Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

doi:10.1007/s11705-021-2085-3

Front. Chem. Sci. Eng.

2021, Vol. 15

Issue (6) : 1487-1499 https://doi.org/10.1007/s11705-021-2085-3

RESEARCH ARTICLE

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

Laicong Deng¹, Zhuxian Yang¹, Rong Li², Binling Chen¹, Quanli Jia³, Yanqiu Zhu¹, Yongde Xia¹(

)

¹. College of Engineering, Mathematics and Physical Sciences, University of Exeter, Exeter EX4 4QF, UK
². Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637000, China
³. Henan Key Laboratory of High Temperature Functional Ceramics, Zhengzhou University, Zhengzhou 450052, China

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Abstract

Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

Keywords MOF derivative graphene electrocatalyst oxygen reduction reaction oxygen evolution reaction hydrogen evolution reaction

Corresponding Author(s): Yongde Xia

Online First Date: 09 October 2021 Issue Date: 09 November 2021

Cite this article:

Laicong Deng,Zhuxian Yang,Rong Li, et al. Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts[J]. Front. Chem. Sci. Eng., 2021, 15(6): 1487-1499.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2085-3
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I6/1487

Fig.1 (a) Powder XRD, (b) Raman spectra and (c) N₂ sorption isotherms of CoS@C/10Graphene and CoS@C.

Fig.2 TEM images of (a, b) CoS@C and (c, d) CoS@C/10Graphene; inset in (a, c) is SAED patterns for corresponding sample; (e) elemental mappings for CoS@C/10Graphene.

Fig.3 (a) Element survey by XPS and high resolution XPS spectra of (b) C 1s, (c) Co 2p, (d) S 2p and (e) N 1s of CoS@C and CoS@C/10Graphene.

Fig.4 (a) CV curves of CoS@C and CoS@C/10Graphene in N₂- or O₂-saturated 0.1 mol·L^–1 KOH; (b, d) ORR polarization curves of CoS@C/10Graphene and CoS@C at different rotating speeds, respectively; (c, e) K-L plots of samples CoS@C/10Graphene and CoS@C at different potentials, respectively; (f) n and the corresponding J_k of CoS@C/10Graphene and CoS@C as a function of the electrode potentials.

Fig.5 (a) ORR polarization curves and (b) current-time chronoamperometric responses of CoS@C/10Graphene, CoS@C and Pt/C at 1600 r·min^–1 in O₂-saturated 0.1 mol·L^–1 KOH solution; (c) chronoamperometric responses of CoS@C/10Graphene, CoS@C and Pt/C at –0.15 V in O₂-saturated 0.1 mol·L^–1 KOH solution (1600 r·min^–1) with 1 mol·L^–1 methanol; (d) ORR polarization curves of CoS@C/Graphene composites with various graphene content.

Fig.6 (a) LSV polarization curves of CoS@C/10Graphene, CoS@C and Pt/C; (b) current-time chronoamperometric responses of CoS@C/10Graphene measured in 0.1 mol·L^–1 KOH solution.

Fig.7 (a) Polarization curves and (b) corresponding Tafel plots of CoS@C, CoS@C/10Graphene and Pt/C for HER measured in 0.5 mol·L^–1 H₂SO₄ solution.

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