缺陷型电催化剂在氧还原反应中的应用

Progress of Non-Precious Metal Electrocatalysts with Defects for Oxygen Reduction Reaction

摘要:

氧还原反应（ORR）在现代能量转换和先进合成技术中扮演着至关重要的角色。对于燃料电池及金属-空气电池而言，ORR在提升能量效率和增强稳定性方面发挥着不可或缺的作用。此外，在绿色合成过氧化氢的过程中，ORR同样发挥着不可替代的作用。然而，ORR的缓慢动力学特性限制了这些技术的发展，因此需要合适的催化剂来调控和加速该反应变得尤为迫切。在众多催化剂中，贵金属催化剂因具有良好的导电性、高的电化学活性和优异的稳定性等优点而展现出较好的ORR性能，但这些催化剂因价格昂贵和地球储量低等限制了大规模应用的可行性。因此，探索和开发非贵金属基ORR催化剂，尤其是通过缺陷工程策略来对非贵金属催化剂的性能进行调控和优化至关重要。在深入阐述ORR机理的基础上，综述了含缺陷的非贵金属催化剂在ORR研究中的最新进展，分别探讨了边缘缺陷、空位、拓扑缺陷等本征缺陷及杂原子掺杂对催化活性的影响。同时，梳理了这些缺陷在促进特定电子转移路径中所起到的关键作用。此外，对单原子催化剂、双原子催化剂及金属氧化物中存在的缺陷在ORR中的应用潜力进行了综述。最后，对ORR催化剂的未来研究方向进行了展望，指出含缺陷非贵金属材料由于独特的结构和组成，在催化ORR中会展现出广阔的应用前景。

Abstract:

The oxygen reduction reaction （ORR） plays a crucial role in modern energy conversion and advanced synthesis technologies. For fuel cells and metal-air batteries， ORR plays an indispensable role in enhancing energy efficiency and stability. Additionally， ORR also plays an irreplaceable role in the green synthesis of hydrogen peroxide. However， the slow kinetics of ORR limit the development of these technologies， making it particularly urgent to find suitable catalysts to regulate and accelerate the progress of this reaction. Among various catalysts， precious metal catalysts exhibit good ORR performance due to their advantages such as good conductivity， high electrochemical activity， and excellent stability. However， these catalysts are limited in their feasibility for large-scale applications due to their high price and low earth reserves. Therefore， exploring and developing non-precious metal-based ORR catalysts， especially through defect engineering strategies to regulate and optimize the performance of non-precious metal catalysts， is crucial. Based on an in-depth explanation of the ORR mechanism， this article reviews the latest progress in the study of ORR using defective non-precious metal catalysts. It discusses the effects of intrinsic defects such as edge defects， vacancies， topological defects， and heteroatom doping on catalytic activity. At the same time， it outlines the key roles played by these defects in promoting specific electron transfer pathways in ORR. Additionally， it reviews the potential applications of defects in single-atom catalysts， di-atom catalysts， and metal oxides in ORR. Finally， this article looks forward to the future research directions of ORR catalysts. Due to their unique structure and composition， defective non-precious metal materials show broad application prospects in catalyzing ORR.