期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 8, 期 32, 页码 16195-16202出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta05282e
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
- Graduate Teaching Reform Project [JG201922]
The nitrogen reduction reaction (NRR) is a pivotal step in electrochemical N(2)fixation to NH3. VS(2)holds great promise as a NRR electrocatalyst, but its high activity requires the sufficient activation of inert basal planes. Herein, we demonstrate the first successful activation of VS(2)basal planes toward the NRR by introducing S-vacancies (Vs) and B-dopants. The theoretical calculations unravel that the synergistic role of V(S)and B-dopants enables the most effective activation of VS(2)basal planes by creating unique B-adjacent-unsaturated-V active sites that can significantly promote the NRR while suppressing hydrogen evolution. The synthesized B-doped VS(2)nanoflowers with enriched surface Vs delivered an NH(3)yield of 55.7 mu g h(-1)mg(-1)(-0.4 V) and a faradaic efficiency (FE) of 16.4% (-0.2 V) and represent the best V-based catalysts to date. Our theoretical and experimental findings may facilitate the exploration and understanding of advanced transition-metal disulfide catalysts for the NRR.
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