li yanping 20130728 讨论制备方法对光催化剂 cuo/tio 2 活性的影响. recent experimental...
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Li Yanping20130728
讨论制备方法对光催化剂CuO/TiO2活性的影响
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Recent experimental summary
Other researchers’ reports
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Other researchers’ reports
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1.Fabrication and comparison of highly efficient Cu incorporated TiO2 photocatalyst for hydrogen generation from water
Efficient Cu incorporated TiO2 photocatalysts for hydrogen generation were fabricated by four methods: in situ sol-gel, wet impregnation, chemical reduction of Cu salt, and in situ photo-deposition.
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Characteristics:
different chemical states of Cu
different distribution ratio of Cu between surface and bulk phases of the photocatalyst
the Cu content in the photocatalyst play a significant role in hydrogen generation
Conclusion:situ sol-gel method exhibited the highest stability
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It was discovered that the fabrication methods determined: the chemical state of Cu,
distribution ratio of Cu within the photocatalyst, BET surface area of thecatalyst,
crystal structure of the TiO2support.
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2. Wu and Lee reported that Cu doping within the TiO2
lattice had a negative effect on photocatalytic hydrogen generation as opposed to Cu deposition.
Wu NL, Lee MS. Enhanced TiO2photocatalysis by Cu in hydrogen production from aqueous methanol solution. Int J Hydrog Energy 2004;29:1601-5.
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3. Boccuzzi et al. compared properties and activity ofCu-TiO2 prepared by wet impregnation and chemisorption hydrolysis methods, and found that samples with the samechemical composition exhibited a marked difference of up to 100 times in the hydrogenation of 1,3-cyclooctadiene.
Boccuzzi F, Chiorino A, Gargano M, Ravasio N. Preparation,characterization, and activity of Cu/TiO2catalysts. 2. Effect of the catalyst morphology on the hydrogenation of 1,3-cyclooctadiene and the CO-NO reaction on Cu/TiO2 catalysts. J Catal 1997;165:140-9.
Boccuzzi F, Chiorino A, Martra G, Gargano M, Ravasio N,Carrozzini B. Preparation, characterization, and activity of Cu/TiO2catalysts. 1. Influence of the preparation method onthe dispersion of copper in Cu/TiO2. J Catal 1997;165:129-39.
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Recent experimental summary
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1.Different preparation methods of CuO/TiO2catalysts
1.1 The activity of catalyst
3155.72667
2353.47316
1996.899771827.822031821.91958
1280.63688
355.77204
Chemical adsorption Composite precipitation Ethanol immersion Simple wet impregnation Second impregnation Sol-gel Pure P25
0
500
1000
1500
2000
2500
3000
Hyd
rog
en
Pro
du
ctio
n r
ate
(μ
mo
l/(g
.h))
different methods of CuO-TiO2 photocatalyst (15)
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0 2 4 6 8 10 12 14 160
500
1000
1500
2000
2500
3000
Hyd
rog
en
Pro
du
ctio
n r
ate
(μ
mo
l/(g
.h))
Time (h)
Chemical adsorption2674.44
1460.30
1.2The stability of the catalystsThe stability of the chemical adsorption
54.6%
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Ethanol immersion
0 2 4 6 8 10 12 14 16 180
200
400
600
800
1000
1200
1400
1600
1800
2000H
ydro
ge
n P
rod
uct
ion
ra
te (
μm
ol/(
g.h
))
Time (h)
1609.41
1125.29
69.9%
The stability of the ethanol impregnation
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0 2 4 6 8 10 12 14 16 18-0.50
-0.45
-0.40
-0.35
-0.30
-0.25
-0.20
-0.15
-0.10
-0.05
0.00
activ
ity d
eclin
e (%
)
Time (h)
Chemical adsorption
0 2 4 6 8 10 12 14 16 18-0.50
-0.45
-0.40
-0.35
-0.30
-0.25
-0.20
-0.15
-0.10
-0.05
0.00
activ
ity d
eclin
e (%
)
Time (h)
Ethanol immersion
-0.45
-0.3
Activity decline: x-initial initial
活性 1.34倍,下降 1.5倍
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0 200 400 600 800 1000
0.01
0.00
-0.01
-0.02
-0.03
-0.04
Con
sum
ptio
n of
H2
(a.u
.)
temperature ( )℃
Ethanol impregnation
0 200 400 600 800 10000.01
0.00
-0.01
-0.02
-0.03
-0.04
-0.05
-0.06
-0.07
Con
sum
ptio
n of
H2
(a.u
.)
temperature ( )℃
chemical adsorption decomposition
H2-TPR
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1.3BET data of the catalystsPore distribution of the catalyst
1 10 100-0.1
0.0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
dV/dD
(cm
3/(g
.nm))
Pore Diameter (nm)
simple wet impregnation
1 10 100
0.000
0.002
0.004
0.006
0.008
0.010
dV/dD
(cm
3/(g
.nm))
Pore Diameter (nm)
Second impregnation
1 10 100
0.000
0.001
0.002
0.003
0.004
0.005
0.006
dV/dD
(cm
3 /(g.nm
))
Pore Diameter (nm)
Ethanol impregnation
26nm 2nm,31nm
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1 10 100
0.000
0.001
0.002
0.003
0.004
0.005
0.006
0.007
dV/dD
(cm
3 /(g.nm
))
Pore Diameter (nm)
Composite precipitation
1 10 100
0.00
0.02
0.04
0.06
0.08
0.10
0.12
dV/dD
(cm3 /(g
.nm))
Pore Diameter (nm)
sol-gel
1 10 100
0.000
0.001
0.002
0.003
0.004
0.005
0.006
0.007
dV/dD
(cm
3/(g
.nm))
Pore Diameter (nm)
chemical adsorption
3.9nm
3nm,33nm
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2% CuO/TiO2 SBET
(m2/g)Pore
diameter(nm)
Pore volume(cm3/g)
Chemical adsorption
46.8 29.0 0.326
Composite deposition
47.2 33.3 0.372
Ethanol impregnation
46.9 31.8 0.370
Sol-gel 92.0 3.9 0.137Simple wet
impregnation45.6 26.3 0.344
Second impregnation
44.9 25.9 0.322
Specific surface area,pore diameter and pore volume of the catalysts
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0.0 0.2 0.4 0.6 0.8 1.0
0
50
100
150
200
250
Volu
ne A
dsor
bed
(cm
3 STP
/g)
Relative Pressure (P/PO)
chemical adsorption
0.0 0.2 0.4 0.6 0.8 1.0
10
20
30
40
50
60
70
80
90
Volu
ne A
dsor
bed
(cm
3 S
TP/g
)
Relative Pressure (P/PO)
sol-gel
N2 adsorption stripping curve
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H2-TPR
0 200 400 600 800 1000
0.01
0.00
-0.01
-0.02
-0.03
-0.04
Consu
mption
of H2
(a.u.)
temperature ( )℃
simple wet impregnation
0 200 400 600 800
0.000
-0.005
-0.010
-0.015
-0.020
-0.025
-0.030
Consu
mption
of H2
(a.u.)
temperature ( )℃
second impregnation
0 200 400 600 800 1000
0.01
0.00
-0.01
-0.02
-0.03
-0.04
Cons
umpti
on of
H2 (
a.u.)
temperature ( )℃
Ethanol impregnation
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0 200 400 600 800 1000
0.02
0.00
-0.02
-0.04
-0.06
-0.08
-0.10
-0.12
Consu
mption
of H2
(a.u.)
temperature ( )℃
composite precipitation
0 200 400 600 800 10000.005
0.000
-0.005
-0.010
-0.015
-0.020
-0.025
Consu
mption
of H2
(a.u.)
temperature ( )℃
sol-gel
0 200 400 600 800 10000.01
0.00
-0.01
-0.02
-0.03
-0.04
-0.05
-0.06
-0.07
Consu
mption
of H2
(a.u.
)
temperature ( )℃
chemical adsorption decomposition
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200 300 400 500 600 700 800-0.1
0.0
0.1
0.2
0.3
0.4
0.5
0.6
Ab
so
rbe
nce
(a
.u.)
Wavalength (nm)
P25 simple wet impregnation second impregnation ethanol impregnation composite precipitation chemical adsorption sol-gel
Uv-vis
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Plasmonic photocatalysis(Ag/SiO2core –shell, TiO2)Reason:TiO2,3.2eV, near UV irradiation can excite pairs of electrons and holes Ag NPs , a very intense LSP absorption band in the near-UV a considerable enhancement of the electric near-field in the vicinity of the Ag NPsenhanced near-field could boost the excitation of electron –hole pairsBut, Ag NPs, would be oxidized at direct contactwith TiO2
A Plasmonic Photocatalyst Consisting of Silver Nanoparticles Embedded in Titanium Dioxide
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To prevent this oxidation, Ag NPs have to be coated with a passive material, such as SiO2, to separate them from TiO2.
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Thanks