Luo Qingsong, Wang Hai, Wang Liang, Xiao Feng-Shou
Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
ACS Mater Au. 2022 Feb 9;2(3):313-320. doi: 10.1021/acsmaterialsau.1c00080. eCollection 2022 May 11.
Selective hydrogenation of acetylene to ethylene is an industrially important process to purify the raw ethylene stream for producing high-grade polyethylene. The supported Pd catalyst exhibits superior activity for acetylene hydrogenation but suffers from poor ethylene selectivity because of the easy overhydrogenation to produce ethane. Here, we report that the PdCu alloy nanoparticles within siliceous zeolite crystals effectively tuned Pd-catalyzed overhydrogenation into semihydrogenation. This catalyst displayed an ethylene selectivity of 92.9% with a full conversion of acetylene. Mechanism studies reveal that the zeolite fixation stabilized the alloyed structure, where the electron-enriched Pd surface benefits the rapid ethylene desorption to hinder the deep hydrogenation. This work provides an efficient strategy for a rational design of bimetallic metal catalysts for selective hydrogenations.
乙炔选择性加氢制乙烯是一种工业上重要的工艺,用于净化粗乙烯物流以生产高等级聚乙烯。负载型钯催化剂在乙炔加氢反应中表现出优异的活性,但由于易于过度加氢生成乙烷,导致乙烯选择性较差。在此,我们报道了硅质沸石晶体中的钯铜合金纳米颗粒有效地将钯催化的过度加氢转变为半加氢。该催化剂在乙炔完全转化的情况下,乙烯选择性达到92.9%。机理研究表明,沸石固定作用稳定了合金结构,其中富电子的钯表面有利于乙烯快速脱附,从而阻碍深度加氢。这项工作为合理设计用于选择性加氢的双金属催化剂提供了一种有效策略。