期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 267, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.118693
关键词
Electrocatalytic nitrogen fixation; Metal-free catalysts; Nitrogen vacancy; Sulphur doping; Density functional theory
资金
- National Natural Science Foundation of China [51761024]
- Feitian Scholar Program of Gansu Province
- CAS Light of West China Program
- Foundation of A Hundred Youth Talents Training Program of Lanzhou Jiaotong University
Exploring active and durable metal-free electrocatalysts represents a promising direction for electrocatalytic N-2 reduction reaction (NRR). Herein, by filling the nitrogen vacancies (NVs) with S dopants in graphitic C3N4, we showed that the resultant S-NV-C3N4 could be an efficient and robust metal-free NRR catalyst in neutral solution. S-NV-C3N4 with a high S concentration of 5.2 at.% exhibited a fascinating NRR performance with an NH3 yield of 32.7 mu g h(-1) mg(-1) and a Faradaic efficiency of 14.1 % at -0.4 V (vs. RHE), considerably outperforming pristine C3N4 and NV-containing C3N4. S-NV-C3N4 also showed exceptional durability for at least 20 h, in stark contrast to the inferior stability of NV-containing C3N4. Density functional theory calculations disclosed that the filled S dopants could break the scaling relation to effectively stabilize *N2H and destabilize *NH2 on S-NV-C3N4, leading to more optimized adsorption of NRR intermediates and a significantly reduced energy barrier. Meanwhile, the competitive HER can be effectively suppressed on S-NV-C3N4 due to the high energy barrier for water dissociation.
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