Issue 4, 2022

Amorphization engineered VSe2−x nanosheets with abundant Se-vacancies for enhanced N2 electroreduction

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.

Graphical abstract: Amorphization engineered VSe2−x nanosheets with abundant Se-vacancies for enhanced N2 electroreduction

Supplementary files

Article information

Article type
Communication
Submitted
08 Mha 2021
Accepted
23 N’w 2021
First published
24 N’w 2021

J. Mater. Chem. A, 2022,10, 1742-1749

Amorphization engineered VSe2−x nanosheets with abundant Se-vacancies for enhanced N2 electroreduction

Y. Luo, Q. Li, Y. Tian, Y. Liu and K. Chu, J. Mater. Chem. A, 2022, 10, 1742 DOI: 10.1039/D1TA06746J

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