Photochromic radical states in 3D covalent organic frameworks with zyg topology for enhanced photocatalysis

扫码查看

原文链接

NETL
NSTL
万方数据

外文摘要：Covalent-organic frameworks(COFs)with photoinduced donor-acceptor(D-A)radical pairs show enhanced photocatalytic activity in principle.However,achieving long-lived charge separation in COFs proves challenging due to the rapid charge recombination.Here,we develop a novel strategy by combining[6+4]nodes to construct zyg-type 3D COFs,first reported in COF chemistry.This structure type exhibits a fused Olympic-rings-like shape,which provides a platform for stabilizing the photoinduced D-A radical pairs.The zyg-type COFs containing catalytically active moieties such as triphenylamine and phenothiazine(PTZ)show superior photocatalytic production rates of hydrogen peroxide(H2O2).Significantly,the photochromic radical states of these COFs show up to 400％enhancement in photocatalytic activity compared to the parent states,achieving a remarkable H2O2 synthesis rate of 3324 μmol g-1 h-1,which makes the PTZ-COF one of the best crystalline porous photocatalysts in H2O2 production.This work will shed light on the synthesis of efficient 3D COF photocatalysts built on topologies that can facilitate photogenerating D-A radical pairs for enhanced photocatalysis.

外文关键词：

3D covalent-organic frameworksphotochromic radical statesdonor and acceptorhydrogen peroxidephotocatalysis

作者：

Tian-Tian Ma、Guo-Zhang Huang、Xiao-Han Wang、Yan Liang、Run-Han Li、Bin Wang、Su-Juan Yao、Jia-Peng Liao、Shun-Li Li、Yong Yan、Ya-Qian Lan

展开 >

作者单位：

School of Chemistry,South China Normal University,Guangzhou 510006,China

Department of Chemistry,Guangdong Provincial Key Laboratory of Catalytic Chemistry,Southern University of Science and Technology,Shenzhen 518055,China

基金：

National Key R&D Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of China

项目编号：

2023YFA1507204222251092207110922271103

出版年：

2024

DOI：

10.1093/nsr/nwae177

国家科学评论(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.11(7)