The present work introduces a novel catalytic strategy to promote the nitrogen reduction reaction (NRR) by employing a cooperative Cu-based single-atom alloy (SAA) and oriented external electric fields (OEEFs) as catalysts. The field strength (F)-dependent reaction pathways are investigated by means of first-principles calculations. Different dipole-induced responses of intermediates to electric fields break the original scaling relationships and effectively tune not only the activity but also the product selectivity of the NRR. When the most active Os₁Cu SAA is taken as an example, in the absence of an OEEF, the overpotential (η) of the NRR is 0.62 V, which is even larger than that of the competitive hydrogen evolution reaction (HER). A negative field not only reduces η but switches the preference to the NRR over the HER. In particular, η at F = −1.14 V/Å reaches the bottom of 0.18 V, which is 70% lower than that in the field-free state.

中文翻译：

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电场下单原子合金刺激-响应集成催化电化学氮还原机理研究

目前的工作介绍了一种新颖的催化策略，通过采用协同铜基单原子合金（SAA）和定向外部电场（OEEF）作为催化剂来促进氮还原反应（NRR）。通过第一性原理计算研究了场强 ( F ) 相关的反应路径。中间体对电场的不同偶极诱导响应打破了原始的标度关系，不仅有效地调节了 NRR 的活性，而且还调节了产物选择性。以最活跃的Os ₁ Cu SAA为例，在没有OEEF的情况下，NRR的过电势（η）为0.62 V，甚至比竞争性析氢反应（HER）的过电势还要大。负场不仅会降低 η，还会优先选择 NRR 而不是 HER。特别是，F = -1.14 V/Å 时的 η 达到 0.18 V 的底部，比无场状态下低 70%。