核电用超疏水消氢Pt-Pd/Al_2O_3催化剂的研究
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摘要
为解决核电安全事故下大量氢气泄露所带来的爆炸威胁,研究了一种新型超疏水消氢催化剂。结果表明:合金催化剂较单质催化剂拥有更好的消氢性能,并且对水和杂质碘也有更好的抗性。经疏水改性的Pt_(0.5)Pd_(0.5)催化剂,可以很好的应对模拟核电严重事故下的氢气消除。随着反应的进行,在25 min后,氢气转化率可以达到近乎100%。疏水改性的Pt_(0.5)Pd_(0.5)合金催化剂在核电安全消氢领域有着良好的应用前景。
In the case of a severe accident in a nuclear plant,a large amount of hydrogen is released in nuclear power plant containment.The high hydrogen concentrations in local areas could result in a threat to containment integrity.For converting the hydrogen into water,supported noble catalysts were studied as an effective hydrogen mitigation system in this paper.Compared with monometallic catalysts,bimetal catalysts(Pt and Pd)exhibit better activity and resistance towards poisoning of both water and fission products.In addition,hydrophobic modification greatly weakens the delayed response of start-up for hydrogen oxidation under humid conditions at low temperatures.The conversion of hydrogen was almost 100%after 25 min.The channel plate reactor with superhydrophobic catalyst(modified Pt_(0.5)Pd_(0.5))coatings shows great potential for conversion of released hydrogen into water in a nuclear plant.
In the case of a severe accident in a nuclear plant,a large amount of hydrogen is released in nuclear power plant containment.The high hydrogen concentrations in local areas could result in a threat to containment integrity.For converting the hydrogen into water,supported noble catalysts were studied as an effective hydrogen mitigation system in this paper.Compared with monometallic catalysts,bimetal catalysts(Pt and Pd)exhibit better activity and resistance towards poisoning of both water and fission products.In addition,hydrophobic modification greatly weakens the delayed response of start-up for hydrogen oxidation under humid conditions at low temperatures.The conversion of hydrogen was almost 100%after 25 min.The channel plate reactor with superhydrophobic catalyst(modified Pt_(0.5)Pd_(0.5))coatings shows great potential for conversion of released hydrogen into water in a nuclear plant.
引文
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[18]Yu XH,Li HL,Tu ST,Yan JY,Wang ZD.Pt-Co catalyst coated channel plate reactor for preferential CO oxidation[J].International Journal of Hydrogen Energy,2011;36:3778-88.
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[20]Xu J,Ouyang L,Da G J,et al.Pt promotional effects on Pd-Pt alloy catalysts for hydrogen peroxide synthesis directly from hydrogen and oxygen[J].Journal of Catalysis,2012,285(1):74-82.
[21]Kim Y,Noh Y,Lim E,et al.Star-shaped Pd@Pt core-shell catalysts supported on reduced graphene oxide with superior electrocatalytic performance[J].Journal of Materials Chemistry A,2014,2(19):6976-86.
[22]Fang H,Gao JF,Wang HT,Chen CS.Hydrophobic porous alumina hollow fiber for water desalination via membrane distillation process[J].Journal of Membrane Science,2012,403-404(6):41-46.
[2]彭华清,汪伟,唐华雄,等.核电厂乏燃料水池液位、温度测量装置的设计与应用探讨[J].核科学与工程,2011(S2):25-29.
[3]钟昊良.核电厂乏燃料水池非能动喷淋冷却技术研究[D].华北电力大学,2015.
[4]Payot F,Reinecke E A,Morfin F,et al.Understanding of the operation behaviour of a Passive Autocatalytic Recombiner(PAR)for hydrogen mitigation in realistic containment conditions during a severe Light Water nuclear Reactor(LWR)accident[J].Nuclear Engineering&Design,2012,248(1):178-96.
[5]Lalik E,Kosydar R,Tokarz-Sobieraj R,et al.Humidity induced deactivation of Al2O3,and SiO2,supported Pd,Pt,Pd-Pt catalysts in H2+O2,recombination reaction:The catalytic,microcalorimetric and DFT studies[J].Applied Catalysis A General,2015,501:27-40.
[6]Ledjeff K.Elimination of hydrogen or oxygen from explosive mixtures by catalytic techniques[J].International Journal of Hydrogen Energy,1987,12(5):361-67.
[7]Deng J,Cao X W.A study on evaluating a passive autocatalytic recombiner PAR-system in the PWR large-dry containment[J].Nuclear Engineering&Design,2008,238(10):2554-60.
[8]张应超,季松涛,魏严凇,等.用MELCOR程序分析600 MWe核电厂乏燃料水池失去厂内外电源严重事故[J].原子能科学技术,2016,50(3):440-45.
[9]肖建军,周志伟,经荥清.核电站安全壳内氢气扩散和燃烧的分析程序GASFLOW及其应用[J].核科学与工程,2005,25(4):317-21.
[10]Belapurkar A D,Gupta N M.A hydrophobic catalyst for recombining H2/D2 and O2 in nuclear reactors[J].Power Plant Chemistry,2000,2(8):452-55.
[11]Pai M R,Varma S,Belapurkar A D,et al.Development of catalysts for mitigation of hydrogen in water cooled nuclear power reactors.Part 1.Preparation,characterization,and activity measurements[J].Power Plant Chemistry,2001,3(8):453-57.
[12]Pai M R,Varma S,Belapurkar A D,et al.Development of catalysts for the mitigation of hydrogen in water cooled nuclear power reactors.Part 2.Poisoning characteristics[J].Power Plant Chemistry,2001,3(9):518-21.
[13]Belapurkar A D,Varma S,Shirole A,et al.Cordieritesupported platinum catalyst for hydrogen-oxygen recombination for use in nuclear reactors under LOCA[J].Power Plant Chemistry,2008,10(8):461-67.
[14]Morfin F,Sabroux J C,Renouprez A.Catalytic combustion of hydrogen for mitigating hydrogen risk in case of a severe accident in a nuclear power plant:study of catalysts poisoning in a representative atmosphere[J].Applied Catalysis B:Environmental,2004,47(1):47-58.
[15]Miwa S,Yamashita S,Osaka M.Prediction of the effects of boron release kinetics on the vapor species of cesium and iodine fission products[J].Progress in Nuclear Energy,2016.
[16]Lalik E,Drelinkiewicz A,Kosydar R,et al.A role of Au-content in performance of Pd-Au/SiO2 and Pd-Au/Al2O3 catalyst in the hydrogen and oxygen recombination reaction.The microcalorimetric and DFTstudies[J].Applied Catalysis A:General,2016,517:196-210.
[17]Lalik E,Drelinkiewicz A,Kosydar R,et al.Activity and deactivation of Pd/Al2O3 catalysts in hydrogen and oxygen recombination reaction;a role of alkali(Li,Cs)dopant[J].International Journal of Hydrogen Energy,2015,40(46):16127-36.
[18]Yu XH,Li HL,Tu ST,Yan JY,Wang ZD.Pt-Co catalyst coated channel plate reactor for preferential CO oxidation[J].International Journal of Hydrogen Energy,2011;36:3778-88.
[19]Yu W,Tao J,Yu X,et al.A microreactor with superhydrophobic Pt-Al2O3 catalyst coating concerning oxidation of hydrogen off-gas from fuel cell[J].Applied Energy,2016.
[20]Xu J,Ouyang L,Da G J,et al.Pt promotional effects on Pd-Pt alloy catalysts for hydrogen peroxide synthesis directly from hydrogen and oxygen[J].Journal of Catalysis,2012,285(1):74-82.
[21]Kim Y,Noh Y,Lim E,et al.Star-shaped Pd@Pt core-shell catalysts supported on reduced graphene oxide with superior electrocatalytic performance[J].Journal of Materials Chemistry A,2014,2(19):6976-86.
[22]Fang H,Gao JF,Wang HT,Chen CS.Hydrophobic porous alumina hollow fiber for water desalination via membrane distillation process[J].Journal of Membrane Science,2012,403-404(6):41-46.