期刊
ACS NANO
卷 16, 期 5, 页码 7915-7925出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c00596
关键词
electrocatalytic reduction reaction; water-in-salt electrolytes; density functional theory calculations; molecular dynamics simulations; in situ spectroscopy
类别
资金
- National Natural Science Foundation of China [52161025]
- Natural Science Foundation of Gansu Province [20JR10RA241]
Combining catalyst and electrolyte engineering, a high-efficiency electrocatalytic nitrogen reduction reaction (NRR) is achieved using a Se-vacancy-rich WSe2-x catalyst in water-in-salt electrolyte (WISE), which suppresses H2 evolution, improves N2 affinity, and enhances active site pi-back-donation ability for promoting both activity and selectivity of NRR. The WSe2-x in 12m LiClO4 exhibits excellent faradaic efficiency and NH3 yield, among the highest reported to date.
Electrocatalytic nitrogen reduction reaction (NRR) is a promising approach for renewable NH 3 production, while developing the NRR electrocatalysis systems with both high activity and selectivity remains a significant challenge. Herein, we combine catalyst and electrolyte engineering to achieve a high-efficiency NRR enabled by a Se-vacancy-rich WSe2-x, catalyst in water-in-salt electrolyte (WISE). Extensive characterizations, theoretical calculations, and in situ X-ray photoelectron/Raman spectroscopy reveal that WISE ensures suppressed H-2 evolution, improved N-2 affinity on the catalyst surface, as well as an enhanced pi-back-donation ability of active sites, thereby promoting both activity and selectivity for the NRR. As a result, an excellent faradaic efficiency of 62.5% and NH3 yield of 181.3 mu g h(-1) mg(-1) is achieved with WSe2-x in 12 m LiClO4, which is among the highest NRR performances reported to date.
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