电催化剂
电子转移
化学动力学
电解质
格式化
贵金属
动力学
氢
材料科学
化学
催化作用
化学物理
金属
无机化学
电化学
离解(化学)
过电位
物理化学
电极
物理
生物化学
量子力学
作者
Onyu Jung,Megan N. Jackson,Ryan P. Bisbey,Nicole E. Kogan,Yogesh Surendranath
出处
期刊:Joule
[Elsevier]
日期:2022-02-01
卷期号:6 (2): 476-493
被引量:8
标识
DOI:10.1016/j.joule.2022.01.007
摘要
Summary
The hydrogen evolution reaction (HER) is a critical transformation for a renewable energy economy and an ideal testbed for refining mechanistic models of interfacial electrocatalysis. The HER is less efficient in alkaline than in acidic electrolytes; however, the mechanistic origin of this is widely debated. Activation-controlled kinetics at intermediate pH are non-existent due to pH swings or buffer convolution, impeding mechanistic analysis. We identify formate and borate as buffers that minimally perturb the HER kinetics on Au and Pt and report activation-controlled kinetic data between pH 1 and 12. We find that the reaction order in H3O+ is fractional across the pH range as a result of intermediate metal–H coverage and propose that efficiency loss arises from slow proton-coupled electron transfer (PCET) of H2O versus H3O+. These studies highlight the role of surface coverage in electrocatalytic kinetics and motivate strategies to promote efficient PCET in alkaline media.
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