期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 15, 页码 17273-17281出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c00280
关键词
Ni doping; Mo2C; graphitized porous carbon; nitrogen reduction reaction; electrocatalysis
资金
- National Natural Science Foundation of China [52101182]
This study presents a Ni-doped Mo2C catalyst anchored on carbon matrix for efficient nitrogen reduction reaction (NRR). The catalyst was designed to regulate electronic structure and catalytic properties, leading to high catalytic activity and selectivity. The heteroatom doping and porous structure design optimize the electronic configuration and N-2 adsorption, resulting in lowered energy barrier and improved catalytic performance. As a result, a high NH3 yield rate and faradic efficiency were achieved, demonstrating the importance of heteroatom doping in NRR.
Facilitating the efficient activation of N-2 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 N-2 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 mu g 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.
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