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

Developing noble-metal-free electrocatalysts is of utmost importance to industrially viable ammonia synthesis through 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 TiO2 nanofibrous membrane, is developed. As an active matrix, the TiO2 nanofibrous membrane can uniformly confine the CoS nanosheets against agglomeration, and contribute substantially to the NRR performance. The intimate coupling between CoS and TiO2 enables easy carrier transport in between, resulting in fast reaction kinetics at the heterointerface. Moreover, the conductivity and structural integrity of the heterojunction are further enhanced by carbon nanoplating. Profited by this interfacial design, the resulting C@CoS@TiO2 electrocatalyst achieves strikingly high ammonia yield (8.09×10-10 mol s-1 cm-2) and Faradaic efficiency (28.6%), as well as superior long-term durability.

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