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Durable Photosynthesis of Hydrogen Peroxide Using a Uranyl Coordination Polymer: Exciton Dissociation and Hydrogen Abstraction
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-11-19 , DOI: 10.1021/acs.inorgchem.4c03947
Mengnan Yuan, Lisha Jiang, Jinlu Li, Zhenyu Li, Jianxin Song, Xuemin Wang, Zuju Ma, Yanlong Wang, Wei Liu

The photosynthesis of hydrogen peroxide (H2O2), 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 H2O2 and its photocatalytic mechanism was systematically investigated. The excellent stability of NDC-UCP enables continuous H2O2 production for up to 96 h. Its unique hydrogen extraction capability enhances the photocatalytic performance, achieving a H2O2 production rate of 283.80 μmol g–1 h–1. Two mechanisms for H2O2 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 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.

中文翻译:


使用铀酰配位聚合物对过氧化氢进行持久光合作用:激子解离和氢提取



过氧化氢 (H2O2) 的光合作用涉及水氧化和氧还原,对于优化光利用至关重要。本研究采用一维链状半导电铀酰配位聚合物 (NDC-UCP) 进行 H2O2 的高效整体光合反应,并系统研究了其光催化机理。NDC-UCP 出色的稳定性使 H2O2 的连续生产长达 96 小时。其独特的氢萃取能力增强了光催化性能,实现了 283.80 μmol g–1 h–1 的 H2O2 生成速率。揭示了 H2O2 生成的两种机制:NDC-UCP 中的高效电子-空穴分离促进了两步单电子氧还原和直接水氧化,而 UO22+ 的氢提取产生羟基 (·OH) 和氢过氧自由基 (HO2) 的光合作用,增强 H2O2 的光合作用。本研究强调了铀酰配位聚合物在 H2O2 生产中的潜力及其在光催化氧化还原反应中的协同激子解离和氢提取功能。
更新日期:2024-11-19
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