Reconciling the Volcano Trend with the Butler–Volmer Model for the Hydrogen Evolution Reaction
Reconciling the Volcano Trend with the Butler–Volmer Model for the Hydrogen Evolution Reaction
复制标题
协调火山趋势与析氢反应的巴特勒·沃尔默模型
DOI：
10.1021/acs.jpclett.2c01411
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Saidi, Wissam A.
中科院分区：
文献类型：
--
作者：
Yang, Timothy T.;Saidi, Wissam A.
在计算化学中，火山趋势已被广泛用于预测新的最佳催化剂，而在分析化学中，Butler-Volmer关系是解释循环伏安法电流-电位特性的标准。在这里，我们开发了一个电化学模型的析氢反应交换电流，调和设备级化学，原子级火山的趋势，和巴特勒-沃尔默关系。我们表明，该模型是一个易于计算的氢吸附能总是从第一原理原子模拟的函数。此外，该模型再现高保真度的实验交换电流超过15个数量级的元素金属催化剂，并与最近提出的基于数据驱动的方法的分析模型是一致的。我们的研究结果基于基本的电化学原理是普遍的，可以应用到其他反应，包括CO2还原，金属氧化，和锂（脱）插反应。
The volcano trend has been widely utilized to forecast new optimum catalysts in computational chemistry while the Butler–Volmer relationship is the norm to explain current–potential characteristics from cyclic voltammetry in analytical chemistry. Herein, we develop an electrochemical model for hydrogen evolution reaction exchange currents that reconciles device-level chemistry, atomic-level volcano trend, and the Butler–Volmer relation. We show that the model is a function of the easy-to-compute hydrogen adsorption energy invariably obtained from first-principles atomic simulations. In addition, the model reproduces with high fidelity the experimental exchange currents for elemental metal catalysts over 15 orders of magnitude and is consistent with the recently proposed analytical model based on a data-driven approach. Our findings based on fundamental electrochemistry principles are general and can be applied to other reactions including CO2reduction, metal oxidation, and lithium (de)intercalation reactions.