Design strategy for low-temperature sulfur etching to achieve high-performance hollow multifunctional electrode material

doi:10.1016/j.jmst.2021.12.045

Abstract

Abstract:

Zeolite Imidazole Framework (ZIF) has the advantages of large specific surface area, high porosity, and easy functionalization, so it looked like one of the most promising energy storage and conversion materials. In the meantime, transition metal oxides and sulfides have been widely used in environmental and energy conversion applications. Hence, a NaOH-assisted thioacetamide etching strategy is, therefore, designed with the metal-organic framework as precursor to realize the hollow nanostructure of ZIF bimetallic sulfide (Sx-CoCd-350) with abundant sulfur vacancies for enhanced catalysts oxygen evolution reaction (OER)/hydrogen evolution reaction (HER)) performance and capacitance performance of capacitor. The overpotential of S2-CoCd-350 in the OER process is 355 mV at 50 mA cm-2, which is substantially lower than other reported ZIF-based catalysts. S2-CoCd-350 has an overpotential of 84 mV at 10 mA cm-2 when employed as HER catalyst. Furthermore, the S2-CoCd-350 electrode did not alter appreciably during a long-term durability test of more than 10 h. More impressively, S2-CoCd-350 matches the activated carbon (AC) electrode with excellent capacitance performance 1220 μWh cm-2 energy density (at 3370 μW cm-2) and 25,000 μW cm-2 (at 700 μWh cm-2) maximum power density. In addition, the assembled supercapacitor has excellent cycling stability.

Key words: Electrocatalyst, OER/HER, Supercapacitor, Sulfur vacancies, Hollow nanostructure

Hui Wen, Ziyu Yi, Zhenyu Hu, Rui Guo, Xuanwen Liu. Design strategy for low-temperature sulfur etching to achieve high-performance hollow multifunctional electrode material[J]. J. Mater. Sci. Technol., 2022, 119: 209-218.

Figures/Tables 7

Fig. 1. Schematic diagram of the route of hollow S2-CoCd-350 with sulfur-rich vacancies.

Fig. 2. (a) XRD patterns of S2-CoCd-350. (b, c) TEM of S2-CoCd-350 dodecahedron (The illustration shows corresponding SAED). (d) EDS element mapping of Co, Cd, S, O, C, and N of S2-CoCd-350 dodecahedron. (e-g) TEM, HRTEM and corresponding SAED patterns of S2-CoCd-350 hollow nanowires. (h) EDS element mapping of Co, Cd, S, O, C, and N of S2-CoCd-350 hollow nanowires.

Fig. 3. (a) OER curve fitting graph of catalyst S2-CoCd-350. (b, c) OER curves and Tafel plots curves for CoCd, CoCd-ZIF, CoCd-350, and S2-CoCd-350. (d) Linear plots of cathodic charging currents versus the scan rate derived from cyclic voltammetry diagrams under different scan rates. (e, f) HER curves and Tafel plots curves for CoCd, CoCd-ZIF, CoCd-350, and S2-CoCd-350.

Fig. 4. (a) EPR spectra of S2-CoCd-350 samples. (b) Survey XPS spectrum. High-resolution XPS spectra of (c) S 2p (d) Cd 3d (e) Co 2p of S2-CoCd-350. (f) S2-CoCd-350 i-t curve in 3 h.

Fig. 5. Electrochemical characterizations: (a) CV curves. (b) GCD curves. (c) Specific capacitances. (d) CV curves at 10-50 mV/s. (e) GCD curves at a range of 5-30 mA cm-2. (f) Nyquist plots. (g) b value of S2-CoCd-350. (h) Capacitance contribution. (i) Cycle performance at a current density of 30 mA/cm2.

Fig. 6. (a) Schematic illustration showing the fabrication of supercapttery device and (b) CV curves of S2-CoCd-350 and biomass-derived AC electrodes measured individually at a scan rate of 50 mV/s, indicating possible cell potential of 1.7 V. (c) CV curves of the supercapattery system measured at various scan rates of 10-100 mV/s. (d) CV curves of S2-CoCd-350//AC device measured at various potential windows of 0-1.6 to 0-2 V. (e) GCD curves of the supercapattery system measured at various current densities of 5-30 mA/cm2. (f) Ragone plot and (g) cycling stability of the supercapttery.

Fig. 7. (a) The working status of the motor fan at the beginning and end. (b) Supercapacitors supply power for LEDs for different periods of time.

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