{"title":"An alternative photochemical water oxidation pathway driven by halide ions as electron relay","authors":"Chaowei Peng, Miao Shui, Haorui Wang, Hongfei Liu","doi":"10.1016/j.apcata.2025.120287","DOIUrl":null,"url":null,"abstract":"<div><div>The development of robust catalysts to drive the water oxidation half reaction, i.e. oxygen evolution, is crucial to achieve efficient artificial photosynthesis toward clean solar fuel production. The use of [Ru<sup>II</sup>(bpy)<sub>3</sub>]<sup>2+</sup> as photosensitizer and S<sub>2</sub>O<sub>8</sub><sup>2-</sup> as electron acceptor has been established as a standard photochemical protocol for activity assessment and mechanistic study of synthetic water oxidation catalysts. While a metal-based catalyst is considered indispensable for oxygen evolution therein, we here report that halide (Cl<sup>-</sup> and Br<sup>-</sup>) ions alone can straightforwardly drive water oxidation through acting as electron relays (X<sup>-</sup>→X<sub>2</sub>→XO<sup>-</sup>→O<sub>2</sub>). This may open up new strategies to manage the demanding four-electron transfer kinetics of the photocatalytic oxygen evolution reaction.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"699 ","pages":"Article 120287"},"PeriodicalIF":4.7000,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25001887","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The development of robust catalysts to drive the water oxidation half reaction, i.e. oxygen evolution, is crucial to achieve efficient artificial photosynthesis toward clean solar fuel production. The use of [RuII(bpy)3]2+ as photosensitizer and S2O82- as electron acceptor has been established as a standard photochemical protocol for activity assessment and mechanistic study of synthetic water oxidation catalysts. While a metal-based catalyst is considered indispensable for oxygen evolution therein, we here report that halide (Cl- and Br-) ions alone can straightforwardly drive water oxidation through acting as electron relays (X-→X2→XO-→O2). This may open up new strategies to manage the demanding four-electron transfer kinetics of the photocatalytic oxygen evolution reaction.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.