Synergistic roles of platinum nanoparticles and sodium ions within beta zeolites in N-alkylation of amines with aromatic alcohols  

作　　者：Yue Wu Shibo Xi Cailing Chen Qizhi Hu Zhuo Xiong Jianyue Wang Yihu Dai Yu Han Shi Jiang Jun Wang Yu Zhou 

机构地区：[1]State Key Laboratory of Materials-Oriented Chemical Engineering,College of Chemical Engineering,Nanjing Tech University,Nanjing 211816,China [2]Institute of Sustainability for Chemicals,Energy and Environment,A*STAR(Agency for Science,Technology and Research),Singapore 627833,Singapore [3]Advanced Membranes and Porous Materials Center,Physical Sciences and Engineering Division,King Abdullah University of Science and Technology,Thuwal 23955-6900,Saudi Arabia [4]Institute of Advanced Synthesis,School of Chemistry and Molecular Engineering,Nanjing Tech University,Nanjing 211816,China

出　　处：《Science China Chemistry》2023年第9期2690-2699,共10页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China (22178162, 22108116, 22072065, and 22222806);the Distinguished Youth Foundation of Jiangsu Province (BK20220053);the Six talent peaks project in Jiangsu Province (JNHB035);Natural Science Foundation of Jiangsu Province (BK20200688);State Key Laboratory of Materials-Oriented Chemical Engineering-Open Fund (KL20-07)。

摘　　要：N-alkylation of amines with alcohols is a promising green route for the synthesis of N-alkylamines, but the designation of highly active and stable heterogeneous catalysts remains one challenge. In this work, we initiated the application of zeolite-encapsulated noble metal nanoparticles(NPs) in the N-alkylation of amines with aromatic alcohols. Platinum(Pt) NPs were directly confined into the framework of BEA zeolite with tunable Si/Al molar ratios and Na^(+) contents. The champion catalyst afforded the extremely high turnover number(TON) of 6,176 and turnover frequency(TOF) of 3,390 h^(-1) plus stable recyclability and broad substrate compatibility. The Na ions modulated the electronic state of Pt NPs to reach a moderate Pt–H strength, which wellbalanced the two crucial steps of dehydrogenation and H-transfer and accounted for the high catalytic performance. The encapsulation of zeolites provided spatial satisfaction for the synergy effect above and enhanced the stabilization of Pt NPs.

关 键 词：heterogeneous catalysis ZEOLITE AMINES N-ALKYLATION nano catalysts 

分 类 号：TQ426[化学工程] TB383.1[一般工业技术—材料科学与工程]