电催化析氧反应过渡金属磷化物和硫化物催化剂研究进展

doi:10.1016/S1872-2067(18)63130-4

摘要/Abstract

摘要：

对化石能源的依赖所造成的环境污染和能源危机在全球引起了广泛的关注.氢能由于其高能量密度、低分子质量以及清洁无污染的优点，被认为是人类根本性解决能源与环境等全球性问题的理想替代能源.电解水是生产高纯度氢的重要方法，是现代清洁能源技术的重要组成部分.水电解由阴极析氢（HER）和阳极析氧（OER）两个半反应构成.对于HER反应，其反应是基于二电子转移过程，反应过程相对容易进行.相比于HER反应，OER反应涉及四电子转移及氧-氧键形成，其反应动力学缓慢，是影响水电解效率的主要原因.因此，为了提高电解水制氢的能量转化效率，发展OER电催化剂成为水电解制氢技术的关键.在过去的十余年间，硫化物、硒化物、磷化物、硼化物等非贵金属基OER电催化剂被大量地研究及报道并取得了长足发展.在这些催化剂中，金属磷化物和硫化物不仅具有成本优势，而且在析氧过电位、耐久性方面正趋接近甚至超越RuO₂和IrO₂等贵金属催化剂，颇具应用潜力.本文总结磷化物和硫化物作为OER电催化剂的研究进展，重点介绍了磷化物和硫化物性能提升策略及其在OER过程中催化反应活性位的变化.
本文首先介绍了电解水析氧反应在不同电解质中的反应机理，讨论了析氧反应在动力学和热力学过程的主要障碍.通过对大量文献的归纳，本文分别综述了磷化物和硫化物的化学性质、合成方法和催化性能，介绍了近年来磷化物和硫化物的重要研究进展.通过分析催化剂导电性、质子传输、活性面积、界面化学等因素对催化析氧反应的影响，总结了磷化物和硫化物电催化OER性能提升的策略.由于磷化物和硫化物在OER强氧化条件下，电催化剂表面的成分、物相及结构均会发生显著变化，进而催化反应活性位也会发生相应改变.本文综述了磷化物和硫化物在OER反应过程前后表面组分的变化，探讨了磷化物和硫化物作为OER电催化剂的活性组分，为进一步提高磷化物和硫化物的电催化析氧反应性能提供了崭新的思路.

关键词: 析氧反应, 电催化剂, 金属磷化物, 金属硫化物, 原位氧化, 活性组分

Abstract:

Oxygen evolution reaction (OER), as an important half-reaction involved in water splitting, has been intensely studied since the last century. Transition metal phosphide and sulfide-based compounds have attracted increasing attention as active OER catalysts due to their excellent physical and chemical characters, and massive efforts have been devoted to improving the phosphide and sulfide-based materials with better activity and stability in recent years. In this review, the recent progress on phosphide and sulfide-based OER electrocatalysts in terms of chemical properties, synthetic methodologies, catalytic performances evaluation and improvement strategy is reviewed. The most accepted reaction pathways as well as the thermodynamics and electrochemistry of the OER are firstly introduced in brief, followed by a summary of the recent research and optimization strategy of phosphide and sulfide-based OER electrocatalysts. Finally, some mechanistic studies of the active phase of phosphide and sulfide-based compounds are discussed to give insight into the nature of active catalytic sites. It is expected to indicate guidance for further improving the performances of phosphide and sulfide-based OER electrocatalysts.

Key words: Oxygen evolution reaction, Electrocatalysis, Metal phosphide, Metal sulfide, In situ oxidation, Active component

彭立山, Syed Shoaib Ahmad Shah, 魏子栋. 电催化析氧反应过渡金属磷化物和硫化物催化剂研究进展[J]. 催化学报, 2018, 39(10): 1575-1593.

Lishan Peng, Syed Shoaib Ahmad Shah, Zidong Wei. Recent developments in metal phosphide and sulfide electrocatalysts for oxygen evolution reaction[J]. Chinese Journal of Catalysis, 2018, 39(10): 1575-1593.

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