Coupled cation–electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL Nature Catalysis Pub Date : 2025-01-13 DOI:10.1038/s41929-024-01279-1

Kaiyue Zhao, Mingchuan Luo, Yongfan Zhang, Xiaoxia Chang, Bingjun Xu

引用次数: 0

Abstract

Electrochemical interfaces between polymer electrolytes and electrodes are central to electrochemical devices in the global transition towards renewable energy. Here we show that the adsorption and desorption of sulfonates in Nafion on Pt(111) involve distinct elementary steps, with the latter proceeding through a coupled cation–electron transfer. Adsorbed sulfonates not only block a fraction of surface Pt sites but, more importantly, generate two additional types of surface adsorbate, OH_Nafion and O_Nafion, which exhibit distinct kinetic properties from adsorbed OH and O on bare Pt(111), respectively. The impact of the adsorption of sulfonate groups in Nafion on the activity of the oxygen reduction reaction (ORR) on Pt cannot be rationalized by existing thermodynamic descriptors. The reduced ORR activity on the Nafion-covered Pt(111) is caused by the kinetically hindered *O→*OH conversion and *OH reduction on sites close to adsorbed sulfonates.

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.