A visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst for high-performance rechargeable zinc-air batteries beyond 500 mW cm^(-2)  

可见光驱动的CoS_(2)/CuS@CNT-C_(3)N_(4)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

作　　者：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 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(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;上海市污染控制与生态安全研究所,上海20009;中国新疆大学化工学院,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;盐城工学院化学化工学院,江苏盐城224051;东国大学物理系,首尔,韩国;华北电力大学能源动力与机械工程学院,北京102206;嘉泉大学化工与生化工程系,城南市,韩国)

机构地区：[1]State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,College of Environmental Science and Engineering,Donghua University,Shanghai 201620,China [2]Shanghai Institute of Pollution Control and Ecological Security,Shanghai 200092,China [3]School of Chemical Engineering and Technology,Xinjiang University,Urumqi 830017,Xinjiang,China [4]School of Chemistry and Chemical Engineering,Yancheng Institute of Technology,Yancheng 224051,Jiangsu,China [5]Department of Physics,Dongguk University,Seoul 04620,Korea [6]School of Energy Power and Mechanical Engineering,North China Electric Power University,Beijing 102206,China [7]Department of Chemical&Biochemical Eng,Gachon University,Seongnam-si 13120,Korea

出　　处：《Chinese Journal of Catalysis》2025年第1期300-310,共11页催化学报(英文)

基　　金：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).

摘　　要：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 CoS_(2)/CuS@CNT-C_(3)N_(4)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 CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)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.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200mW cm^(-2),这限制了其在高功率需求场景下的实际应用.因此,函需开发高效、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CoS_(2)/CuS@CNT-C_(3)N_(4)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CoS_(2)/CuS@CNT-C_(3)N_(4)光电催化剂表现出较好的ORR活性(0.84V)和低OER过电位(0.47V).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CoS_(2)/CuS@CNT-C_(3)N_(4)光催化剂组装的可见光驱动ZABs表现出更高的功率密度(588.90mW cm^(-2))和连续643h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0.54V,明显低于黑暗条件下的0.94V.扫描电镜、透射电镜和N吸附-脱附结果表明,Cu的掺杂可有效降低CoS_(2)/CuS@CNT-C_(3)N_(4)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-C_(3)N_(4)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-C_(3)N_(4)和助催化剂CoS_(2)/CuS@C_(3)N_(4)之间,构建高效双功能CoS_(2)/CuS@CNT-C_(3)N_(4)光催化剂.X射线光电子能谱结果表明,Cu的掺杂提高了CoS_(2)/CuS@CNT-C_(3)N_(4)的Co^(3+)峰强度,降低了Co^(2+)峰强度.值得一提的是,Co^(3+)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CoS_(2)/CuSCNT-C_(3)N_(4)光催化剂的成功�

关 键 词：Visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst Zinc-air battery Heterojunction Photogenerated carriers 

分 类 号：TM9[电气工程—电力电子与电力传动]