Sulfur-deficient CoNi<sub>2</sub>S<sub>4</sub> nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

doi:10.1007/s11705-023-2308-x

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (11) : 1707-1717 https://doi.org/10.1007/s11705-023-2308-x

RESEARCH ARTICLE

Sulfur-deficient CoNi₂S₄ nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

Gaohui Du^1,²(

), Yi Fan², Lina Jia², Yunting Wang², Yawen Hao², Wenqi Zhao², Qingmei Su², Bingshe Xu^1,²(

)

¹. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030000, China
². Materials Institute of Atomic and Molecular Science, Shaanxi University of Science and Technology, Xi’an 710021, China

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Abstract

Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi₂S₄ nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi₂S₄. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi₂S₄ from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi₂S₄ nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm^–2 for oxygen evolution reaction and 380 mV@100 mA·cm^–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm^–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

Keywords nanoparticle sulfur vacancy porous carbon nanofiber transition metal sulfides electrolysis

Corresponding Author(s): Gaohui Du,Bingshe Xu

About author:

Peng Lei and Charity Ngina Mwangi contributed equally to this work.

Just Accepted Date: 11 April 2023 Online First Date: 26 May 2023 Issue Date: 25 October 2023

Cite this article:

Gaohui Du,Yi Fan,Lina Jia, et al. Sulfur-deficient CoNi₂S₄ nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting[J]. Front. Chem. Sci. Eng., 2023, 17(11): 1707-1717.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2308-x
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I11/1707

Fig.1 Schematics of the fabrication of CoNi₂S₄@PCNFs.

Fig.2 (a) XRD pattern of CoNi₂S₄@PCNFs, Ni₃S₂@PCNFs and CoNi₂S₄; (b) SEM, (c, d) TEM and (e) HRTEM images of CoNi₂S₄@PCNFs. The inset in (b) is the diameter distribution of PCNFs, and the inset in (c) is the diameter distribution of nanoparticles. (f) Raman spectra of PCNFs, Ni₃S₂@PCNFs and CoNi₂S₄@PCNFs.

Fig.3 (a) Survey XPS spectra, high resolution XPS spectra of (b) Co 2p, (c) Ni 2p and (d) S 2p of CoNi₂S₄@PCNFs.

Fig.4 (a) TG curve of CoNi₂S₄@PCNFs; (b) EPR spectra of pure CoNi₂S₄ and CoNi₂S₄@PCNFs.

Fig.5 Atomic structures of (a) CoNi₂S₄ and (b) CoNi₂S₄ with S vacancies; site projected DOS of (c) CoNi₂S₄ and (d) CoNi₂S₄ containing S vacancies.

Tab.1 The values of R_s and R_ct of the samples

Fig.6 (a) OER LSV and (b) HER LSV curves of CoNi₂S₄@PCNFs-1, CoNi₂S₄@PCNFs, CoNi₂S₄@PCNFs-2.

Fig.7 (a) LSV curves of PCNFs, Ni₃S₂@PCNFs, CoNi₂S₄ and CoNi₂S₄@PCNFs; (b) overpotentials required for 20 and 100 mA·cm^–2; (c) Tafel plots, (d) EIS curves and (e) C_dl of PCNFs, Ni₃S₂@PCNFs, CoNi₂S₄ and CoNi₂S₄@PCNFs; (f) normalized LSV curves obtained from panel (e); (g) TOF tests; (h) chronoamperometric measurement of CoNi₂S₄@PCNFs toward OER in 1.0 mol·L^–1 KOH.

Tab.2 Comparison of the HER/OER overpotentials of NiCo₂S₄-based electrocatalysts

Fig.8 (a) HER polarization curves of PCNFs, Ni₃S₂@PCNFs, CoNi₂S₄, and CoNi₂S₄@PCNFs; (b) overpotentials required for 20 and 100 mA·cm^–2; (c) Tafel plots, (d) EIS curves, and (e) C_dl of the samples; (f) normalized LSV curves obtained from panel (e); (g) TOF tests. (h) chronoamperometric measurement of CoNi₂S₄@PCNFs toward HER in 1.0 mol·L^–1 KOH.

Fig.9 (a) Polarization curves of the CoNi₂S₄@PCNF cell for overall water splitting in alkaline electrolyte; (b) chronoamperometric curve of CoNi₂S₄@PCNFs cell and the two-electrode configuration for water splitting (inset).

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