电池阳极的Sabatier原理：异质界面上的化学动力学和可逆电沉积
The Sabatier principle for Battery Anodes: Chemical Kinetics and Reversible Electrodeposition at Heterointerfaces
摘要：
几个世纪以来，表面化学如何影响其上发生的反应一直是广泛科学和技术兴趣的长期问题。最近，它再次成为化学的一个分支学科-异相电化学中的一个关键问题，其中答案对人类如何以及以何种形式储存世界各地太阳能和风能装置产生的越来越多的可再生电功率具有影响。在这里，我们认为在这样的界面处的表面化学之间的关系和在可充电电池电极的电化学转化的可逆性。传统观点认为，金属沉积物和电极之间较强的化学相互作用促进可逆性。相反，我们报告说，沉积物和基板之间的化学相互作用的中等强度，既不太弱也不太强，使最高的可逆性和稳定性的电镀/剥离氧化还原过程在电池阳极。类似于化学多相催化的经验Sabatier原理，我们的发现来自于竞争过程的汇合-一个由电化学驱动，另一个由化学合金化驱动。基于当代感兴趣的电池阳极中的金属电镀/剥离系统的实验评估，我们表明，这些知识为基于地球丰富的低成本金属的高度可逆的电化学储能技术中的关键材料的设计提供了一个强大的工具。
英文摘要：
How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest for centuries. Recently, it has re-emerged as a critical question in a subdiscipline of chemistry - electrochemistry at heterointerphases, where the answers have implications for both how, and in what forms, humanity stores the rising quantities of renewable electric power generated from solar and wind installations world-wide. Here we consider the relation between the surface chemistry at such interphases and the reversibility of electrochemical transformations at a rechargeable battery electrode. Conventional wisdom holds that stronger chemical interaction between the metal deposits and electrode promotes reversibility. We report instead that a moderate strength of chemical interaction between the deposit and the substrate, neither too weak nor too strong, enables highest reversibility and stability of the plating/stripping redox processes at a battery anode. Analogous to the empirical Sabatier principle for chemical heterogeneous catalysis, our finding arises from the confluence of competing processes - one driven by electrochemistry and the other by chemical alloying. Based on experimental evaluation of metal plating/stripping systems in battery anodes of contemporary interest, we show that such knowledge provides a powerful tool for designing key materials in highly reversible electrochemical energy storage technologies based on earth-abundant, low-cost metals.
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