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Effect of oxygen coordination on the electrocatalytic nitrogen fixation of a vanadium single-atom catalyst embedded in graphene.
- Source :
- New Journal of Chemistry; 12/21/2022, Vol. 46 Issue 47, p22936-22943, 8p
- Publication Year :
- 2022
-
Abstract
- The rational design of efficient electrocatalysts for nitrogen reduction reaction (NRR) to produce NH<subscript>3</subscript> under ambient condition is a longstanding challenge. The graphene-based single-atom catalyst (SAC) has been revealed as a promising candidate. Previous studies mainly focused on the metal center coordinated with N atoms, while those coordinated with other heteroatoms were rarely reported. Herein, we theoretically investigated the effect of oxygen coordination on the performance of vanadium (V) SAC embedded in graphene (VO<subscript>4</subscript>/G) towards NRR owing to the fact that V with less d electrons usually exhibits high chemical activity. It is revealed that VO<subscript>4</subscript>/G with good stability can efficiently convert N<subscript>2</subscript> into NH<subscript>3</subscript> through a distal mechanism with a low limiting potential of −0.60 V, which is superior to the experimentally synthesized FeN<subscript>4</subscript>/G and FeO<subscript>4</subscript>/G SACs. Moreover, the stronger adsorption of N<subscript>2</subscript> than the H atom renders the high NRR selectivity of VO<subscript>4</subscript>/G against the competing hydrogen evolution reaction, and the rapid removal of the produced NH<subscript>3</subscript> endows VO<subscript>4</subscript>/G with excellent recyclability. The good stability, high catalytic activity and selectivity, and excellent recyclability make VO<subscript>4</subscript>/G a prospective NRR catalyst. This work provides a promising NRR electrocatalyst awaiting experimental exploration and will stimulate further studies on other coordination atoms beyond N for graphene-based SAC. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 11440546
- Volume :
- 46
- Issue :
- 47
- Database :
- Complementary Index
- Journal :
- New Journal of Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 160586821
- Full Text :
- https://doi.org/10.1039/d2nj04716k