可见光驱动的CoS2/CuS@CNT-C3N4光催化剂用于500 mW cm-2 以上的高性能可充放电锌-空气电池

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

催化学报 ›› 2025, Vol. 68: 300-310.DOI: 10.1016/S1872-2067(24)60173-7

可见光驱动的CoS₂/CuS@CNT-C₃N₄光催化剂用于500 mW cm^-2 以上的高性能可充放电锌-空气电池

张杨^a, 徐能能^a^,^*(), 巩兵兵^c, 叶笑笑^a, 阳宜^a, 王昭娣^a, 庄碧艳^a, 王敏^d, Woochul Yang^e, 刘桂成^f, Joong Kee Lee^g, 乔锦丽^a^,^b^,^*()

^a东华大学环境科学与工程学院, 化学纤维与高分子材料改性国家重点实验室, 上海 201620, 中国
^b上海市污染控制与生态安全研究所, 上海 200092, 中国
^c新疆大学化工学院, 石油天然气精细化工教育部暨自治区重点实验室, 新疆乌鲁木齐 830017, 中国
^d盐城工学院化学化工学院, 江苏盐城 224051, 中国
^e东国大学物理系, 首尔, 韩国
^f华北电力大学能源动力与机械工程学院, 北京 102206, 中国
^g嘉泉大学化工与生化工程系, 城南市, 韩国

收稿日期:2024-08-10 接受日期:2024-10-09 出版日期:2025-01-18 发布日期:2025-01-02
通讯作者: * 电子信箱: nengnengxu@dhu.edu.cn (徐能能), qiaojl@dhu.edu.cn (乔锦丽).
基金资助:
国家重点研发计划(2022YFE0138900);国家自然科学基金(21972017);上海市科委“科技创新行动计划”基础研究领域(19JC1410500)

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

Yang Zhang^a, Nengneng Xu^a^,^*(), Bingbing Gong^c, Xiaoxiao Ye^a, Yi Yang^a, Zhaodi Wang^a, Biyan Zhuang^a, Min Wang^d, Woochul Yang^e, Guicheng Liu^f, Joong Kee Lee^g, Jinli Qiao^a^,^b^,^*()

^aState Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
^bShanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
^cSchool of Chemical Engineering and Technology, Xinjiang University, Urumqi 830017, Xinjiang, China
^dSchool of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China
^eDepartment of Physics, Dongguk University, Seoul 04620, Korea
^fSchool of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China
^gDepartment of Chemical & Biochemical Eng, Gachon University, Seongnam-si 13120, Korea

Received:2024-08-10 Accepted:2024-10-09 Online:2025-01-18 Published:2025-01-02
Contact: * E-mail: nengnengxu@dhu.edu.cn (N. Xu), qiaojl@dhu.edu.cn (J. Qiao).
Supported by:
National Key Research and Development Program of China(2022YFE0138900);National Natural Science Foundation of China(21972017);“Scientific and Technical Innovation Action Plan” Basic Research Field of Shanghai Science and Technology Committee(19JC1410500)

摘要/Abstract

摘要：

水系锌-空电池(ZABs)具有理论能量密度大、应用场景广泛的特点, 是新兴的动力电池之一. 它们能够在电池系统中存储太阳能, 为实现可持续发展做出贡献. 然而, 由于空气电极上的氧还原反应(ORR)和析氧反应(OER)的动力学过程缓慢, 大多数已报道的金属硫化物双功能电极的峰值功率密度通常低于200 mW cm^-2, 这限制了其在高功率需求场景下的实际应用. 因此, 亟需开发高效、稳定的可见光驱动催化剂.
基于光电耦合机理, 本文设计并开发了具有独特花瓣层状结构的可见光驱动的CoS₂/CuS@CNT-C₃N₄光催化剂, 用于制备高效可见光驱动ZABs的空气电极. 优化后的CoS₂/CuS@CNT-C₃N₄光电催化剂表现出较好的ORR活性(0.84 V)和低OER过电位(0.47 V). 具体来说, 与目前已报道的光电化学ZABs和最先进的双功能催化剂组装的ZABs相比, 由CoS₂/CuS@CNT-C₃N₄光催化剂组装的可见光驱动ZABs表现出更高的功率密度(588.90 mW cm^-2)和连续643 h的高度稳定的充放电循环. 更重要的是, ZABs在可见光照射下的充放电压降仅为0.54 V, 明显低于黑暗条件下的0.94 V. 扫描电镜、透射电镜和N₂吸附-脱附结果表明, Cu的掺杂可有效降低CoS₂/CuS@CNT-C₃N₄光催化剂中Co基硫化物的聚集, 使其呈现花瓣层状结构, 提高光催化剂的比表面积. 此外, g-C₃N₄不仅可以作为光收集器, 同时也作为金属硫化物的分散剂, 减少其团聚. 而碳纳米管(CNTs)作为“电子隧道”, 交错于光催化剂g-C₃N₄和助催化剂CoS₂/CuS@CNT之间, 构建高效双功能CoS₂/CuS@CNT-C₃N₄光催化剂. X射线光电子能谱结果表明, Cu的掺杂提高了CoS₂/CuS@CNT-C₃N₄的Co³⁺峰强度, 降低了Co²⁺峰强度. 值得一提的是, Co³⁺处于高活性自旋态, 具有吸引和贡献电子的能力, 有利于提高ORR性能. Cu和Co之间表现出强的电子相互作用, 进一步表明CoS₂/CuS@CNT-C₃N₄光催化剂的成功合成. 同时, 进一步通过一系列光电化学测试探究了具有肖特基异质结结构的CoS₂/CuS@CNT-C₃N₄光催化剂在光电化学ZABs中的工作机制. 在可见光照射下, N型g-C₃N₄的VB被光子碰撞产生光生电子-空穴对. 在放电过程中, g-C₃N₄产生的光生电子通过电子隧道(CNTs)转移到助催化剂(CoS₂/CuS)上, 参与ORR过程, 增强电催化ORR活性. 同时, 在充电过程中, N型g-C₃N₄在VB处积累的光生空穴氧化OH^-, 参与OER过程, 增强电催化OER活性. 因此, 与黑暗条件相比, 在可见光照射条件下, 由于异质结效应促进了光生载流子的分离, 由CoS₂/CuS@CNT-C₃N₄组装的光增强ZABs的ORR和OER性能有望同时提高.

综上所述, 本文设计了高效、稳定的可见光驱动的双功能催化剂, 为未来可再生能源的实际应用提供了新思路.

关键词: 可见光驱动, CoS₂/CuS@CNT-C₃N₄光催化剂, 锌-空气电池, 异质结, 光生载流子

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

张杨, 徐能能, 巩兵兵, 叶笑笑, 阳宜, 王昭娣, 庄碧艳, 王敏, Woochul Yang, 刘桂成, Joong Kee Lee, 乔锦丽. 可见光驱动的CoS₂/CuS@CNT-C₃N₄光催化剂用于500 mW cm^-2 以上的高性能可充放电锌-空气电池[J]. 催化学报, 2025, 68: 300-310.

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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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(24)60173-7

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

图/表 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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可见光驱动的CoS₂/CuS@CNT-C₃N₄光催化剂用于500 mW cm^-2 以上的高性能可充放电锌-空气电池

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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