文献类型：期刊文献

中文题名：Urchin-like Nb_(2)O_(5)hollow microspheres enabling efficient and selective photocatalytic C–C bond cleavage in lignin models under ambient conditions

作者：Huan Chen[1];Donghui Hong[1];Kun Wan[1];Junjie Wang[1];Bo Niu[1];Yayun Zhang[1];Donghui Long[1,2]

机构：[1]State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]Shanghai Key Laboratory of Multiphase Materials Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China

年份：2022

卷号：33

期号：9

起止页码：4357

中文期刊名：Chinese Chemical Letters

外文期刊名：中国化学快报（英文版）

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：financially supported by the National Natural Science Foundation of China (No. 22008073);Shanghai Sailing Program (No. 20YF1410600)

语种：英文

中文关键词：Niobium oxide;Urchin-like hierarchical structure;Photocatalysis;β-O-4 Lignin model;C_(β)radical

摘要：Selective cleavage of robust C?C bonds to harvest value-added aromatic oxygenates is an intriguing but challenging task in lignin depolymerization.Photocatalysis is a promising technology with the advantages of mild reaction conditions and strong sustainability.Herein,we show a novel urchin-like Nb_(2)O_(5)hollow microsphere(U-Nb_(2)O_(5)HM),prepared by one-pot hydrothermal method,are highly active and selective for C_(α)?C_(β)bond cleavage of ligninβ-O-4 model compounds under mild conditions,achieving 94%substrate conversion and 96%C?C bond cleavage selectivity.Systematic experimental studies and density functional theory(DFT)calculations revealed that the superior performance of U-Nb_(2)O_(5)HMs arises from more exposed active sites,more efficient free charge separation and the active(001)facet,which facilitates the activation of Cβ?H bond of lignin models and generate key Cβradical intermediates by photogenerated holes,further inducing the C_(α)?C_(β)bond cleavage to produce aromatic oxygenates.This work could provide some suggestions for the fabrication of hierarchical photocatalysts in the lignin depolymerization system.