Achieving precise control and an accurate understanding of reaction processes that occur on catalysts at the molecular level is still challenging yet crucial to digging out ideal materials for the nitrate reduction reaction (NO3RR). Considering the representativeness of non-precious metal catalysts and the adjustability of their d electronic states, NiFe bimetallic nanocatalysts with various content ratios were synthesized to evaluate their positive characteristics on the electrochemical NO3RR. Eventually, the Ni0.7Fe0.3 sample inclined toward the cubic FeNi3 structure was proven to have the best electrocatalytic NO3RR performance: 13.61 mol g−1 h−1 ammonia production efficiency (APE) and 99.53% Faradaic efficiency (FE) under 1 M KNO3 and 47.94 mmol g−1 h−1 APE and 95.04% FE under 1 mM KNO3, superior to most reported electrocatalysts. Moreover, the above data outline the complete evolution of the distinct nitrogen-containing intermediate restricted by the NiFe-based asymmetric bridge structure.

中文翻译：

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基于 NiFe 双金属位点的不对称桥结构用于优化硝酸盐还原反应


在分子水平上实现对催化剂上发生的反应过程的精确控制和准确理解仍然具有挑战性，但对于挖掘硝酸盐还原反应 （NO3RR） 的理想材料至关重要。考虑到非贵金属催化剂的代表性及其 d 电子态的可调性，合成了不同含量比的 NiFe 双金属纳米催化剂，以评价其对电化学 NO3RR 的积极特性。最终，倾向于立方 FeNi3 结构的 Ni0.7Fe0.3 样品被证明具有最佳的电催化 NO3RR 性能：13.61 mol g-1 h-1 氨生产效率 （APE） 和 99.53% 法拉第效率 （FE），在 1 mM KNO3 下为 47.94 mmol g-1 h-1 APE 和 95.04% FE，优于大多数报道的电催化剂。此外，上述数据概述了受 NiFe 基不对称桥结构限制的不同含氮中间体的完整演变。