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深入了解铂族金属基碱性氢氧化催化剂的中间行为和设计策略。

Insight Into Intermediate Behaviors and Design Strategies of Platinum Group Metal-Based Alkaline Hydrogen Oxidation Catalysts.

作者信息

Su Lixin, Wu Hao, Zhang Shaokun, Cui Chenxi, Zhou Shengnan, Pang Huan

机构信息

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, Jiangsu, 225009, P. R. China.

State Key Laboratory of Coordination Chemistry, Nanjing University, Nanjing, Jiangsu, 210023, P. R. China.

出版信息

Adv Mater. 2025 Jan;37(4):e2414628. doi: 10.1002/adma.202414628. Epub 2024 Nov 19.

Abstract

Hydrogen oxidation reaction (HOR) can effectively convert the hydrogen energy through the hydrogen fuel cells, which plays an increasingly important role in the renewable hydrogen cycle. Nevertheless, when the electrolyte pH changes from acid to base, even with platinum group metal (PGM) catalysts, the HOR kinetics declines with several orders of magnitude. More critically, the pivotal role of reaction intermediates and interfacial environment during intermediate behaviors on alkaline HOR remains controversial. Therefore, exploring the exceptional PGM-based alkaline HOR electrocatalysts and identifying the reaction mechanism are indispensable for promoting the commercial development of hydrogen fuel cells. Consequently, the fundamental understanding of the HOR mechanism is first introduced, with emphases on the adsorption/desorption process of distinct reactive intermediates and the interfacial structure during catalytic process. Subsequently, with the guidance of reaction mechanism, the latest advances in the rational design of advanced PGM-based (Pt, Pd, Ir, Ru, Rh-based) alkaline HOR catalysts are discussed, focusing on the correlation between the intermediate behaviors and the electrocatalytic performance. Finally, given that the challenges standing in the development of the alkaline HOR, the prospect for the rational catalysts design and thorough mechanism investigation towards alkaline HOR are emphatically proposed.

摘要

氢氧化反应(HOR)能够通过氢燃料电池有效地转换氢能,这在可再生氢循环中发挥着越来越重要的作用。然而,当电解质的pH值从酸性变为碱性时,即使使用铂族金属(PGM)催化剂,氢氧化反应动力学也会下降几个数量级。更关键的是,在碱性氢氧化反应中,反应中间体和界面环境在中间行为过程中的关键作用仍存在争议。因此,探索优异的基于铂族金属的碱性氢氧化反应电催化剂并确定反应机理对于推动氢燃料电池的商业发展至关重要。因此,首先介绍了对氢氧化反应机理的基本理解,重点是不同反应中间体的吸附/解吸过程以及催化过程中的界面结构。随后,在反应机理的指导下,讨论了先进的基于铂族金属(基于Pt、Pd、Ir、Ru、Rh)的碱性氢氧化反应催化剂合理设计的最新进展,重点是中间行为与电催化性能之间的相关性。最后,鉴于碱性氢氧化反应发展中存在的挑战,着重提出了碱性氢氧化反应合理催化剂设计和深入机理研究的前景。

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