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

IF 4.3 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry 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

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Abstract

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.

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使用铀配位聚合物进行过氧化氢的持久光合作用：激子解离与氢汲取。

过氧化氢（H2O2）的光合作用涉及水的氧化和氧的还原，是优化光利用的关键。本文利用之前合成的一维链状半导电铀酰配位聚合物（NDC-UCP）进行了高效的 H2O2 整体光合反应，并系统地研究了其光催化机理。NDC-UCP 具有优异的稳定性，可持续产生 H2O2 长达 96 h，其独特的氢萃取能力提高了光催化性能，H2O2 产生率达到 283.80 μmol g-1 h-1。研究揭示了产生 H2O2 的两种机制：NDC-UCP 中高效的电子-空穴分离促进了两步单电子氧还原和直接水氧化，而 UO22+ 的氢萃取产生羟基（-OH）和氢过氧自由基（HO2-），增强了 H2O2 的光合作用。这项研究凸显了铀酰配位聚合物在 H2O2 生成中的潜力，以及它们在光催化氧化还原反应中的协同激子解离和氢抽取功能。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.