太原理工大学学报2025，Vol.56Issue(4)：639-647,9.DOI:10.16355/j.tyut.1007-9432.20240279
[MB12Hx]2-催化乙烯中微量乙炔半加氢反应的理论研究
Mechanism of Semi-Hydrogenation of Trace Acetylene in Ethylene by[MB12Hx]2-
摘要
Abstract
[Purposes]The main problem of semi-hydrogenation of trace acetylene in ethylene is excessive hydrogenation.High concentration of ethylene is the main cause of excessive hydrogenation,so it is important to design a catalyst with acetylene enrichment ability for semi-hydrogenation of acetylene.[Methods]A model catalyst with acetylene enrichment capability,[MB12Hx]2-(M=Pd,Ni,Ag;x=9,10),based on density functional theory was designed,the adsorption behavior of ethyl-ene and acetylene on its surface and the reaction mechanism of selective hydrogenation of acetylene were systematically studied.The adsorption energy,reaction heat,and activation energy of each spe-cies involved in acetylene hydrogenation reaction(C2H2,C2H3,CHCH3,C2H4,C2H5,H2,and H at-oms)on the catalyst surface were calculated in detail.[Results]The calculation results show that the energy barriers of excessive hydrogenation(C2H4+H=C2H5)at[PdB12H9]2-,[NiB12H9]2-,and[AgB12H10]2-are significantly higher than that of semi-hydrogenation(C2H4 desorption).Among them,[PdB12H9]2-shows the best ethylene selectivity(2.02 eV),and[PdB12H9]2-shows a high reactivity(1.18 eV)with a lower rate-limiting step activation energy barrier.关键词
[MB12Hx]2-/乙炔/乙烯/密度泛函理论/选择性加氢反应Key words
[MB12Hx]2-/acetylene/ethylene/DFT/selective hydrogenation分类
化学化工引用本文复制引用
陈康杰,王婉楠,史秀锋,任瑞鹏,吕永康..[MB12Hx]2-催化乙烯中微量乙炔半加氢反应的理论研究[J].太原理工大学学报,2025,56(4):639-647,9.基金项目
国家自然科学基金资助项目(22178244) （22178244）
山西省自然科学基金(20210302123118) （20210302123118）
山西浙大新材料与化工研究院项目(2021SX-FR001) （2021SX-FR001）
吕梁市校地合作重点研发专项(2022XDHZ07) （2022XDHZ07）
