A visible-light-driven CoS2/CuS@CNT-C3N4 photocatalyst for high-performance rechargeable zinc-air batteries beyond 500 mW cm‒2

doi:10.1016/S1872-2067(24)60173-7

Abstract

Abstract:

Storing solar energy in battery systems is crucial to achieving a green and sustainable society. However, the efficient development of photo-enhanced zinc-air batteries (ZABs) is limited by the rapid recombination of photogenerated carriers on the photocathode. In this work, the visible-light-driven CoS₂/CuS@CNT-C₃N₄ photocatalyst with unique petal-like layer structure was designed and developed, which can be used as air electrode for visible-light-driven ZABs. The superior performance of ZABs assembled by CoS₂/CuS@CNT-C₃N₄ was mainly attributed to the successful construction of Schottky heterojunction between g-C₃N₄ and carbon nanotubes (CNTs), which accelerates the transfer of electrons from g-C₃N₄ to CoS₂/CuS cocatalysts, improves the carrier separation ability, and extends the carrier lifetime. Thereinto, the visible-driven ZABs assembled by CoS₂/CuS@CNT-C₃N₄ photocatalyst has a power density of 588.90 mW cm^-2 and a charge-discharge cycle of 643 h under visible light irradiation, which is the highest performance ever reported for photo-enhanced ZABs. More importantly, the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation, which is significantly lower than the voltage drop (0.94 V) in the dark. This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.

Key words: Visible-light-driven, CoS₂/CuS@CNT-C₃N₄ photocatalyst, Zinc-air battery, Heterojunction, Photogenerated carriers

Yang Zhang, Nengneng Xu, Bingbing Gong, Xiaoxiao Ye, Yi Yang, Zhaodi Wang, Biyan Zhuang, Min Wang, Woochul Yang, Guicheng Liu, Joong Kee Lee, Jinli Qiao. A visible-light-driven CoS₂/CuS@CNT-C₃N₄ photocatalyst for high-performance rechargeable zinc-air batteries beyond 500 mW cm^‒2[J]. Chinese Journal of Catalysis, 2025, 68: 300-310.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60173-7

https://www.cjcatal.com/EN/Y2025/V68/I1/300

Figures/Tables 5

Fig. 1. (a) Schematic illustration of the preparation of CoS2/CuS@CNT-C3N4. (b,c) SEM images of CoS2/CuS@CNT-C3N4. TEM (d,e) and HRTEM (f) images of CoS2/CuS@CNT-C3N4. (g) HAADF-STEM image and STEM elemental mapping results of CoS2/CuS@CNT-C3N4.

Fig. 2. (a) XRD pattern of CoS2/CuS@CNT-C3N4. N2 sorption isotherms (b) and Raman spectra (c) of CoS2/CuS@CNT-C3N4, CoS2/Co(SO4)2@CNT-C3N4 and (Cu, Co)3OS3@CNT. High-resolution XPS surveys of C 1s region (d), N 1s region (e), O 1s region (f), S 2p region (g), Cu 2p region (h), and Co 2p region (i) for CoS2/CuS@CNT-C3N4.

Fig. 3. (a) ORR polarization curves of CoS2/CuS@CNT-C3N4 and Pt/C in O2-saturated 0.1 mol L?1 KOH. (b) Half-wave potential and kinetic current density at 0.85 V (vs. RHE) of CoS2/CuS@CNT-C3N4 and Pt/C. (c) Curves of the average electron transfer number and percentage of peroxide of CoS2/CuS@CNT-C3N4 under visible light irradiation. (d) OER polarization curves of CoS2/CuS@CNT-C3N4 and IrO2 in O2-saturated 0.1 mol L?1 KOH. (e) Bar plots of overpotentials obtained at 10 mA cm?2. (f) Tafel plots reordered from (d).

Fig. 4. (a) A schematic configuration of a photo-enhanced ZABs assembled by CoS2/CuS@CNT-C3N4. Open-circuit potential (b), rate discharge curves (c), discharge specific capacity (d), polarization and corresponding power density curves (e) and galvanostatic charge-discharge cycling profiles (f) of CoS2/CuS@CNT-C3N4 and Pt/C + IrO2 air cathode-based ZABs under visible light irradiation and in the dark. (g) Comparison of the performance of photoelectrochemical ZABs reported recently and in this work.

Fig. 5. (a) UV-vis diffuse reflectance spectrum of g-C3N4, CoS2/CuS-C3N4 and CoS2/CuS@CNT-C3N4. (b) Mott-Schottky plots of g-C3N4 in 0.5 mol L?1 Na2SO4 aqueous solution with a frequency of 1200, 1500 and 2000 Hz. Transient photocurrent responses (c), steady-state PL spectra (d), TRPL spectra (e) of g-C3N4, CoS2/CuS-C3N4 and CoS2/CuS@CNT-C3N4. (f) Working mechanism of CoS2/CuS@CNT-C3N4 with the Schottky heterojunction for photo-enhanced ORR and OER in aqueous electrolytes.

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A visible-light-driven CoS₂/CuS@CNT-C₃N₄ photocatalyst for high-performance rechargeable zinc-air batteries beyond 500 mW cm^‒2

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