Green and environmentally friendly electrocatalytic nitrogen (N₂) fixation to synthesize ammonia (NH₃) is recognized as an effective method to replace the traditional Haber–Bosch process. However, the difficulties in N₂ adsorption and fracture of hard N≡N bond still remain major challenges in electrocatalytic N₂ reduction reactions (NRR). From the perspectives of enhancing N₂ adsorption and providing more catalytic sites, two-dimensional (2D) FeS₂ nanosheets and three-dimensional (3D) metal organic framework-derived ZnS embedded within N-doped carbon polyhedras are grown on the carbon cloth (CC) template in this work. Thus, a composite NRR catalyst with multi-dimensional structures, which is signed as FeS₂/ZnS-NC@CC, is obtained for using over a wide pH range. The uniform distribution of hollow ZnS-NC frameworks and FeS₂ nanosheets on the surface of CC largely increase the N₂ enrichment efficiency and offer more active sites, while the CC skeleton acts as an independent conductive substrate and S-doping helps promote the fracture of N≡N bond during the NRR reaction. As a result, the FeS₂/ZnS-NC@CC electrode achieves a high Faraday efficiency of 46.84% and NH₃ yield of 58.52 μg h⁻¹ mg⁻¹ at -0.5 V vs. Ag/AgCl in 0.1 M KOH. Furthermore, the FeS₂/ZnS-NC@CC electrode displays excellent NRR catalytic activity in acidic and neutral electrolytes as well, which outperforms most previously reported electrocatalysts including noble metals. Therefore, this work provides a new way for the design of multi-dimensional electrocatalysts with excellent electrocatalytic efficiency and stability for NRR applications.

绿色的环保电催化氮（N ₂）固定到合成氨（NH ₃）被认为是取代传统的哈柏法的有效方法。然而，在电催化N ₂还原反应（NRR）中，N ₂吸附和硬N≡N键断裂的困难仍然是主要挑战。从增强N ₂吸附并提供更多催化位点的角度来看，二维（2D）FeS ₂在这项工作中，在碳布（CC）模板上生长了嵌入N掺杂的碳多面体中的纳米片和三维（3D）金属有机骨架衍生的ZnS。因此，获得了具有宽结构的复合NRR催化剂，其被标记为FeS ₂ / ZnS-NC @ CC，用于在宽的pH范围内使用。空心ZnS-NC骨架和FeS ₂纳米片在CC表面上的均匀分布大大提高了N _2的富集效率并提供了更多的活性位，而CC骨架充当了独立的导电基底，S掺杂有助于促进Al的断裂。 NRR反应中的N≡N键。结果，FeS ₂ / ZnS-NC @ CC电极实现了46.84％的法拉第效率和NH ₃的高效率。在-0.5 V时相对于0.1 M KOH中的Ag / AgCl的收率为58.52μgh ^-1  mg ^-1 此外，FeS ₂ / ZnS-NC @ CC电极在酸性和中性电解质中也显示出出色的NRR催化活性，其性能优于大多数先前报道的包括贵金属的电催化剂。因此，这项工作为设计具有优异电催化效率和稳定性的多维电催化剂提供了一种新方法，适用于NRR应用。