Regulating the Local Spin State and Band Structure in Ni3S2 Nanosheet for Improved Oxygen Evolution Activity

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Abstract
The separate modulation of the adsorption of *O and *OOH is challenging in oxygen evolution reaction (OER), which results in a large overpotential and slow kinetics. To balance the adsorption of the two active species, here, a way to regulate the local spin state and band structure simultaneously in Ni3S2 nanosheets is reported. The adequate doping of W heteroatoms causes the electron depletion from the Ni active site, which modulates the spin state of eg electrons, weakening the adsorption of *O. Additionally, the introduction of S vacancies contributes to the upshift of the d band center, which strengthens the adsorption of *OOH. In this manner, the adsorption of Ni3S2 for the active intermediates is optimized, resulting in a considerably improved overpotential of 246 mV at 100 mA cm−2 and a Tafel slope of 66 mV dec−1. This work provides insights into the exploration of OER catalysts through synergistic modulation of the spin state and the band structure.
Funding Information
  • National Natural Science Foundation of China (52102365, 51902220, 52072255)
  • Science Fund for Distinguished Young Scholars of Zhejiang Province (LR22E020003)
  • Natural Science Foundation of Zhejiang Province (LY21E020001, LTY20E020001)

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