光催化
异质结
亚胺
共价键
桥接(联网)
Boosting(机器学习)
材料科学
化学工程
对偶(语法数字)
还原(数学)
化学
光化学
纳米技术
光电子学
催化作用
计算机科学
有机化学
工程类
计算机网络
艺术
文学类
机器学习
数学
几何学
作者
Manman Mu,Lingqi Meng,Siting Ma,Wenjuan Chen,Xiaohong Yin,Guoyi Bai
标识
DOI:10.1016/j.jcis.2025.01.232
摘要
Covalent organic frameworks (COFs) equipped with controllable porosity and excellent structural stability are regarded as promising candidates for photocatalytic CO 2 reduction, yet some inherent drawbacks including low CO 2 activation and sluggish charge carriers’ transfer properties urgently need to be addressed. Herein, we developed an imine-bridged strategy to construct ZnO/COF heterostructure by integrating donor–acceptor COF (TAPT-DMTP COF) on the surface of amino-modified ZnO for photocatalytic CO 2 reduction. The optimal photocatalyst , N ZnO/TAPT-DMTP COF-3, exhibited superior photocatalytic activity for reducing CO 2 to CO and CH 4 , which was significantly higher than pristine COF and non-covalently bridged ZnO/TAPT-DMTP COF. Experimental and photo-electrochemical results reveal that the microstructure of TAPT-DMTP COF, interfacial imine-bridging and S-scheme heterojunction play a crucial role in promoting photoinduced charge transfer and separation, thus improving photocatalytic efficiency. Moreover, in-situ characterization and theoretical calculations indicate the photoinduced electrons transfer from N ZnO to TAPT-DMTP COF upon hybridization, and this S-scheme heterostructure dramatically lowers the energy barrier of rate-determining step from *COOH to *CO. This work provides insight into the covalent-linked COF-based S-scheme photocatalyst and highlights its vital role in enhancing CO 2 reduction.
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