Activating VS basal planes for enhanced NRR electrocatalysis: the synergistic role of S-vacancies and B dopants

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2020-08, Vol.8 (32), p.16195-1622
• Main Authors: Li, Qingqing, Guo, Yali, Tian, Ye, Liu, Wuming, Chu, Ke
• Format: Article
• Language: English
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d0ta05282e

The nitrogen reduction reaction (NRR) is a pivotal step in electrochemical N 2 fixation to NH 3 . 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 μg 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. The synergistic role of S-vacancies and B-dopants enables the effective activation of VS 2 basal planes for achieving dramatically enhanced NRR activity.