期刊
ADVANCED ENERGY MATERIALS
卷 12, 期 3, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202103022
关键词
density functional theory; electrocatalytic nitrogen reduction; heterostructures; in situ spectroscopy; molecular dynamics simulations; O-vacancies
类别
资金
- National Natural Science Foundation of China [51761024, 52161025]
- Natural Science Foundation of Gansu Province [20JR10RA241]
- Longyuan Youth Innovative and Entrepreneurial Talents Project [[2021]17]
- CAS Light of West China Program
- Longyuan Young Talents Program of Gansu Province
- Feitian Scholar Program of Gansu Province
In this study, vacancy and heterostructure engineering were integrated to develop O-vacancy-rich MoO3-x anchored on Ti3C2Tx-MXene as a highly active and selective NRR electrocatalyst. Experimental results demonstrated exceptional NRR activity, increased NH3 yield, and Faradaic efficiency for the catalyst.
The electrochemical N-2 reduction reaction (NRR) offers a promising approach for sustainable NH3 production, and modulating the structural/electronic configurations of the catalyst materials with optimized electrocatalytic properties is pivotal for achieving high-efficiency NRR electrocatalysis. Herein, vacancy and heterostructure engineering are rationally integrated to explore O-vacancy-rich MoO3-x anchored on Ti3C2Tx-MXene (MoO3-x/MXene) as a highly active and selective NRR electrocatalyst, achieving an exceptional NRR activity with an NH3 yield of 95.8 mu g h(-1) mg(-1) (-0.4 V) and a Faradaic efficiency of 22.3% (-0.3 V). A combination of in situ spectroscopy, molecular dynamics simulations and density functional theory computations is employed to unveil the synergistic effect of O-vacancies and heterostructures for the NRR, which demonstrates that O-vacancies on MoO3-x serve as the active sites for N-2 chemisorption and activation, while the MXene substrate can further regulate the O-vacancy sites to break the scaling relation to effectively stabilize *N-2/*N2H while destabilizing *NH2/*NH3, resulting in more optimized binding affinity of NRR intermediates toward reduced energy barriers and an enhanced NRR activity for MoO3-x/MXene.
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