气候变化领域集成服务门户(CCPortal): Interpreting Tafel behavior of consecutive electrochemical reactions through combined thermodynamic and steady state microkinetic approaches

CCPortal

DOI	10.1039/c9ee02697e
	Interpreting Tafel behavior of consecutive electrochemical reactions through combined thermodynamic and steady state microkinetic approaches
	Mefford J.T.; Zhao Z.; Bajdich M.; Chueh W.C.
发表日期	2020
ISSN	1754-5692
起始页码	622
结束页码	634
卷号	13 期号:2
英文摘要	Assessing the reaction pathway of multi-electron-transfer reactions is an essential yet difficult task for the rational design of electrocatalysts. In this work, we develop a heuristic approach that combines thermodynamic adsorption energetics calculated through density functional theory with microkinetic modeling using the steady state approximation to interpret the potential-dependent Tafel behavior of consecutive electrochemical reactions. In doing so, we introduce a kinetic framework for ab initio calculations that ensures self-consistent adsorption energetics based on kinetically limited adsorbate coverages. The approach is applied to experimental results on CoOx(OH)2-x single crystal electrocatalyst particles yielding coverage dependent mechanistic information and identification of the rate-limiting step with standard rate constants for the oxygen evolution reaction on the (1120) surfaces of the β-Co(OH)2, β-CoOOH, and CoO2 bulk phases. This generalizable method enables catalyst benchmarking based on determining the active species involved and associated intrinsic reaction rate constants in consecutive multi-electron-transfer reactions. © 2020 The Royal Society of Chemistry.
语种	英语
scopus关键词	Calculations; Density functional theory; Electrocatalysts; Electron transitions; Heuristic methods; Rate constants; Single crystals; Ab initio calculations; Adsorption energetics; Electrochemical reactions; Intrinsic reaction rate; Microkinetic modeling; Standard rate constant; Steady state approximation; Thermodynamic adsorption; Oxygen evolution reaction; benchmarking; catalyst; cobalt; design method; electrochemistry; energetics; kinetics; reaction rate; thermodynamics
来源期刊	Energy and Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/162674
作者单位	Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, United States; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, United States; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, United States
推荐引用方式 GB/T 7714	Mefford J.T.,Zhao Z.,Bajdich M.,et al. Interpreting Tafel behavior of consecutive electrochemical reactions through combined thermodynamic and steady state microkinetic approaches[J],2020,13(2).
APA	Mefford J.T.,Zhao Z.,Bajdich M.,&Chueh W.C..(2020).Interpreting Tafel behavior of consecutive electrochemical reactions through combined thermodynamic and steady state microkinetic approaches.Energy and Environmental Science,13(2).
MLA	Mefford J.T.,et al."Interpreting Tafel behavior of consecutive electrochemical reactions through combined thermodynamic and steady state microkinetic approaches".Energy and Environmental Science 13.2(2020).