Journal
SMALL
Volume 18, Issue 47, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202204557
Keywords
electrocatalytic hydrogen evolution reaction; pH universal; single atom defects; single vacancy defects; VSe; (2)
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Funding
- National Natural Science Foundation of China [52072182, U1732126, 51872145]
- Natural Science Foundation of Jiangsu Province [BK20211278]
- China Postdoctoral Science Foundation [2019M650120, 2020M671554]
- National Synergetic Innovation Center for Advanced Materials (SICAM)
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A facile and scalable atomic-level di-defect strategy has been reported in this study to improve the electrocatalytic hydrogen evolution reaction (HER) performance through defect engineering of VSe2 nanoflakes. The di-defect configuration effectively triggers the electrocatalytic activity of the inert VSe2 basal plane, leading to superior performance compared to previously reported non-noble metal HER electrocatalysts.
Defect engineering of transition metal dichalcogenides (TMDCs) is important for improving electrocatalytic hydrogen evolution reaction (HER) performance. Herein, a facile and scalable atomic-level di-defect strategy over thermodynamically stable VSe2 nanoflakes, yielding attractive improvements in the electrocatalytic HER performance over a wide electrolyte pH range is reported. The di-defect configuration with controllable spatial relation between single-atom (SA) V defects and single Se vacancy defects effectively triggers the electrocatalytic HER activity of the inert VSe2 basal plane. When employed as a cathode, this di-defects decorated VSe2 electrocatalyst requires overpotentials of 67.2, 72.3, and 122.3 mV to reach a HER current density of 10 mA cm(-2) under acidic, alkaline, and neutral conditions, respectively, which are superior to most previously reported non-noble metal HER electrocatalysts. Theoretical calculations reveal that the reactive microenvironment consists of two adjacent SA Mo atoms with two surrounding symmetric Se vacancies, yielding optimal water dissociation and hydrogen desorption kinetics. This study provides a scalable strategy for improving the electrocatalytic activity of other TMDCs with inert atoms in the basal plane.
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