☆ 4.8 Article

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

ADVANCED FUNCTIONAL MATERIALS (2022)

期刊

ADVANCED FUNCTIONAL MATERIALS

卷 32, 期 18, 页码 -

出版社

WILEY-V C H VERLAG GMBH

DOI: 10.1002/adfm.202112832

关键词

doping; Ni; S-3; (2); oxygen evolution; spin state

类别

Chemistry, Multidisciplinary Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter

资金

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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摘要

This study reports a method to optimize the adsorption of active intermediates by modulating the local spin state and band structure of Ni3S2 nanosheets, resulting in a considerable improvement in the oxygen evolution reaction.

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 e(g) 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.

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