Amorphization engineered VSe2−x nanosheets with abundant Se-vacancies for enhanced N2 electroreduction. Issue 4 (13th January 2022)

• Record Type: Journal Article
• Authors: Luo, Yaojing; Li, Qingqing; Tian, Ye; Liu, Yaping; Chu, Ke
• Is Part Of: Journal of materials chemistry. Volume 10:Issue 4(2022)
• Page Start: 1742
• Page End: 1749
• Publication Date: 2022-01-13
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1ta06746j
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Amorphous VSe2− x nanosheets with abundant Se-vacancies (VSe ) showed dramatically enhanced NRR activity and selectivity, attributed to the amorphization-triggered Se-vacancies that promote the NRR and impeding the H2 evolution. Abstract : Electrochemical N2 fixation through the nitrogen reduction reaction (NRR) is a promising route for sustainable NH3 synthesis, while exploring high-performance NRR catalysts lies at the heart of achieving high-efficiency NRR electrocatalysis. Herein, we reported the structural regulation of VSe2 by amorphization engineering, which simultaneously triggered the enriched Se-vacancies. The developed amorphous VSe2− x nanosheets with abundant Se-vacancies (a-VSe2− x ) delivered a much enhanced NRR activity with an NH3 yield of 65.7 μg h −1 mg −1 and a faradaic efficiency of 16.3% at −0.4 V, being 8.8- and 3.5-fold higher than those of their crystalline counterparts, respectively. Density functional theory computations combined with molecular dynamics simulations revealed that the amorphization-triggered Se-vacancies could induce the upraised d-band center of unsaturated V atoms, capable of promoting the binding of key *N2 /*NNH species to result in an energetically favorable NRR process.