liquid Waste Treatment Project, Year 2

Y. Pokhitonov, V. KamachevV.G. Khlopin Radium Institute, Russia

D. KelleyPacific Nuclear Solutions, USA

Purpose of Project

• IPP sponsored by DOE to engage Russian weapons scientists in peaceful use of existing and newly developed technologies (17 projects underway)

• DOE’s IPP program is a mechanism for U.S. private sector companies to enter Russian market: radwaste treatment

• Introduce USA environmental technology to weapons sector and seek joint technologies – first foreign firm

• Investigate solutions for Russia & USA liquid radwaste problems resulting from Cold War

• DOE compensates scientists to participate in program

• Long-term, commercialize project, employ scientists

Project Participants

• Russia– Russian State Atomic Energy Corporation (ROSATOM)– VG Khlopin Radium Institute (project manager)– Seversk (SCC ), Zheleznogorsk (MCC), Ozersk (MAYAK), Gatchyna– 90+ participants, 68 weapons scientists

• USA– Department of Energy (GIPP)– Argonne National Lab– Pacific Nuclear Solutions (project manager)

• International Science & Technology Center (ISTC)– Project administrator, Moscow

Polymer Technology

• Variety of polymers for all organic, oil and aqueous streams• Solidification of LLW, ILW & HLW• Packaging:

– Standard drums / B-25 box– Encapsulation in cement

• Disposal options:– Short term, intermediate term – Final storage– Incineration

• Advantages:– No special equipment, low cost to process / treat– High performance, long term stability, no degradation– Waste minimization: oil 2:1 or 3:1 bonding ratio (liquid : polymer)– Safe to use, safe for transport

Solidification Process

Experiments

• Stability (Differential Thermal Analysis)• Irradiation• Gas generation• Polymer solidification /capacity / evaporation• Encapsulation in cement

Differential Thermal AnalysisPolymers: N910, N930, N960Solidified samples with nitric acid and sodium nitrate possess high thermal stability

-8

-6

-4

-2

0

2

fact

um

wei

gh

t ch

ang

e (%

/°C

)

-100

-80

-60

-40

-20

0

20

wei

gh

t ch

ang

e (%

)

0 50 100 150 200 250 300 350 400 Temperature (°C)

910.002 ––––––– 930.001 – – – – 960.001 ––––– ·

Universal V4.4A TA Instruments

Irradiation Tests / Results

• Extensive irradiation testing conducted, required for ROSATOM certification

– Over 25 irradiation tests– All similar outcomes with China, USA tests

• All high dose rates• Cobalt 60 gamma irradiator• One example: nitric / organic solution, solidified

30 rad per second30 days = 77 M Rad+ 73 days = 270 M Rad

• Brittle, size reduction, no degradation / leaching• Conducted for gas generation tests

Irradiation Tests

Stability and IrradiationCobalt 60, gamma installation, dose rate 3.9·10⁶ grayN960 polymer, HNO₃, 1M, after irradiationN910 polymer, oil + TBP, after irradiation

Gas Generation Tests

• Tests required to determine fire and explosion safety conditions

• Tests carried out under static conditions in sealed glass ampoules

• N960 polymer + nitric solution: no changes in the solidification and no gas release

• N910 polymer + TBP / oil: variable results • Preliminary judgment: polymers are not gas

generators

Rate of gas release during irradiation of sample: N910 polymer + 50%-TBP / 50%-oil

-0,02

0,00

0,02

0,04

0,06

0,08

0,10

0,12

0,14

0,16

0,18

0,20

0 100 200 300 400 500 600 700 800 900 1000

Dose, Grx103

W, m

l/h

Characteristic (composition)

of wastesConditions of solidification

Results

Volume of waste used, ml

Amount of # 960 used, g

Amount of # 910 used, g

4232Sludge residue from the bottom of the apparatus (aqueous phase). U-80g., NaNO₃~ 200g, HNO₃-0,8 M/I

6 8 0,5Successfully

solidified

4231

Sludge residue from the top of the apparatus (occurrence of organic

phase is probable). U-80g., NaNO₃~ 200g, HNO₃-0,8 M/I. Very thick black

liquid.

6 8 0,5Successfully

solidified

4237

LL decontaminationg solution with low amounts of organic substances, U-153 g/l, NaNO₃~ 100-150g, HNO₃

2,5 M/I

12 8 0,5Successfully

solidified

4238

LL decontaminating solution with low amounts of organic substances. U-153 g/l, NaNO₃~ 100-150g, HNO₃

2,5 M/I

20 4 2Successfully

solidified

4125U-20 g, NaNO₃ 40g, HNO₃ 1,2 M/I.

There was a precipitate in the solution.

15 16 0,5Successfully

solidified

4283Uranium re-extracts. U-70g, HNO₃

0,07 M/I. 20 4 1Successfully

solidified

No

Relationship between the

mass of polymer and the mass of

liquid phase, Mp:Mj

Loss of weight after

aging samples,

during 21 days, %

Amount of water absorbed by samples after solidification during 21 days. (weight of water/1

gram solidified sample)

H₂O

1 2:1 33,7 All water has been absorbed by the sample



NaOH, 0,1M




HNO₃, 1,0M




Solidified sample after addition of waterSolution: HNO₃ 1,0MNo volumetric increase

Polymer Solidification/ Capacity / Evaporation: Conclusions

• Polymer technology is irreversible, liquid permanently immobilized in polymer matrix

• Advantage: direct application of polymer to waste without conditioning / additives

• Little or no volumetric increase in the process• Appreciable volume reduction through evaporation; no

measurement of water vapor• Polymers slow the evaporation process• Polymers are versatile, solidify aqueous / organic waste

of varying acidities, specific activities, suspensions and sludge types & salts

Encapsulation of Polymer Solidification

• Cementation tests at AREVA & Sellafield successfully completed, with 90% organic / 10% aqueous streams

• When aqueous is above 10%, new technique for encapsulation is required

• Encapsulation research underway:– additives to solidification– additives to cement– tests with inorganic materials encouraging

Conclusions

• Experiments conducted thus far provide greater understanding of polymer’s capabilities

• Validates the polymer’s application with ILW / HLW waste

• First actual project planned for 1st Q, 2011– ILW aqueous waste with some organic material

• Results of work 3 sub-sites will be presented in 2011

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