Pyrimidine-containing covalent organic frameworks for efficient photosynthesis of hydrogen peroxide via one-step two electron oxygen reduction process  

作　　者：Hongyu Chen Hao Zhang Kai Chi Yan Zhao 

机构地区：[1]Second Medical Center and National Clinical Research Center for Geriatric Diseases, Chinese People’s Liberation Army General Hospital, Beijing, 100853, China [2]Laboratory of Molecular Materials and Devices, Department of Materials Science, Fudan University, Shanghai, 200433, China

出　　处：《Nano Research》2024年第11期9498-9506,共9页纳米研究（英文版）

基　　金：financially supported by the Nation Key Research and Development(R&D)Program of China(No.2022YFB3603804);Natural Science Foundation of Shanghai(No.22ZR1407800).

摘　　要：The photocatalytic oxygen reduction reaction (ORR), particularly the one-step two-electron (2e−) pathway, is a highly promising strategy for efficient and selective hydrogen peroxide (H_(2)O_(2)) synthesis. However, constructing efficient photocatalysts to achieve a one-step 2e− ORR process remains a significant challenge. Herein, we developed an efficient photocatalyst by incorporating pyrimidine units into benzotrithiophene-based covalent organic framework (BTT-MD-COF), enabling the photosynthesis of H_(2)O_(2) via the one-step 2e− ORR pathway with O_(2) and water. Under visible-light irradiation, BTT-MD-COF exhibited a high H_(2)O_(2) production rate of up to 5691.2 µmol·h^(−1)·g^(−1). Further experimental results and theoretical studies revealed that the introduction of pyrimidine units accelerates the separation of photoinduced electron–hole pairs and promotes Yeager-type O_(2) adsorption, which alters the two-step 2e− ORR process to the direct one-step 2e− process. This work offers a new avenue to create metal-free catalysts for efficient photosynthesis of H_(2)O_(2).

关 键 词：covalent organic frameworks photocatalysis hydrogen peroxide oxygen reduction reaction pyrimidine units 

分 类 号：O64[理学—物理化学]