计算pH 12和pH 14之间的析氧反应的Tafel斜率和反应级数，用于吸附物机理
Calculation of the Tafel slope and reaction order of the oxygen evolution reaction between pH 12 and pH 14 for the adsorbate mechanism
摘要：
尽管大量的实验和理论研究致力于析氧反应，OER的过渡金属氧化物的机制仍然存在争议。这部分是由于电化学参数的机制，如塔菲尔斜率和反应级数的模糊性。我们采取了最常见的假设吸附机制和计算的塔菲尔斜率和反应级数相对于pH值的基础上的微动力学分析。我们证明，可能的塔菲尔斜率的数量强烈依赖于一些先前的步骤和表面覆盖。此外，塔菲尔斜率成为pH值依赖性时，中间体的覆盖范围随pH值的变化。这些见解复杂化的一个限速步骤的识别由一个单一的塔菲尔斜率在一个单一的pH值。然而，模拟反应顺序互补塔菲尔斜率可以解决一些模糊性，以区分可能的限速步骤。最有洞察力的信息可以从塔菲尔图的低过电位区域获得。在这项工作中的模拟提供了明确的指导方针，实验者的识别的限制步骤中的吸附机制，使用观察到的值的塔菲尔斜率和反应顺序在pH值依赖性的研究。
英文摘要：
Despite numerous experimental and theoretical studies devoted to the oxygen evolution reaction, the mechanism of the OER on transition metal oxides remains controversial. This is in part owed to the ambiguity of electrochemical parameters of the mechanism such as the Tafel slope and reaction orders. We took the most commonly assumed adsorbate mechanism and calculated the Tafel slopes and reaction orders with respect to pH based on microkinetic analysis. We demonstrate that number of possible Tafel slopes strongly depends on a number of preceding steps and surface coverage. Furthermore, the Tafel slope becomes pH dependent when the coverage of intermediates changes with pH. These insights complicate the identification of a rate-limiting step by a single Tafel slope at a single pH. Yet, simulations of reaction orders complementary to Tafel slopes can solve some ambiguities to distinguish between possible rate-limiting steps. The most insightful information can be obtained from the low overpotential region of the Tafel plot. The simulations in this work provide clear guidelines to experimentalists for the identification of the limiting steps in the adsorbate mechanism using the observed values of the Tafel slope and reaction order in pH-dependent studies.
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