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.
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)。