低碳化学与化工2025，Vol.50Issue(5)：11-17,7.DOI:10.12434/j.issn.2097-2547.20250044
Pd2/CeO2上OV和H2O对催化CO2加氢反应影响的理论计算研究
Theoretical calculation study on effects of OV and H2O on CO2 hydrogenation over Pd2/CeO2
摘要
Abstract
CO2 hydrogenation to produce ethanol and other advanced products is one of the important ways to realize the resource utilization of CO2.Pd2/CeO2 catalyst is one of the ideal catalysts for CO2 hydrogenation to ethanol.The simulation methods can provide a more intuitive representation of the reaction process.The influence of oxygen vacancy(OV)and H2O on the CO2 hydrogenation process on Pd2/CeO2 catalyst was studied and analyzed by density functional theory(DFT).The results show that compared to clean catalyst surfaces,OV promotes CO2 adsorption and activation.In addition,OV also changes the electronic state between the support and the supported Pd,allowing Pd to provide more electrons to the C species,which is beneficial for subsequent C—O bond cleavage and C—C bond coupling reactions.However,when H2O is present on the surface of the catalyst,due to the high electronegativity of O species and H2O competes with CO2 and its derivatives for electrons,resulting in a decrease in the electron density of C species,which is not conducive to the cleavage of C—O bonds and the coupling of C—C bonds,thereby increasing the reaction energy barriers for ethanol generation.关键词
CO2/乙醇/氧空位/H2O/DFT计算Key words
CO2/ethanol/oxygen vacancy/H2O/DFT calculation分类
化学工程引用本文复制引用
张东健,查雅君,刘冰,刘小浩..Pd2/CeO2上OV和H2O对催化CO2加氢反应影响的理论计算研究[J].低碳化学与化工,2025,50(5):11-17,7.基金项目
国家重点研发计划(2023YFB4103201) （2023YFB4103201）
国家自然科学基金(22379053). （22379053）
