Two-dimensional (2D) transition metal compounds have been explored as promising catalysts in dinitrogen electroreduction (NRR) for ammonia synthesis, while the immense basal planes of the 2D materials are inert towards the electrocatalysis. Herein, we report a porous exfoliated FePS₃ nanosheet with rich sulfur vacancy (Vs-FePS₃ NSs) synthesized by electrochemical exfoliation and hydrogenation treatment. Owing to the rich sulfur vacancy and unique 2D morphology with a thickness of ~15 nm and lateral dimension of ~500 nm, Vs-FePS₃ NSs show an excellent activity in electrochemical NRR with a high Faradaic efficiency of 12.36% at − 0.20 V and an ammonia yield rate of 3.88 μg h⁻¹ cm⁻² at − 0.25 V versus reversible hydrogen electrode in acid. Experimental observations reveal the Fe species as real active sites and S vacancies for hydrogenation of N₂ toward a synergistic effect for enhanced NRR. In addition, Vs-FePS₃ NSs can serve as the cathode of a Zn-N₂ battery to achieve a power density of 2.6 mW cm⁻².

二维（2D）过渡金属化合物已被开发为氨合成二氮电还原（NRR）中有希望的催化剂，而2D材料的巨大基面对电催化是惰性的。在本文中，我们报道了通过电化学剥落和氢化处理合成的具有丰富的硫空位（Vs-FePS ₃ NSs）的多孔剥落的FePS ₃纳米片。Vs-FePS ₃ NSs具有丰富的硫空位和独特的2D形态，厚度约为15 nm，侧面尺寸约为500 nm，在电化学NRR中表现出出色的活性，在-0.20 V和2.50 V时具有高达12.36％的法拉第效率。氨水产率为3.88μgh ^-1 cm ^-2在-0.25 V时相对于可逆氢电极在酸中。实验观察表明，Fe物种是真实的活性位点和S空位，用于N _2的氢化，朝着增强NRR的协同效应起作用。此外，Vs-FePS ₃ NSs可以用作Zn-N ₂电池的阴极，以实现2.6 mW cm ^-2的功率密度。