Abstract
Ammonia is among the available sustainable fuels for humans in the future. Electrochemical nitrogen fixation, which is a promising ammonia synthesis method, can achieve artificial N2 fixation at room temperature and pressure. We report that 5% Co4N/Co2C@rGO is a high-efficiency nitrogen reduction reaction electrocatalyst for ammonia synthesis under ambient conditions. The catalyst obtains high NH3 yield (24.12 μg h–1 mgcat–1) and Faradaic efficiency (24.97%) at −0.1 V (vs RHE) in 0.1 M HCl. The addition of graphene reduces CoN to Co2C and Co4N. A high ratio of Co–C bonds improves NRR performance. The excellent performance of the catalyst is attributed to the high proportion of pyridine N and pyrrole N. Data analysis results show that the NRR on the surface of Co4N adopts a favorable Mars–van Krevelen reaction mechanism. Moreover, the Co2C(101) crystal plane is more conducive to NRR.
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