醋酸乙酯在Pd/Au表面的形成机理研究  

Study on formation mechanism of ethyl acetate on Pd/Au surface

作　　者：邱鹏远 孙浩洋 杨运信 刘军晓 张丽斌 QIU Pengyuan;SUN Haoyang;YANG Yunxin;LIU Junxiao;ZHANG Libin(State Key Laboratory of Green Chemical Engineering and Industrial Catalysis,Sinopec Shanghai Research Institute of Petrochemical Technology Co.,Ltd.,Shanghai 201208,China)

机构地区：[1]中石化(上海)石油化工研究院有限公司绿色化工与工业催化国家重点实验室,上海201208

出　　处：《石油化工》2024年第2期175-181,共7页Petrochemical Technology

基　　金：中国石油化工股份有限公司资助项目(223029)。

摘　　要：采用密度泛函理论研究了醋酸乙烯合成过程中关键副产物醋酸乙酯在Pd/Au(100)及Pd/Au(111)表面的形成机理,从微观层面揭示Pd/Au(100)及Pd/Au(111)表面不同Pd原子数、Pd/Au原子构型对醋酸乙酯形成的影响。研究结果表明,Pd/Au(100)和Pd/Au(111)表面邻位Pd活性位构型最有利于醋酸乙酯的生成,而随着Pd/Au表面Pd原子数的增加,生成醋酸乙酯的反应活性逐渐降低,团簇Pd活性位(Pd原子数大于等于4)可以有效抑制醋酸乙酯的生成。该机理为开发高选择性Pd/Au催化剂、抑制醋酸乙酯副产物生成提供了理论依据。Ethyl acetate is a key by-product in the synthesis of vinyl acetate.The formation mechanism of ethyl acetate on the Pd/Au(100)and Pd/Au(111)surfaces was investigated using density functional theory.The effects of Pd atomic number and Pd/Au atomic configuration on ethyl acetate formation over the Pd/Au(100)and Pd/Au(111)surfaces were revealed from a micro level.The study results show that the adjacent Pd active site configuration on the surfaces of Pd/Au(100)and Pd/Au(111)is most favorable for the formation of ethyl acetate,while the reactivity of ethyl acetate formation gradually decreases with the increase of the number of Pd atoms on the surface of Pd/Au,the cluster Pd active sites(Pd atom number above or equal to 4)can effectively inhibit the formation of ethyl acetate.This mechanism provides a theoretical basis for the development of highly selective Pd/Au catalysts to inhibit the generation of by-product ethyl acetate.

关 键 词：醋酸乙烯 Pd/Au催化剂 醋酸乙酯 密度泛函理论 

分 类 号：TQ426.94[化学工程]