摘要
能源危机与环境恶化的危害日益严峻,亟需发展环境友好型可持续生产技术。将丰富的太阳能直接转化为化学能,被视为一种极具前景的绿色高效技术方案。在此过程中,光催化剂扮演着至关重要的角色。共价有机框架材料(COFs)作为一种通过共价键连接的多孔材料,凭借其高比表面积、优异的结晶性和可调控的结构,展现出卓越的光催化潜力。本综述深入探讨了组分调控对提升COFs光催化性能的作用机制,涵盖调控光吸收、增加活性位点、促进激子解离以及改善载流子分离,并对相关计算模拟与机理表征方法进行了详细论述。更为重要的是,系统总结了组分调控的核心策略,包括杂原子工程、金属单原子工程、离子工程、官能团工程、供体-受体(D-A)分子工程、侧链工程、多组分工程、同分异构工程、共轭桥工程、单分子结工程和层间工程。此外,本文还详细阐述了这些策略在光催化析氢(H_(2))、过氧化氢(H_(2)O_(2))合成及二氧化碳(CO_(2))还原等领域的多样化改性策略与应用。最后,对COF基光催化技术当前面临的挑战及未来发展方向进行了前瞻性展望。
The harmful effects of the energy crisis and environmental degradation are becoming increasingly severe,which urgently demands the advancement of ecofriendly and sustainable production techniques.Direct conversion of abundant solar energy into chemical energy represents a promising green and efficient technological solution.In this process,photocatalysts play a pivotal role.Covalent organic frameworks(COFs),a class of porous materials interconnected by covalent bonds,exhibit exceptional potential for photocatalysis due to their high surface area,excellent crystallinity,and tunable structures.This review discusses the roles of compositional regulation in enhancing the photocatalytic performance of COFs,including modulating light absorption,increasing active sites,promoting exciton dissociation,and improving carrier separation.Furthermore,computational and mechanistic characterization methods are also discussed.More importantly,the key strategies in compositional regulation,such as heteroatom engineering,metal single-atom engineering,ion engineering,functional group engineering,Donor-Acceptor(D-A)molecular engineering,side chain engineering,multi-component engineering,isomerism engineering,conjugate bridge engineering,single-molecule junction engineering,and interlayer engineering,are carefully summarized.Moreover,their diversified modification strategies and applications in photocatalytic hydrogen(H_(2))evolution,hydrogen peroxide(H_(2)O_(2))production,and carbon dioxide(CO_(2))reduction are also addressed.Finally,the current challenges and future opportunities for COF-based photocatalysis are outlined.
作者
邵毅宏
沈荣晨
王松
李世杰
张鹏
李鑫
Yihong Shao;Rongchen Shen;Song Wang;Shijie Li;Peng Zhang;Xin Li(Institute of Biomass Engineering,Key Laboratory for Biobased Materials and Energy of Ministry of Education,College of Materials and Energy,South China Agricultural University,Guangzhou 510642,Guangdong Province,China;Hubei Key Lab Low Dimens Optoelect Mat&Devices,Hubei University of Arts and Science,Xiangyang 441053,Hubei Province,China;Key Laboratory of Health Risk Factors for Seafood of Zhejiang Province,National Engineering Research Center for Marine Aquaculture,College of Marine Science and Technology,Zhejiang Ocean University,Zhoushan 316022,Zhejiang Province,China;State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM),School of Materials Science and Engineering,Zhengzhou University,Henan,Zhengzhou 450001,Henan Province,China)
出处
《物理化学学报》
北大核心
2025年第12期1-48,共48页
Acta Physico-Chimica Sinica
基金
国家自然科学基金(22378148,21975084)
国家自然科学基金(2230082074)的资助
广东省自然科学基金(2024A1515012433)。
关键词
共价有机框架
组分调控
光催化应用
工程和改性策略
激子解离
Covalent organic frameworks
Compositional regulation
Photocatalytic applications
Engineering and modification strategies
Exciton dissociation
