Work

Durable Photosynthesis of Hydrogen Peroxide Using a Uranyl Coordination Polymer: Exciton Dissociation and Hydrogen Abstraction

Year: 2024

Type: article

Abstract: The photosynthesis of hydrogen peroxide (H 2 O 2 ), 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 H 2 O 2 and its photocatalytic mechanism was systematically investigated. The excellent stability of NDC-UCP enables continuous H 2 O 2 production for up to 96 h. Its unique hydrogen extraction capability enhances the photocatalytic performance, achieving a H 2 O 2 production rate of 283.80 μmol g –1 h –1 . Two mechanisms for H 2 O 2 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 2 2+ generates hydroxyl (·OH) and hydroperoxyl radicals (HO 2 · ), enhancing H 2 O 2 photosynthesis. This study highlights the potential of uranyl coordination polymers in H 2 O 2 production and their synergistic exciton dissociation and hydrogen abstraction functionalities in photocatalytic redox reactions.

Source: Inorganic Chemistry

DOI: 10.1021/acs.inorgchem.4c03947