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A Challenge to the G similar to 0 Interpretation of Hydrogen Evolution

机译：对G类似于0解释的氢演化的挑战

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摘要

Platinum is a nearly perfect catalyst for the hydrogen evolution reaction, and its high activity has conventionally been explained by its close-to-thermoneutral hydrogen binding energy (G similar to 0). However, many candidate nonprecious metal catalysts bind hydrogen with similar strengths but exhibit orders-of-magnitude lower activity for this reaction. In this study, we employ electronic structure methods that allow fully potential-dependent reaction barriers to be calculated, in order to develop a complete working picture of hydrogen evolution on platinum. Through the resulting ab initio microkinetic models, we assess the mechanistic origins of Pt's high activity. Surprisingly, we find that the G similar to 0 hydrogen atoms are inert in the kinetically relevant region and that the active hydrogen atoms have Delta G's much weaker, similar to that of gold. These on-top hydrogens have particularly low barriers, which we compare to those of gold, explaining the high reaction rates, and the exponential variations in coverage lead directly to Pt's strong kinetic response to the applied potential. This explains the unique reactivity of Pt that is missed by conventional Sabatier analyses and suggests true design criteria for nonprecious alternatives.
机译：铂是氢进化反应的近乎完美的催化剂，其高活性通常通过其近温度氢结合能（G类似于0）来解释。然而，许多候选的非普烈金属催化剂与相似的强度结合氢，但表现出该反应的倍率下降的活性。在这项研究中，我们采用了允许计算完全潜在的反应障碍的电子结构方法，以便在铂中开发氢气进化的完整工作情况。通过由此产生的AB Initio MicroInetic模型，我们评估了PT的高活动的机制起源。令人惊讶的是，我们发现类似于0氢原子的G在动力学相关区域中是惰性的，并且活性氢原子具有Delta G的更弱，类似于金。这些顶部氢的屏障特别低，我们与黄金的屏障相比，解释了高反应速率，以及覆盖率的指数变化直接引导到PT对施加电位的强烈动力学响应。这解释了传统的萨巴替尔分析错过的PT的独特反应性，并表明了非审视替代品的真实设计标准。

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