基于镍铁层状双氢氧化物的氧析出催化剂:催化机制、电极设计和稳定性  

Use of NiFe Layered Double Hydroxide as Electrocatalyst in Oxygen Evolution Reaction:Catalytic Mechanisms,Electrode Design,and Durability

作　　者：王往 刘宇澄 陈胜利[1] Wang Wang;Yucheng Liu;Shengli Chen(Electrochemical Power Sources Key Laboratory,College of Chemistry and Molecular Sciences,Wuhan University,Wuhan 430072,China;Core Facility of Wuhan University,Wuhan 430072,China)

机构地区：[1]武汉大学化学与分子科学学院,化学电源材料与技术湖北省重点实验室,武汉430072 [2]武汉大学科研条件公共服务平台,武汉430072

出　　处：《物理化学学报》2024年第2期12-44,共33页Acta Physico-Chimica Sinica

基　　金：国家自然科学基金(22102121,21832004);中国博士后创新人才支持计划(BX20200253)资助项目。

摘　　要：近几十年来,氧析出反应因其在能量储存和转换技术中的关键作用而受到了广泛关注。然而,它需要高效的催化剂例如IrO2和RuO2,来加速其缓慢的反应动力学。在所开发的低成本材料中,镍铁层状双氢氧化物(NiFe LDH)较为有前景,其在碱性电解质中表现出出色的氧析出性能,过电位很低,在10 mA·cm^(-2)处仅需200-300 mV。虽然人们在开发基于NiFe LDH的高效电催化剂方面做出了巨大努力并取得了一些成果,但是要进一步降低其过电位具有相当的挑战性。为了克服这个瓶颈,就需要明确识别其活性位点和催化机理,从根本出发来探究新的解决方案,以获得具有超低过电位的催化剂。本综述首先回顾了NiFe LDH的结构、组成和发展历史。虽然人们在研究催化活性位点和机制方面付出了巨大努力,但其真正的催化位点和机制仍然是模棱两可并存在争议的。我们对催化位点研究的代表性工作进行了全面分析,希望对催化机理和活性位点能提供一些深入认识和理解。此外,我们还就增强其催化活性的各种策略,如杂原子掺杂和引入空位等,进行了总结并基于电子和几何结构对其活性提高原理进行了分类,为开发高性能的NiFe LDH基催化剂提供新的见解和方向。此外,催化剂的稳定性,尤其是在高电流密度等技术条件下的稳定性至关重要,但常常被人们忽视。最新的研究表明,NiFe LDH基催化剂在高电流密度下运行一段时间就会出现严重的活性衰减。因此,本综述强调了稳定性问题的重要性,以引起更多研究者对此问题的关注,并分析了NiFe LDH基催化剂的衰减机理,总结和讨论了基于这些衰减机理开发的改善稳定性问题的最新策略。最后,本综述讨论了制备兼具优异催化活性和稳定性的NiFe LDH基的高效催化剂的可能发展方向。In recent decades,the oxygen evolution reaction(OER)has attracted significant attention because of its critical role in energy storage and conversion technologies.This reaction requires highly efficient catalysts such as IrO2 and RuO2 to accelerate its slow reaction rate.Among existing developed low-cost materials,NiFe layered double hydroxides(NiFe LDH)have demonstrated great potential for use in OERs in alkaline electrolytes with low overpotential(200-300 mV at 10 mA∙cm-2).Extensive efforts have been devoted to developing efficient electrocatalysts based on NiFe LDHs;Further reducing their overpotential can be a challenging task.To overcome this bottleneck,it is necessary to clearly identify the catalytic mechanism and active sites and finding new solutions to obtain catalysts with ultra-low overpotential.Through this review,we thoroughly examined the structure,composition,and development history of NiFe LDHs.Despite the extensive investigation of the catalytic active sites and mechanism,it still remains elusive and controversial.Herein,existing studies that have aimed to elucidate the catalytic sites are presented and comprehensively analyzed,providing an insightful understanding of the catalytic mechanism and active sites of NiFe LDHs.Additionally,various strategies,such as heteroatom doping and the introduction of vacancies,have been proposed to enhance the catalytic activities of these materials.Considering the electronic and geometrical structures of NiFe LDHs,this review summarizes and categorizes activity enhancement methods based on different enhancement mechanisms,offering new insights and directions for developing high-performance NiFe LDH-based catalysts.Furthermore,despite being crucial to the practical use of the catalyst,catalyst stability is often overlooked,especially under technological conditions such as high current densities.Recent works have suggested that NiFe LDH-based catalysts suffer severe activity fading under high current densities after a short period of operation.It is important

关 键 词：镍铁层状双氢氧化物 氧析出反应 催化机制 电极设计 稳定性 

分 类 号：O646[理学—物理化学]