Yuan Mengnan, Jiang Lisha, Li Jinlu, Li Zhenyu, Song Jianxin, Wang Xuemin, Ma Zuju, Wang Yanlong, Liu Wei
School of Environmental and Material Engineering, Yantai University, Yantai 264005, China.
Shandong Nuclear and Radiation Safety Monitoring Center, No. 145 Jingshi West Road, Shandong, Jinan 25117, China.
Inorg Chem. 2024 Dec 2;63(48):22892-22902. doi: 10.1021/acs.inorgchem.4c03947. Epub 2024 Nov 19.
The photosynthesis of hydrogen peroxide (HO), involving water oxidation and oxygen reduction, is crucial for optimizing light utilization. Here, a previously synthesized one-dimensional chain-like semiconductive uranyl coordination polymer (NDC-UCP) was used for the efficient overall photosynthetic reaction of HO and its photocatalytic mechanism was systematically investigated. The excellent stability of NDC-UCP enables continuous HO production for up to 96 h. Its unique hydrogen extraction capability enhances the photocatalytic performance, achieving a HO production rate of 283.80 μmol g h. Two mechanisms for HO generation were revealed: efficient electron-hole separation in NDC-UCP facilitates a two-step one-electron oxygen reduction and direct water oxidation, while hydrogen abstraction of UO generates hydroxyl (·OH) and hydroperoxyl radicals (HO), enhancing HO photosynthesis. This study highlights the potential of uranyl coordination polymers in HO production and their synergistic exciton dissociation and hydrogen abstraction functionalities in photocatalytic redox reactions.
