期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 8, 期 10, 页码 5200-5208出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta00220h
关键词
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资金
- National Natural Science Foundation of China [51761024]
- Feitian Scholar Program of Gansu Province
- Foundation of A Hundred Youth Talents Training Program of Lanzhou Jiaotong University
- CAS Light of West China Program
The development of highly efficient and durable electrocatalysts for the nitrogen reduction reaction (NRR) is of paramount significance for NH3 electrosynthesis. Herein, we report an effective B-doping strategy for the structural engineering of MnO2 toward the NRR through combined experimental and theoretical studies. Introducing B-dopants into MnO2 nanosheets was found to create abundant O-vacancies which cooperated with B-dopants to promote the conductivity and enhance the intrinsic NRR activity of MnO2. The developed B-doped MnO2 nanosheets grown on carbon cloth (B-MnO2/CC) exhibited a significantly enhanced NRR performance with an NH3 yield of 54.2 mu g h(-1) mg(-1) (-0.4 V) and a faradaic efficiency of 16.8% (-0.2 V), and are among the best Mn-based NRR catalysts reported so far. Density functional theory calculations further revealed the synergistic role of B-dopants and O-vacancies in inducing asymmetric charge distribution, which could activate the neighboring Mn atoms to facilitate the stabilization of the key intermediate *N2H on MnO2, leading to reduced reaction energy barrier and enhanced intrinsic NRR activity.
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