Encapsulating Electron-Rich Pd NPs with Lewis Acidic MOF: Reconciling the Electron-Preference Conflict of the Catalyst for Cascade Condensation via Nitro Reduction

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First Author:Yiming Wang

Correspondence Author:Qionglin Liang,Hong-Bin Sun

Co author:Tian Haimeng,Li Hong,Deng Xinchen,Zhang Qiao,Ai Yongjian,Sun Zejun,Wang Yu,Liu Lei,Hu Zenan, Zhang Xinyue,Guo Rongxiu,Xu Wenjuan

Journal:Acs Applied Materials & Interfaces

Issue:6

Volume:14

Impact Factor:8.3

DOI number:10.1021/acsami.1c22256

Teaching and Research Group:物理化学

Place of Publication:Energy & Fuels

Abstract:Cascade reactions take advantage of step-saving and facileoperation for obtaining chemicals. Herein, catalytic hydrogenation ofnitroarene coupled condensation with β-diketone to afford β-ketoenaminesis achieved by an integrated nanocatalyst, Pd-e@UiO-66. The catalyst hasthe structure of an acid-rich metal−organic framework (MOF), UiO-66-encapsulated electron-rich Pd nanoparticles, and it reconciles the electron-effect contradiction of cascade catalytic reactions: catalytic hydrogenationrequires an electron-rich catalyst, while condensation requires electron-deficient Lewis acid sites. The catalyst showed good activity, highchemoselectivity, and universal applicability for the synthesis of β-ketoenamines using nitroarenes. More than 30 β-ketoenamines havebeen successfully prepared with up to 99% yield via the methodology ofrelay catalysis. The catalyst exhibited excellent stability to maintain itscatalytic performance for more than five cycles. Furthermore, we conducted an in-depth exploration of the reaction mechanism withtheoretical calculations

Key Words:cascade synthesis,β-ketoenamines,hydrogenation of nitroarenes,relay catalysis,reconciliation of electron-preference conflict,atmospheric H2

Document Code:WOS:000758112600001

Discipline:Natural Science

First-Level Discipline:Chemistry

Page Number:7949-7961

ISSN No.:1944-8244

Translation or Not:no