伯醇对镍基催化剂在转移氢化反应中的抑制作用研究  

Primary alcohols as killers of Ni‐based catalysts in transfer hydrogenation

作　　者：Nikolay Nesterov Alexey Philippov Vera Pakharukova Evgeny Gerasimov Stanislav Yakushkin Oleg Martyanov Nikolay Nesterov;Alexey Philippov;Vera Pakharukova;Evgeny Gerasimov;Stanislav Yakushkin;Oleg Martyanov(Boreskov Institute of Catalysis SB RAS,Novosibirsk 630090,Russia)

机构地区：[1]博列斯科夫催化研究所,俄罗斯新西伯利亚

出　　处：《Chinese Journal of Catalysis》2024年第3期168-179,共12页催化学报（英文）

基　　金：俄罗斯联邦科学和高等教育部(101411).

摘　　要：本文研究了在转移加氢条件下,不同类型醇作为氢供体对镍基催化剂在苯并呋喃加氢反应中的活性影响.结果表明,使用异丙醇作为氢供体时,苯并呋喃的加氢过程为底物先发生脱芳构化,然后再进行脱氧反应.然而,当使用伯醇如甲醇、乙醇和正丙醇作为氢供体时,会导致镍基催化剂的不可逆失活.针对这一现象,进一步研究了伯醇使镍基金属催化剂失活的机理.结果表明,在250°C条件下,催化剂与伯醇的相互作用会导致形成非活性的碳化物Ni_(3)C,并且镍金属颗粒在氧化铝载体表面会发生烧结和偏析.The effect of different types of alcohols used as hydrogen donors on the activity of a metal Ni-based catalyst in the hydrogenation of benzofuran as a model substrate under transfer hydrogenation conditions has been studied.The hydrogenation process of benzofuran using 2-PrOH as a hydrogen donor leads sequentially to dearomatization and then to deoxygenation of the substrates.At the same time,the use of primary alcohols such as MeOH,EtOH and 1-PrOH as hydrogen donors leads to irreversible deactivation of the Ni-containing catalyst.A clear mechanism of deactivation of Ni-based metal catalysts by primary alcohols has been established.The interaction of the catalyst with primary alcohols at a temperature of 250°C leads to the formation of an inactive Ni_(3)C carbide phase,as well as sintering and segregation of metal particles on the surface of the alumina support.

关 键 词：苯并呋喃 转移加氢 超临界共沉淀 NI催化剂 醇 

分 类 号：TQ116.2[化学工程—无机化工] TQ426