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

Abstract

The photosynthesis hydrogen peroxide (H2O2), involving water oxidation and oxygen reduction, is crucial for optimizing light utilization. Here, a one-dimensional chain-like semiconductive uranyl coordination polymer (NDC-UCP) was synthesized for efficient overall photosynthetic reaction of H2O2. NDC-UCP shows ultra-high stability and benefits from the hydrogen abstraction of UO22+, leading to a significant increase in photocatalysis response time and efficiency for up to 96 h. In air, the H2O2 production rate of NDC-UCP reached 283.80 μmol g-1 h-1. The study reveals two mechanisms for H2O2 generation: efficient electron-hole separation in NDC-UCP facilitates two-step one-electron oxygen reduction and direct water oxidation, while hydrogen abstraction of UO22+ generates hydroxyl (·OH) and hydroperoxyl radicals (HO2·), enhancing H2O2 photosynthesis. This study highlights the potential of uranyl coordination polymers in H2O2 production and their synergistic exciton dissociation and hydrogen abstraction functionalities in photocatalytic redox reactions.

Keywords: Uranyl coordination polymers, Exciton dissociation, UO22+, Hydrogen abstraction, H2O2