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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	17545692
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.
英文关键词	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
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/189699
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 & 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 & Environmental Science 13.2(2020).