文献类型：期刊文献

英文题名：Mechanical pressure-mediated Pd active sites formation in NaY zeolite catalysts for indirect oxidative carbonylation of methanol to dimethyl carbonate

作者：Wang, Chunzheng[1];Xu, Ningkun[1];Liu, Ting-Ting[2,3,4];Xu, Weisong[1];Guo, Hailing[1];Li, Yanpeng[1];Bai, Peng[1];Wu, Xin-Ping[2,3,4];Gong, Xue-Qing[2,3,4];Liu, Xinmei[1];Mintova, Svetlana[1,5]

机构：[1]China Univ Petr East China, Coll Chem Engn, State Key Lab Heavy Oil Proc, Qingdao 266580, Shandong, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Joint Int Res Lab Precis Chem & Mol Engn, Ctr Computat Chem,Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[5]Normandie Univ, CNRS, UNICAEN, Lab Catalyse & Spectrochim LCS,ENSICAEN, 6 Blvd Marechal Juin, F-14050 Caen, France

年份：2021

卷号：396

起止页码：269

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20211310134643);WOS:【SCI-EXPANDED(收录号:WOS:000641071900009)】；

基金：This work was supported by the National Natural Science Foundation of China (21908246, 21975285, 21991090, 21991091), Shanghai Sailing Program (20YF1410000), Fundamental Research Funds for the Central Universities (18CX02148A) and the SinoFrench International Laboratory (LIA) "Zeolites".

语种：英文

外文关键词：Mechanical pressure; Active site; Palladium; NaY; Carbonylation; Dimethyl carbonate

摘要：The structural transformation of metal-containing zeolite catalysts subjected to mechanical compression is often disregarded in the preparation of catalysts. Herein, the impact of the mechanical compression on the catalytic active sites of Pd/NaY catalysts responsible for the indirect oxidative carbonylation of methanol to dimethyl carbonate (DMC) has been disclosed. The DMC selectivity of the catalysts was found to strongly depend on the mechanical-pressure applied, as the mechanical pressure controlled the ratio of Pd(2+delta)+ and Pd delta+ species (0 < delta <= 2) in the catalysts. The mono-dispersed Pd clusters (1.3 nm) in the Pd/NaY catalyst were obtained under mechanical treatment of 300 MPa. This catalyst showed high CO conversion of 89% and DMC selectivity of 83%, that maintained for at least 150 h. Combining experimental and density functional theory studies, we revealed that the Pd delta+ rather than the Pd(2+delta)+ species enhanced the adsorption of CO and CH3ONO reactants and inhibited the decomposition of CH3ONO reactant into byproducts, and thus enhanced the DMC selectivity. The mechanical pressure applied had a noticeable effect on the structural features of the metal-containing zeolite catalysts, but despite its importance, this aspect has been poorly considered in the field of heterogenous catalysis. (C) 2021 Elsevier Inc. All rights reserved.