Metal-organic framework-derived cation regulation of metal sulfides for enhanced oxygen evolution activity

doi:10.1016/S1872-2067(23)64533-4

Chinese Journal of Catalysis ›› 2023, Vol. 54: 290-297.DOI: 10.1016/S1872-2067(23)64533-4

Metal-organic framework-derived cation regulation of metal sulfides for enhanced oxygen evolution activity

Kai Wan^a^,^b, Jiangshui Luo^c^,^*(), Wenbo Liu^a, Ting Zhang^d, Jordi Arbiol^d^,^e^,^*(), Xuan Zhang^b, Palaniappan Subramanian^b, Zhiyong Fu^a^,^*(), Jan Fransaer^b^,^*()

^aGuangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China
^bDepartment of Materials Engineering, KU Leuven, Leuven 3001, Belgium
^cEngineering Research Center of Alternative Energy Materials & Devices, Ministry of Education, College of Materials Science and Engineering, Sichuan University, Chengdu 610065, Sichuan, China
^dCatalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona 08193, Catalonia, Spain
^eICREA, Pg. Lluís Companys 23, Barcelona08010, Catalonia, Spain

Received:2023-08-15 Accepted:2023-10-11 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: jiangshui.luo@scu.edu.cn (J. Luo), arbiol@icrea.cat (J. Arbiol),zyfu@scut.edu.cn (Z. Y. Fu), jan.fransaer@kuleuven.be (J. Fransaer).
Supported by:
National Natural Science Foundation of China(21975081);National Natural Science Foundation of China(22178126);National Natural Science Foundation of China(22208110);National Natural Science Foundation of China(21776120);National Natural Science Foundation of China(22378270);Science and Technology Program of Guangzhou(2023A04J1357);China Postdoctoral Science Foundation(2022M711196);Open Project of Engineering Research Center of Alternative Energy Materials & Devices, Ministry of Education, Sichuan University(AEMD202204);Sichuan Science and Technology Program(2022ZYD0016);Sichuan Science and Technology Program(2023JDRC0013);Hohhot Science and Technology Program(2023-JieBangGuaShuai-Gao-3);Natural Science Foundation of Fujian Province, China(2023J01254);Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202206);Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202218)

Abstract

Abstract:

Heteroatom doping serves as an important strategy to improve the oxygen evolution reaction (OER) activity of transition-metal compounds, while the investigation of intrinsic active sites and mechanisms remains insufficient. In this work, a facile cation regulation strategy is reported to boost the OER activity of metal sulfides via pyrolysis of the Ni-Co bimetallic metal-organic framework. The obtained Ni-substituted CoS nanoparticles on nitrogen-doped mesoporous carbon (Ni-CoS/NC) catalyst achieves a current density of 10 mA cm^-2 at a small overpotential of 270 mV with a Tafel slope of 37 mV dec^-1 in 1.0 mol L^-1 KOH. Through a combination of spectroscopy study and theoretical computations, the activity origin is revealed at the atomic level. The Co_xNi₁_-xOOH serves as the real active site for the OER generated by the Ni-CoS/NC reconstruction under oxidation potential during OER. The Ni substitution results in a strong electronic interaction between the two metals, thus generating more negatively charged Co atoms and more positively charged Ni atoms in the electrocatalyst. The metal sites with regulated electronic structure exhibit enhanced surface adsorption of OOH* and reduce the OER overpotential. Meanwhile, the conductive porous carbon scaffold facilitates electron transfer, mass diffusion, and the accessibility of active sites. This work not only provides a feasible cation regulation strategy for the design of high-performance electrocatalysts for low-cost energy storage and conversion systems, but also yields fresh insight into the activity enhancement mechanisms and intrinsic active sites.

Key words: Metal-organic framework, Cation regulation, Metal sulfide, Metal oxyhydroxide, Oxygen evolution reaction

Kai Wan, Jiangshui Luo, Wenbo Liu, Ting Zhang, Jordi Arbiol, Xuan Zhang, Palaniappan Subramanian, Zhiyong Fu, Jan Fransaer. Metal-organic framework-derived cation regulation of metal sulfides for enhanced oxygen evolution activity[J]. Chinese Journal of Catalysis, 2023, 54: 290-297.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64533-4

https://www.cjcatal.com/EN/Y2023/V54/I11/290

Figures/Tables 5

Fig. 1. (a-c) TEM images of Ni-CoS/NC. (d) HAADF STEM image and EELS maps of Ni-CoS/NC. (e) XRD patterns of CoS/NC, Ni-CoS/NC, and NiS/NC (Insert are the enlarged diffraction peaks of the (100) plane).

Fig. 2. Co 2p3/2 and Ni 2p3/2 peaks (a), S 2p peaks (b), Co 2p peaks (c) and fitting results, Ni 2p peaks (d) and fitting results. (e) Ratio of the metal valence states (M3+ and M2+) of CoS/NC and Ni-CoS/NC extracted from XPS results. (f) S 2p peaks and fitting results.

Fig. 3. Cyclic voltammograms (a), overpotentials (b) at 10 mA cm-1, Tafel plots (c) of different catalysts. (d) Nyquist plots and fitting results at an applied potential of 1.53 V vs. RHE (Inset is the equivalent circuit, Rs: resistance of electrolyte, Rct: charge transfer resistance, CPE: constant phase element). (e) Cdl values. (f) Stability test of Ni-CoS/NC at 50 mA cm-2.

Fig. 4. XRD patterns (a), S 2p peaks (b), and Co 2p3/2 peaks (c) of Ni-CoS/NC before and after OER. (d) HAADF STEM image and corresponding EELS compositional maps obtained on the Ni-CoS/NC sample after OER. HRTEM image (e) of Ni-CoS/NC after OER and its corresponding indexed FFT patterns (f,g).

Fig. 5. (a) The free energy diagrams of CoOOH and CoxNi1-xOOH for the adsorption of different intermediates on Co site. (b) The free energy diagrams and structure models of NiOOH and CoxNi1-xOOH for the adsorption of different intermediates on Ni site.

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Metal-organic framework-derived cation regulation of metal sulfides for enhanced oxygen evolution activity

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