低碳化学与化工2024，Vol.49Issue(11)：21-27,7.DOI:10.12434/j.issn.2097-2547.20240079
Sn助剂调控Co/ZrO2催化剂用于CO2选择性加氢制CO
Selective hydrogenation of CO2 to CO over Co/ZrO2 catalysts regulated by Sn promoter
摘要
Abstract
The conversion of CO2 to CO via reverse water gas transformation(RWGS)reaction can present a promising strategy to mitigate the environmental impact of CO2 emission.However,the RWGS reaction encounters notable challenges,such as the efficient activation of CO2 and the suppressed generation of CH4.Different doping contents(mass fractions,the same below)of Sn were introduced into 5Co/ZrO2(Co mass fraction of 5％)for modification,and 5CoxSn/ZrO2(x=1,3 or 5,corresponding to Sn doping content of 1％,3％or 5％)catalysts were prepared.The experimental parameters for evaluating the catalytic performances of 5Co/ZrO2 and 5CoxSn/ZrO2 in CO2 hydrogenation reaction were adjusted and screened to explore the influence of Sn additives on the active components and catalytic performance.Among them,5Co5Sn/ZrO2 shows the best RWGS catalytic performance.After pre-reduction for 2 h at 600 ℃,under reaction conditions of temperature of 500 ℃,pressure of 0.1 MPa and space velocity of 36000 mL/(g·h),the CO2 conversion rate reaches 11.9％,and the CO selectivity is 99.4％.The role of Sn promoter in CO2 hydrogenation reaction was comprehensively analyzed by characterization methods such as XRD,H2-TPR,and H2-TPD.The results indicate that the introduction of Sn regulates the CO2 hydrogenation reaction from methanation to RWGS.After reduction,Sn and Co species form Co-Sn alloy,and new active sites reduce the ability of the catalyst surface to adsorb CO2,H2 and CO.Compared with 5Co/ZrO2,5Co5Sn/ZrO2 shows weaker adsorption and activation ability of H2 and much lower adsorption amount of CO2 and CO,which reduces the activity of CO2 hydrogenation and inhibits the deep CO2 hydrogenation,resulting in a decrease in the catalytic performance of the catalyst,a decrease in CH4 selectivity and an increase in CO selectivity to about 100％.关键词
CO2加氢/RWGS/选择性转换/Co-Sn合金/化学吸附Key words
CO2 hydrogenation/RWGS/selectivity switch/Co-Sn alloy/chemisorption分类
化学化工引用本文复制引用
袁金标,陈杰,胥月兵,刘冰,刘小浩..Sn助剂调控Co/ZrO2催化剂用于CO2选择性加氢制CO[J].低碳化学与化工,2024,49(11):21-27,7.基金项目
国家重点研发计划(2023YFB4103201) （2023YFB4103201）
国家自然科学基金(22379053,22372073). （22379053,22372073）
