N₂ electrolysis has been impeded by efficient catalysts for key reactions: cathodic nitrogen reduction reaction (NRR) and anodic oxygen evolution reaction (OER). A bifunctional nickel, iron-nanomesh array electrocatalyst has been developed characteristic of excellent structural features for favorable NRR and OER processes, including highly exposed active sites originated from sub-nanometer-thick nanomeshes, hierarchical porosity resulting from the array-arranged nanolayers, and binary nickel, iron active sites. The electrode demonstrates excellent NRR activity with an ammonia yield of 16.89 μg h^–1 mg^–1_cat and a faradaic efficiency (FE) of 12.50% at −350 mV (vs RHE), in addition to OER activity with a small overpotential of 191 mV to achieve 10 mA cm^–2. Consequently, a full N₂ electrolysis system has been constructed that exhibits remarkable ammonia production performance with an ammonia yield of 2.07 μg h^–1 mg^–1_cat at 1.9 V, an FE of 9.87% at 1.6 V, and good durability for 30 h. Further mechanism study through density function theory shows that the NRR proceeds via an associative distal pathway, whereas the free energies for the N₂* → NNH* intermediate step in the NRR as well as the OH* + H₂O → O* + H₂O intermediate step in the OER can be reduced by tuning the catalysts’ electronic structure by the strong synergistic effect between nickel and iron.

中文翻译：

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二维纳米网格阵列作为N ₂电解的双功能催化剂

N ₂电解已被关键反应的有效催化剂阻碍：阴极氮还原反应（NRR）和阳极氧释放反应（OER）。已开发出一种双功能镍铁纳米阵列电催化剂，具有出色的结构特征，适用于良好的NRR和OER工艺，包括源自亚纳米级纳米网孔的高度暴露的活性位，由阵列排列的纳米层产生的分层孔隙以及二元镍，铁的活性位点。电极显示出优异的NRR活性，氨产量为16.89μgh ^–1 mg ^–1_猫在−350 mV（vs RHE）下，法拉第效率（FE）为12.50％，除了OER活性外，还具有191 mV的小过电位以达到10 mA cm ^–2。因此，构建了一个完整的N ₂电解系统，该系统具有出色的氨生产性能，在1.9 V下的氨产量为2.07μgh ^–1 mg ^–1 _cat，在1.6 V下的FE为9.87％，并且在30 h下具有良好的耐久性。通过密度泛函理论的进一步机理研究表明，NRR通过相关的远端路径进行，而NRR中的N ₂ *→NNH *中间步骤以及OH * + H ₂ O→O * + H的自由能₂通过利用镍和铁之间的强协同作用来调节催化剂的电子结构，可以减少OER的中间步骤。