Carbon‐Nanoplated CoS@TiO2 Nanofibrous Membrane: An Interface‐Engineered Heterojunction for High‐Efficiency Electrocatalytic Nitrogen Reduction

Abstract Developing noble‐metal‐free electrocatalysts is important to industrially viable ammonia synthesis through the nitrogen reduction reaction (NRR). However, the present transition‐metal electrocatalysts still suffer from low activity and Faradaic efficiency due to poor interfacial reaction kinetics. Herein, an interface‐engineered heterojunction, composed of CoS nanosheets anchored on a TiO 2 nanofibrous membrane, is developed. The TiO 2 nanofibrous membrane can uniformly confine the CoS nanosheets against agglomeration, and contribute substantially to the NRR performance. The intimate coupling between CoS and TiO 2 enables easy charge transfer, resulting in fast reaction kinetics at the heterointerface. The conductivity and structural integrity of the heterojunction are further enhanced by carbon nanoplating. The resulting C@CoS@TiO 2 electrocatalyst achieves a high ammonia yield (8.09×10 −10 mol s −1 cm −2 ) and Faradaic efficiency (28.6 %), as well as long‐term durability.