Autobifunctional Mechanism of Jagged Pt Nanowires for Hydrogen Evolution Kinetics via End-to-End Simulation
Autobifunctional Mechanism of Jagged Pt Nanowires for Hydrogen Evolution Kinetics via End-to-End Simulation
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DOI：
10.1021/jacs.0c11261
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发表时间：
2021-03-17
影响因子：
15
通讯作者：
Jung, Yousung
中科院分区：
文献类型：
--
作者：
Gu, Geun Ho;Lim, Juhyung;Jung, Yousung
锯齿状Pt纳米线的非凡质量活性可以显著提高析氢反应（HER）的经济性。然而，这是一个巨大的挑战，完全揭示锯齿状铂纳米线驱动的HER动力学与其多尺度形态。在这里，我们提出了一个端到端的框架，结合实验，机器学习和多尺度的进步，在过去的十年来阐明锯齿状Pt纳米线催化的HER动力学在碱性条件下。双功能催化通常是指通过两种不同催化剂的组合而协同增加活性。我们报告说，单金属，如锯齿状的铂纳米线，可以表现出双功能的特点，由于其复杂的表面形态，其中一个网站更喜欢电化学质子吸附和另一个负责激活，导致在4倍的活性增加。我们发现，传统的设计准则，具有0 eV的吉布斯吸附自由能的网站是最佳的HER不保持在碱性条件下，而是，-0.2和0.0 eV之间的能量被证明是最佳的。在反应温度下，高活性来自于低配位数（
The extraordinary mass activity of jagged Pt nanowires can substantially improve the economics of the hydrogen evolution reaction (HER). However, it is a great challenge to fully unveil the HER kinetics driven by the jagged Pt nanowires with their multiscale morphology. Herein we present an end-to- end framework that combines experiment, machine learning, and multiscale advances of the past decade to elucidate the HER kinetics catalyzed by jagged Pt nanowires under alkaline conditions. The bifunctional catalysis conventionally refers to the synergistic increase in activity by the combination of two different catalysts. We report that monometals, such as jagged Pt nanowires, can exhibit bifunctional characteristics owing to its complex surface morphology, where one site prefers electrochemical proton adsorption and another is responsible for activation, resulting in a 4-fold increase in the activity. We find that the conventional design guideline that the sites with a 0 eV Gibbs free energy of adsorption are optimal for HER does not hold under alkaline conditions, and rather, an energy between -0.2 and 0.0 eV is shown to be optimal. At the reaction temperatures, the high activity arises from low-coordination-number (