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作 者:董晓宇 王辉 张晓东 谢毅[2] Xiao-Yu Dong;Hui Wang;Xiao-Dong Zhang;Yi Xie(Hefei National Research Center for Microscale Materials Science,University of Science and Technology of China,Hefei 230026,China;State Key Laboratory of Precision and Intelligent Chemistry,University of Science and Technology of China,Hefei 230026,China)
机构地区:[1]中国科学技术大学,合肥微尺度物质科学国家研究中心,合肥230026 [2]中国科学技术大学,精准智能化学全国重点实验室,合肥230026
出 处:《科学通报》2025年第7期816-834,共19页Chinese Science Bulletin
基 金:国家自然科学基金(T2122004,92163105,U2032212,92477116)资助。
摘 要:近年来,半导体光催化过氧化氢(H_(2)O_(2))合成因其相较于传统化学合成方法在能耗和环保方面具有显著优势而受到了广泛关注,在污染物处理、化学品合成、生物医疗等领域展现出良好的应用前景.然而,由于半导体光催化H_(2)O_(2)合成涉及复杂的反应机制以及产物相对较高的化学活性,其在催化体系的设计、性能评估及优化方面呈现出一定的特殊性,这也成为了当前研究的重点与难点.本文聚焦半导体光催化H_(2)O_(2)合成,对近期该领域的研究进展进行了综述.在简要介绍H_(2)O_(2)产生机制基础上,从催化体系筛选、催化反应器设计、性能评估、优化策略开发、应用场景拓展等方面对相关研究进行总结、归纳;讨论了半导体光催化H_(2)O_(2)合成研究面临的挑战,展望了该领域未来的研究方向及可能的突破点.Semiconductor-based photocatalysis provides a sustainable and green pathway for pursuing hydrogen peroxide(H_(2)O_(2))production,showing great potential in the fields of pollutant degradation,chemical synthesis,and phototherapy.Compared with other photocatalytic reactions(like carbon dioxide reduction,nitrogen fixation,and water splitting),photocatalytic H_(2)O_(2)production via molecular oxygen(O2)reduction and/or water(H_(2)O)oxidation is more feasible in both thermodynamics and kinetics aspects.Moreover,the high chemical reactivity of H_(2)O_(2)also endows the system with unique performance-evaluation methods and application scenarios.The above characteristics complicate the relevant investigations,and the photocatalyticsystem design deserves more special attention.Recently,benefiting from the development of synthetic and characterization techniques,great progress has been made in semiconductor-based photocatalytic H_(2)O_(2)production.In this work,we provide an overview of recent advances in the field of semiconductor-based photocatalytic H_(2)O_(2)production.In the first part,we summarize the mechanism of semiconductor-based photocatalytic H_(2)O_(2)production.Typically,photocatalytic H_(2)O_(2)production could undergo a series of reaction pathways,mainly involving electron-transfer-mediated O2 reduction and hole-transfer-mediated H_(2)O oxidation.The versatile reaction pathways,on the one hand,make it difficult to quantitate the contributions of different processes,on the other hand,enable diverse optimization methods to be established.The characterization techniques for interrogating excited-state and structural properties involved in the reaction are also summarized.Moreover,we discuss the general optimization methodologies for pursuing advanced photocatalytic H_(2)O_(2)production.To go further,we summarize recent progress in the performance evaluation of photocatalytic H_(2)O_(2)production.Owing to the relatively high reactivity of H_(2)O_(2)and the requirement of product separation,the reactor has been
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