Issue 24, 2024

Enhancing the electronic structure of Ni-based electrocatalysts through N element substitution for the hydrogen evolution reaction

Abstract

The weak orbital coupling between Ni3N and H2O, caused by its interstitial structure and attenuated Ni–N interaction, is attributed to the high unoccupied d orbital energy of Ni3N. Consequently, the kinetics for water dissociation in the HER are slow. In this study, we effectively lowered the energy state of vacant d orbitals in Ni3N, which resulted in an exceptionally efficient HER. The as-synthesized Ni3N catalyst demonstrates an overpotential of 135 mV when subjected to a current density of 10 mA cm−2. The refined structural characterization suggests that the introduction of oxygen results in a reduction in electron densities surrounding the Ni sites. Furthermore, DFT calculations provide additional evidence that the electrocatalyst of Ni3N generates a greater number of lowest unoccupied orbitals (LUMOs) and improved alignment, thereby enhancing the adsorption and splitting of water. The notion of orbital-regulated electronic levels on Ni sites introduces a distinctive methodology for the systematic development of catalysts used in hydrogen evolution and other applications.

Graphical abstract: Enhancing the electronic structure of Ni-based electrocatalysts through N element substitution for the hydrogen evolution reaction

Supplementary files

Article information

Article type
Paper
Submitted
13 мар 2024
Accepted
22 май 2024
First published
23 май 2024

Nanoscale, 2024,16, 11604-11609

Enhancing the electronic structure of Ni-based electrocatalysts through N element substitution for the hydrogen evolution reaction

Y. Yang, X. Jin, F. Zhan and Y. Yang, Nanoscale, 2024, 16, 11604 DOI: 10.1039/D4NR01071J

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