Au/CeO2催化剂上CO2选择加氢为CO反应及其中间物种研究

CO_2的化学转化具有环境及科学双重研究意义.CO_2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO_2选择性还原为CO,即逆水汽变换（RWGS）反应（CO_2＋H_2→CO＋H_2O）,具有重要的理论意义和应用价值：（1）CO作为合成气的重要原料,可以通过F-T合成生产更有价值的液体燃料;（2）H_2可通过可再生能源电解水制取,实现了全过程的零排放碳循环利用.从热力学角度分析,RWGS反应是一个吸热反应,高温有利于平衡转化率的提高.从动力学角度,一个对正反应有活性的催化剂可同时催化逆反应进行.可还原性载体负载贵金属催化剂,如Pt/Ce O_2,Au/Fe Ox,Au/Ce O...

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Published in催化学报 Vol. 37; no. 12; pp. 2053 - 2058
Main Author 朱晓兵 曲新 李小松 刘景林 刘剑豪 朱斌 石川
Format Journal Article
LanguageChinese
Published 等离子体物理化学实验室,辽宁大连 116024 2016
大连理工大学氢能与液体燃料研究中心
Subjects
Au/CeO2催化剂
一氧化碳
二氧化碳还原
原位红外漫反射光谱
甲酸盐中间物种
一氧化碳
甲酸盐中间物种
Formate intermediate
Au/CeO2 catalyst
原位红外漫反射光谱
In situ DRIFT spectroscopy
Carbon monoxide
CO2 reduction
二氧化碳还原
Au/CeO2催化剂
Online AccessGet full text
ISSN0253-9837
1872-2067
DOI10.1016/S1872-2067(16)62538-X

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Abstract CO_2的化学转化具有环境及科学双重研究意义.CO_2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO_2选择性还原为CO,即逆水汽变换（RWGS）反应（CO_2＋H_2→CO＋H_2O）,具有重要的理论意义和应用价值：（1）CO作为合成气的重要原料,可以通过F-T合成生产更有价值的液体燃料;（2）H_2可通过可再生能源电解水制取,实现了全过程的零排放碳循环利用.从热力学角度分析,RWGS反应是一个吸热反应,高温有利于平衡转化率的提高.从动力学角度,一个对正反应有活性的催化剂可同时催化逆反应进行.可还原性载体负载贵金属催化剂,如Pt/Ce O_2,Au/Fe Ox,Au/Ce O_2等,具有很好的低温WGS催化活性,但它们在RWGS反应上的研究较少.我们制备了Ce O_2负载纳米Au催化剂（HRTEM表征结果表明金高度分散于Ce O_2载体表面,粒径为4–5 nm）,其在常压CO2加氢还原为CO反应中表现出优异的低温活性,分别在450℃,CO2/H2=1,WHSV=12000 m L/（h·g）,及400℃,H2/CO2=1,WHSV=6000 m L/（h·g）条件下,CO2转化率接近平衡转化率,且CO的选择性为100%.随着H2/CO2比例增加,CO2转化率明显提高,且维持H2/CO2为1的化学计量比反应.通过原位漫反射红外光谱与质谱相结合的技术,研究了Au/CeO2催化剂上的RWGS反应路径：Au/CeO2催化剂表面形成了甲酸盐中间物种,它的消耗伴随着CO和H2O产物的生成.说明Au/CeO2催化剂遵循中间体机理,这应该是其具有优异低温RWGS反应性能的微观机制.
AbstractList CO2的化学转化具有环境及科学双重研究意义.CO2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO2选择性还原为CO,即逆水汽变换(RWGS)反应(CO2+H2→CO+H2O),具有重要的理论意义和应用价值:(1)CO作为合成气的重要原料,可以通过F-T合成生产更有价值的液体燃料;(2)H2可通过可再生能源电解水制取,实现了全过程的零排放碳循环利用.从热力学角度分析,RWGS反应是一个吸热反应,高温有利于平衡转化率的提高.从动力学角度,一个对正反应有活性的催化剂可同时催化逆反应进行.可还原性载体负载贵金属催化剂,如Pt/CeO2,Au/FeOx,Au/CeO2等,具有很好的低温WGS催化活性,但它们在RWGS反应上的研究较少.我们制备了CeO2负载纳米Au催化剂(HRTEM表征结果表明金高度分散于CeO2载体表面,粒径为4-5 nm),其在常压CO2加氢还原为CO反应中表现出优异的低温活性,分别在450℃,CO2/H2=1,WHSV=12000 mL/(h·g),及400℃,H2/CO2=1,WHSV=6000 mL/(h·g)条件下,CO2转化率接近平衡转化率,且CO的选择性为100%.随着H2/CO2比例增加,CO2转化率明显提高,且维持H2/CO2为1的化学计量比反应.通过原位漫反射红外光谱与质谱相结合的技术,研究了Au/CeO2催化剂上的RWGS反应路径:Au/CeO2催化剂表面形成了甲酸盐中间物种,它的消耗伴随着CO和H2O产物的生成.说明Au/CeO2催化剂遵循中间体机理,这应该是其具有优异低温RWGS反应性能的微观机制.
CO_2的化学转化具有环境及科学双重研究意义.CO_2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO_2选择性还原为CO,即逆水汽变换（RWGS）反应（CO_2＋H_2→CO＋H_2O）,具有重要的理论意义和应用价值：（1）CO作为合成气的重要原料,可以通过F-T合成生产更有价值的液体燃料;（2）H_2可通过可再生能源电解水制取,实现了全过程的零排放碳循环利用.从热力学角度分析,RWGS反应是一个吸热反应,高温有利于平衡转化率的提高.从动力学角度,一个对正反应有活性的催化剂可同时催化逆反应进行.可还原性载体负载贵金属催化剂,如Pt/Ce O_2,Au/Fe Ox,Au/Ce O_2等,具有很好的低温WGS催化活性,但它们在RWGS反应上的研究较少.我们制备了Ce O_2负载纳米Au催化剂（HRTEM表征结果表明金高度分散于Ce O_2载体表面,粒径为4–5 nm）,其在常压CO2加氢还原为CO反应中表现出优异的低温活性,分别在450℃,CO2/H2=1,WHSV=12000 m L/（h·g）,及400℃,H2/CO2=1,WHSV=6000 m L/（h·g）条件下,CO2转化率接近平衡转化率,且CO的选择性为100%.随着H2/CO2比例增加,CO2转化率明显提高,且维持H2/CO2为1的化学计量比反应.通过原位漫反射红外光谱与质谱相结合的技术,研究了Au/CeO2催化剂上的RWGS反应路径：Au/CeO2催化剂表面形成了甲酸盐中间物种,它的消耗伴随着CO和H2O产物的生成.说明Au/CeO2催化剂遵循中间体机理,这应该是其具有优异低温RWGS反应性能的微观机制.
Abstract_FL CO2 selective reduction to CO with H2 over a CeO2-supported nano-Au catalyst at atmospheric pres-sure was investigated. A high CO2 conversion, approaching the thermodynamic equilibrium value, and nearly 100% CO selectivity were obtained. The surface formate intermediates generated during the reverse water-gas shift reaction at 400 ℃ were identified using in situ diffuse-reflectance infra-red Fourier-transform spectroscopy. The formate consumption to give CO and H2O, determined using mass spectrometry, indicated that the reaction proceeded via an associative formate mecha-nism; this contributes to the high Au/CeO2 catalytic activity at low temperatures.
Author 朱晓兵 曲新 李小松 刘景林 刘剑豪 朱斌 石川
AuthorAffiliation 大连理工大学氢能与液体燃料研究中心；等离子体物理化学实验室,辽宁大连116024
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Author_FL Chuan Shi
Xin Qu
Xiaobing Zhu
Jinglin Liu
Jianhao Liu
Xiaosong Li
Bin Zhu
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DocumentTitleAlternate Selective reduction of carbon dioxide to carbon monoxide over Au/CeO2 catalyst and identification of reaction intermediate
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Issue 12
Keywords 一氧化碳
甲酸盐中间物种
Formate intermediate
Au/CeO2 catalyst
原位红外漫反射光谱
In situ DRIFT spectroscopy
Carbon monoxide
CO2 reduction
二氧化碳还原
Au/CeO2催化剂
Language Chinese
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Notes Xiaobing Zhu, Xin Qu, Xiaosong Li, Jinglin Liu, Jianhao Liu, Bin Zhu, Chuan Shi （ Center for Hydrogen Energy and Liquid Fuels; Laboratory of Plasma Physical Chemistry, Dalian University of Technology, Dalian 116024, Liaoning, China）
21-1195/O6
CO2 reductionAu/CeO2 catalystCarbon monoxide Formate intermediate In situ DRIFT spectroscopy
CO2 selective reduction to CO with H2 over a CeO2-supported nano-Au catalyst at atmospheric pres- sure was investigated. A high CO2 conversion, approaching the thermodynamic equilibrium value, and nearly 100% CO selectivity were obtained. The surface formate intermediates generated during the reverse water-gas shift reaction at 400 ℃ were identified using in situ diffuse-reflectance infra- red Fourier-transform spectroscopy. The formate consumption to give CO and H20, determined using mass spectrometry, indicated that the reaction proceeded via an associative formate mecha- nism; this contributes to the high Au/CeO2 catalytic activity at low temperatures.
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PublicationYear 2016
Publisher 等离子体物理化学实验室,辽宁大连 116024
大连理工大学氢能与液体燃料研究中心
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Snippet CO_2的化学转化具有环境及科学双重研究意义.CO_2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO_2选择性还原为CO,即逆水汽变换（RWGS）反...
CO2的化学转化具有环境及科学双重研究意义.CO2具有很高的化学稳定性,加氢还原是一种有效的转化途径.其中将CO2选择性还原为CO,即逆水汽变换(RWGS)反应(CO2+H2→CO+H2O),具有...
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StartPage 2053
SubjectTerms Au/CeO2催化剂
一氧化碳
二氧化碳还原
原位红外漫反射光谱
甲酸盐中间物种
Title Au/CeO2催化剂上CO2选择加氢为CO反应及其中间物种研究
URI http://lib.cqvip.com/qk/93027X/201612/671069690.html
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Volume 37
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