Recent Progress in Halogen-Doped Single-Atom Catalysts for Electrochemical Reactions

Shichang Cai, Qing Wang, Naying Zhang, Chaoqun Chen, Hanlu Zhang, Yagang Feng, Lei Duan, Yapeng Cheng, Zihan Meng, Huaiguang Li, Jiabin Wu
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Abstract

Since the concept of single-atom catalysts (SACs) was first proposed in 2011, related research has grown exponentially, establishing SACs as a highly active research field. Compared to conventional supported nanoparticle catalysts, SACs have attracted significant attention due to their theoretically highest atomic utilization efficiency and tunable active sites. Halogen atoms, with their high electronegativity, possess strong electron-withdrawing ability, enabling them a powerful regulatory effect on the active sites. Although there are numerous comprehensive and high-quality reviews on SACs, specialized research on halogen-doped SACs is relatively scarce. Therefore, this article reviewed recent progress in halogen-doped SACs, categorizing them by the four halogen atoms: fluorine (F), chlorine (Cl), bromine (Br), and iodine (I). We also discussed the application of halogen-doped SACs in several key electrochemical reactions commonly relevant to clean energy storage and conversion, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and CO2 reduction reaction (CO2RR), and elaborated on the corresponding reaction mechanisms. Finally, this paper presented prospects to promote the development of SACs with tunable catalytic activity.

Abstract Image

电化学反应中掺杂卤素单原子催化剂的研究进展
自2011年首次提出单原子催化剂(SACs)的概念以来,相关研究呈指数级增长,使其成为一个非常活跃的研究领域。与传统负载型纳米颗粒催化剂相比,sac因其理论上最高的原子利用效率和可调的活性位点而备受关注。卤素原子具有较高的电负性,具有很强的吸电子能力,对活性位点有很强的调节作用。虽然对SACs进行了大量全面、高质量的综述,但对卤素掺杂SACs的专门研究相对较少。因此,本文综述了近年来卤素掺杂SACs的研究进展,并按四个卤素原子对其进行了分类:氟(F)、氯(Cl)、溴(Br)和碘(I)。我们还讨论了卤素掺杂SACs在几种与清洁能源储存和转化相关的关键电化学反应中的应用,包括析氢反应(HER)、析氧反应(OER)、氧还原反应(ORR)和CO2还原反应(CO2RR),并阐述了相应的反应机理。最后,对催化活性可调SACs的发展进行了展望。
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