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Ni-Doped Mo2C Anchored on Graphitized Porous Carbon for Boosting Electrocatalytic N2 Reduction.

Facilitating the efficient activation of N2 molecules and inhibiting the competing hydrogen evolution reaction remain a challenge in the nitrogen reduction reaction (NRR). A heteroatom doping strategy is an effective way to optimize the energy barrier during the NRR process to improve the catalytic efficiency. Herein, we report Ni-doped Mo2C anchored on graphitized porous conductive carbon for regulating the electronic structure and catalytic properties of electrocatalysts toward NRR. Benefiting from the porous structure and graphitization features of the carbon matrix, more active sites and high electronic conductivity were achieved. Meanwhile, with the doping of Ni atoms, the electronic configuration near the Ni-Mo active sites was optimized and the adsorption of N2 on them was also promoted due to the increased electron transfer. Moreover, the lowered energy barrier of the NRR process and the suppressed hydrogen adsorption on the active site all resulted in the high catalytic activity and selectivity of the catalyst. Therefore, a high NH3 yield rate of 46.49 μg h-1 mg-1 and a faradic efficiency of 29.05% were achieved. This work not only validates the important role of heteroatom doping on the regulation of NRR catalytic activity but also provides a promising avenue for the green synthesis of NH3.