Exploring new catalysts for nitrogen reduction at ambient pressures and temperatures with ultrahigh ammonia (NH₃) yield and selectivity is still a giant challenge. In this work, atomic catalysts with separated Pd atoms on graphdiyne (Pd-GDY) have been synthesized and show fascinating electrocatalytic properties for nitrogen reduction. Outstandingly, the catalyst shows the highest average NH₃ yield of 4.45 ± 0.30 mg_NH3 mg_Pd⁻¹ h⁻¹, almost tens of orders larger than previously reported ones, and 100% reaction selectivity in neutral media. And Pd-GDY exhibits almost no decreases in the NH₃ yield and Faradaic efficiency. Density functional theory calculations show that the reaction pathway prefers to perform at the (Pd, C1, C2) active area due to the strongly coupled (Pd, C1, C2) which elevates the selectivity via enhanced electron-transfer. By adjusting the p-d coupling accurately, the reduction of self-activated nitrogen is promoted by anchoring atom selection, and the side effects are minimized.

中文翻译：

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石墨炔基金属原子合成氨催化剂


探索在环境压力和温度下具有超高氨（NH ₃ ）收率和选择性的新型氮还原催化剂仍然是一个巨大的挑战。在这项工作中，合成了石墨二炔上具有分离的 Pd 原子的原子催化剂 (Pd-GDY)，并显示出令人着迷的氮还原电催化性能。值得注意的是，该催化剂显示出最高的平均NH ₃产率，为4.45 ± 0.30 mg _NH3 mg _Pd ^-1 h ^-1 ，几乎比之前报道的高出数十个数量级，并且在中性介质中具有100%的反应选择性。并且Pd-GDY几乎没有表现出NH ₃产率和法拉第效率的降低。密度泛函理论计算表明，由于强耦合（Pd，C1，C2）通过增强的电子转移提高了选择性，反应路径更倾向于在（Pd，C1，C2）活性区域进行。通过精确调节pd耦合，通过锚定原子选择促进自活化氮的还原，并将副作用降至最低。