Regulating the Built-In Electric field in Covalent Organic Frameworks for Enhanced CO2 Photoreduction: Asymmetry Linkage Structures

被引：0

作者：

Zhang, Qian ^{[1
]}

Zhao, Xiao ^{[2
]}

Gao, Shuaiqi ^{[1
]}

Guo, Yingying ^{[1
]}

Wang, Huiyong ^{[1
]}

Liu, Zhimin ^{[3
]}

Wang, Jianji ^{[1
]}

机构：

[1] Henan Normal Univ, Sch Chem & Chem Engn, Minist Educ, Key Lab Green Chem Media & React,Collaborat Innova, Xinxiang 453007, Henan, Peoples R China

[2] Hubei Inst Aerosp Chemotechnolgy, Sci & Technol Aerosp Chem Power Lab, Xiangyang 441003, Hubei, Peoples R China

[3] Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci,Key Lab Colloid Interface, Beijing 100190, Peoples R China

来源：

ACS CATALYSIS | 2025年 / 15卷 / 09期

基金：

中国国家自然科学基金;

关键词：

CO2; photoreduction; covalent organic framework; asymmetric linkage structure; built-in electric field; reaction mechanism; REDUCTION;

D O I：

10.1021/acscatal.4c07640

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Covalent organic frameworks (COFs) are an emerging kind of photocatalysts which convert CO2 to value-added fuels. However, COFs usually exhibit lower catalytic efficiency without using metal, sacrificial reagent, or photosensitizer due to their easy electron-hole recombination. Herein, a series of imine-linked COFs with different asymmetric linkage structures have been synthesized to enhance the separation efficiency of photoexcited electron-hole pairs in the COFs by tuning the intramolecular built-in electric-field strength. The OH-COF exhibits a high CO production rate of 616 mu mol g(-1) in the 4 h reaction with similar to 100% selectivity, which surpasses most of the metal-free COF photocatalysts reported in the literature. This reveals that the higher polarity of OH-COF with an asymmetric linkage structure leads to a stronger built-in electric-field strength and a faster charge-transfer rate and thus more efficient photocatalytic performance. This work would provide some insights into the built-in electric-field design of COFs for efficient CO2 photoreduction.

引用

页码：6739 / 6748

页数：10

共 70 条

[41] Flexible Films of Covalent Organic Frameworks with Ultralow Dielectric Constants under High Humidity [J].