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Design Principles and Mechanistic Understandings of Non-Noble-Metal Bifunctional Electrocatalysts for zinc-air batteries

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Nano-Micro Letters 2024年第9期16卷 13-48页

作者： Yunnan Gao Ling Liu Yi Jiang Dexin Yu Xiaomei Zheng Jiayi Wang Jingwei Liu Dan Luo Yongguang Zhang Zhenjia Shi Xin Wang Ya‑Ping Deng Zhongwei Chen Power Battery and Systems Research Center State Key Laboratory of CatalysisDalian Institute of Chemical PhysicsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023People’s Republic of China Department of Chemical Engineering University of WaterlooWaterlooON N2L 3G1Canada Institute of Carbon Neutrality Zhejiang Wanli UniversityNingbo 315100People’s Republic of China College of Materials and Chemistry China Jiliang UniversityHangzhou 310018People’s Republic of China

zinc-air batteries(ZABs)are promising energy storage systems because of high theoretical energy density,safety,low cost,and abundance of zinc.However,the slow multi-step reaction of oxygen and heavy reliance on noble-metal catalysts hinder the practical applications of ZABs.Therefore,feasible and advanced non-noble-metal elec-trocatalysts for air cathodes need to be identified to promote the oxygen catalytic reaction.In this review,we initially introduced the advancement of ZABs in the past two decades and provided an overview of key developments in this field.Then,we discussed the work-ing mechanism and the design of bifunctional electrocatalysts from the perspective of morphology design,crystal structure tuning,interface strategy,and atomic engineering.We also included theoretical studies,machine learning,and advanced characterization technologies to provide a comprehensive understanding of the structure-performance relationship of electrocatalysts and the reaction pathways of the oxygen redox reactions.Finally,we discussed the challenges and prospects related to designing advanced non-noble-metal bifunctional electrocatalysts for ZABs.

关键词： zinc-air batteries Bifunctional electrocatalysts Design principles Mechanistic understandings

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A Review of Rechargeable zinc-air batteries:Recent Progress and Future Perspectives

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Nano-Micro Letters 2024年第7期16卷 358-401页

作者： Ghazanfar Nazir Adeela Rehman Jong-Hoon Lee Choong-Hee Kim Jagadis Gautam Kwang Heo Sajjad Hussain Muhammad Ikram Abeer AAlObaid Seul-Yi Lee Soo-Jin Park Department of Nanotechnology and Advanced Materials Engineering Hybrid Materials Research Center(HMC)Sejong UniversitySeoul 05006Republic of Korea Department of Chemical and Biomolecular Engineering Yonsei University50 Yonsei-RoSeodaemun-GuSeoul 03722Republic of Korea Department of Chemistry Inha UniversityIncheon 22212Republic of Korea Solar Cell Applications Research Lab Department of PhysicsGovernment College University LahoreLahore 54000 PunjabPakistan Department of Chemistry College of ScienceKing Saud UniversityP.O.Box 2455Riyadh 11451Saudi Arabia

zinc-air batteries(ZABs)are gaining attention as an ideal option for various applications requiring high-capacity batteries,such as portable electronics,electric vehicles,and renewable energy storage.ZABs offer advantages such as low environmental impact,enhanced safety compared to Li-ion batteries,and cost-effectiveness due to the abundance of zinc.However,early research faced challenges due to parasitic reactions at the zinc anode and slow oxygen redox kinetics.Recent advancements in restructuring the anode,utilizing alternative electrolytes,and developing bifunctional oxygen catalysts have significantly improved ZABs.Scientists have achieved battery reversibility over thousands of cycles,introduced new electrolytes,and achieved energy efficiency records surpassing 70%.Despite these achievements,there are challenges related to lower power density,shorter lifespan,and air electrode corrosion leading to performance degradation.This review paper discusses different battery configurations,and reaction mechanisms for electrically and mechanically rechargeable ZABs,and proposes remedies to enhance overall battery performance.The paper also explores recent advancements,applications,and the future prospects of electrically/mechanically rechargeable ZABs.

关键词： zinc-air batteries Energy storage Affordability Reversibility

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Electronic structure and spin state regulation of vanadium nitride via a sulfur doping strategy toward flexible zinc-air batteries

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Journal of Energy Chemistry 2024年第2期89卷 239-249,I0007页

作者： Daijie Deng Honghui Zhang Jianchun Wu Xing Tang Min Ling Sihua Dong Li Xu Henan Li Huaming Li Institute for Energy Research Institute of Quantum and Sustainable TechnologySchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringJiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural EquipmentJiangsu UniversityZhenjiang 212013JiangsuChina Key Laboratory of Radio Frequency and Micro-Nano Electronics of Jiangsu Province Nanjing 210023JiangsuChina Zhenjiang Kangyuan Electrical Appliance Co. Ltd.Zhenjiang 212013JiangsuChina College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina YTO Group Corporation Dongfanghong(Henan)Agricultural Service Technology Co. Ltd.Luoyang 471033HenanChina

Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.

关键词： S-doped VN Electronic structures Spin state regulation Oxygen reduction reaction zinc-air batteries

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Apically guiding electron/mass transfer reaction induced by Ag/FeNx Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 106-116页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center(Rongjiang Laboratory) Guangdong University of Technology Guangzhou Key Laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical Engineering Hainan Normal University School of Materials and Energy Guangdong University of Technology Department of Materials Science and Engineering Southern University of Science and Technology

The disparity in the transfer of carriers（electrons/mass） during the reaction in zinc-air batteries（ZABs）results in sluggish kinetics of the oxygen reduction reaction（ORR） and oxygen evolution reaction（OER）,along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst（Ag-FeNx-N-C） was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional（3D） hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride（FeNx） nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeNx,of which electron accumulation in the FeNxphase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm-2.A rechargeable ZAB with Ag-FeNx-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles（500 h）,with a power density of 180 mW cm-2.Moreover,when employing AgFeNx-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm-2.Ag-FeNx-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.

关键词： Apically guiding effect Bifunctional catalysis Hollow star structure Mott-Schottky effect zinc-air batteries

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Research progress of transition metal compounds as bifunctional catalysts for zinc-air batteries

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Nano Research Energy 2024年第1期3卷 78-100页

作者： Yan Ran Changfan Xu Deyang Ji Huaping Zhao Liqiang Li Yong Lei Fachgebiet Angewandte Nanophysik Institut für Physik&IMN MacroNanoTechnische Universität IlmenauIlmenau 98693Germany Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistryInstitute of Molecular Aggregation ScienceTianjin UniversityTianjin 300072China

zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.

关键词： transition metal compounds zinc-air batteries bifunctional catalysts electrochemical air electrode

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Wood-derived integrated air electrode with Co-N sites for rechargeable zinc-air batteries

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Nano Research 2022年第2期15卷 1415-1423页

作者： Benji Zhou Yanyan Liu Xianli Wu Huan Liu Tao Liu Yi Wang Sehrish Mehdi Jianchun Jiang Baojun Li Research Center of Green Catalysis College of ChemistryZhengzhou University100 Science RoadZhengzhou 450001China Institute of Chemical Industry of Forest Products CAFNational Engineering Lab for Biomass Chemical UtilizationNanjing 210042China College of Science Henan Agricultural UniversityZhengzhou 450002China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafery National Center for Nanoscience and TechnologyBeijing 100190China Department of Chemistry The Women UniversityKutchery CampusL.M.Q.RoadMultan 66000Pakistan

The sluggish reaction kinetics in oxygen reduction reaction(ORR)is one of the bottlenecks in next generation energy conversion systems.The integrated design strategy based on simultaneously constructing active sites and forming porous carbon network will address this concern by facilitating charge exchange,mass transfer and electron transportation.In this article,a three-dimensional integrated air electrode(Co-N@ACS)containing Co-N sites and hierarchically porous carbon is fabricated via growth of Co-doped ZIF-8 in activated wood substrate and synchronous pyrolysis.The optimized integrated air electrodes exhibit ultrahigh ORR activity(E_(1/2)=0.86 V).Co-N sites provide outstanding ORR activity,and hierarchically porous structures facilitate oxygen diffusion and electrolyte penetration.Aqueous zinc-air battery assembled with Co-N@ACS possesses open-circuit voltage of 1.46 V,peak power density of 155 mW cm^(-2) and long-term stability of 540 cycles(180 h).Solid-state zinc-air battery assembled with Co-N@ACS shows open-circuit voltage up to 1.36 V and low charge-discharge voltage gap(0.8 V).This design strategy paves the way for the conversion of wood biomass to integrated air electrodes and catalytically active carbon for next generation energy storage and conversion devices.

关键词： atomically dispersed Co integrated air electrode oxygen reduction reaction wood biomass zinc-air batteries

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Recent advances in bifunctional catalysts for zinc-air batteries:Synthesis and potential mechanisms

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Science China(Technological Sciences) 2022年第10期65卷 2221-2245页

作者： ZHAO LinWei GU TengTeng LIANG ZiWei LIU Jun School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510641China

zinc-air batteries(ZABs) are considered promising candidates for next-generation clean and sustainable energy storage devices because of their low cost, safety, environment-friendliness, and high specific energy density. However, owing to its poor chargedischarge capacity and low efficiency, its practical application remains challenging. The main obstacles are the intrinsic slow reaction kinetics on the air cathode, including the oxygen reduction reaction(ORR) during discharging and oxygen evolution reaction(OER) during recharging. Therefore, a reasonable design of bifunctional ORR/OER electrocatalysts with high activity and stability is the key to the development of ZABs. In this review, the recent advances in bifunctional ORR/OER electrocatalysts as air cathodes in ZABs are discussed from three perspectives: metal-organic framework-based catalysts, metal-free carbon catalysts, and metal-based catalysts. In particular, the synthesis, electrocatalytic activity, and potential mechanism of bifunctional catalysts in ZABs are discussed. In recent years, research on bifunctional catalysts has intensified, and the performance of these catalysts has significantly improved. However, most of the experimental products have complex preparation processes and high costs;therefore, the industrialization of these experimental products remains difficult. This review offers prospects for the optimal design of high-activity rechargeable ZAB bifunctional air cathodes.

关键词： zinc-air batteries air cathode bifunctional electrocatalysts non-noble metal catalyst

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Regulated electronic structure and improved electrocatalytic performances of S-doped FeWO4 for rechargeable zinc-air batteries

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Journal of Energy Chemistry 2023年第1期76卷 359-367,I0009页

作者： Huan Wang Li Xu Daijie Deng Xiaozhi Liu Henan Li Dong Su Institute for Energy Research School of Chemistry and Chemical EngineeringJiangsu Province and Education Ministry Co-sponsored Synergistic Innovation Center of Modern Agricultural EquipmentKey Laboratory for Theory and Technology of Intelligent Agricultural Machinery and EquipmentJiangsu UniversityZhenjiang 212013JiangsuChina Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

The exploration of active and long-lived oxygen reduction reaction(ORR)catalysts for the commercialization of zinc-air batteries are of immense significance but challenging.Herein,the sulfur doped FeWO_(4)embedded in the multi-dimensional nitrogen-doped carbon structure(S-FeWO_(4)/NC)was successfully synthesized.The doped S atoms optimized the charge distribution in FeWO_(4)and enhanced the intrinsic activity.At the same time,S doping accelerated the formation of reaction intermediates during the adsorption reduction of O_(2)on the surface of S-FeWO_(4)/NC.Accordingly,the S-FeWO_(4)/NC catalyst showed more positive half-wave potential(0.85 V)and better stability than that of the FeWO_(4)/NC catalyst.Furthermore,the S-FeWO_(4)/NC-based zinc-air battery exhibited considerable power density of 150.3m W cm^(-2),high specific capacity of 912.7 m A h g^(-1),and prominent cycle stability up to 220 h.This work provides an assistance to the development of cheap and efficient tungsten-based oxygen reduction catalysts and the promotion of its application in the zinc-air battery.

关键词： S doping FeWO4 Oxygen reduction reaction zinc-air batteries

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Heterogeneous assembling 3D free-standing Co@carbon membrane enabling efficient fluid and flexible zinc-air batteries

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Nano Research 2023年第7期16卷 9327-9334页

作者： Jinming Wang Xiangjian Liu Liuhua Li Rui Liu Yarong Liu Changli Wang Zunhang Lv Wenxiu Yang Xiao Feng Bo Wang Key Laboratory of Cluster Science Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Materials Science and EngineeringAdvanced Technology Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

Developing an efficient,interface-rich,and free-standing non-noble-metal electrocatalyst is vital for the flexible zinc-air batteries(ZABs).Herein,a three-dimensional(3D)heterogeneous carbon-based flexible membrane was assembled by Co@carbon nanosheets/carbon nanotubes and hollow carbon nanofiber(Co@NS/CNT-CNF)as an efficient oxygen reduction reaction(ORR)catalyst with a positive half-wave potential of 0.846 V and a small Tafel slope of 79 mV·dec^(-1).Meanwhile,the Co@NS/CNT-CNF electrode also exhibits excellent open-circuit voltage,peak power density,and long-time cycling stability in liquid-state ZABs(1.605 V,163 mW·cm^(-2),and 400 h)and flexible ZABs under flat/bending condition(1.47 V,102 mW·cm^(-2),and 80 h).Such heterogeneous flexible membrane architecture not only optimizes the electrolyte infiltration,but also provides capacious possibility for O_(2)and electrolyte transfer.Meanwhile,work-function analyses coupled with density functional theory(DFT)results demonstrate that the electron transfer capability and metal-support interaction can be well optimized in the obtained Co@NS/CNT-CNF catalyst.

关键词： free-standing membrane electrocatalysts carbon nanomaterials zinc-air batteries

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Edge atomic Fe sites decorated porous graphitic carbon as an efficient bifunctional oxygen catalyst for zinc-air batteries

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能源化学:英文版 2023年第8期83卷 602-611,I0014页

作者： Ruihui Gan Yali Wang Xiangwu Zhang Yan Song Jingli Shi Chang Ma Tianjin Municipal Key Lab of Advanced Fiber and Energy Storage Technology Tiangong UniversityTianjin 300387China Fiber and Polymer Science Program Department of Textile EngineeringChemistry and ScienceWilson College of TextilesNorth Carolina State UniversityRaleighNC 27695-8301uNITED sTATES CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina

The development of advanced bifunctional oxygen electrocatalysts for oxygen reduction and evolution reactions(ORR and OER) is critical to the practical application of zinc-air batteries(ZABs). Herein, a silica-assisted method is reported to integrate numerous accessible edge Fe-Nx sites into porous graphitic carbon(named Fe-N-G) for achieving highly active and robust oxygen electrocatalysis. Silica facilitates the formation of edge Fe-Nx sites and dense graphitic domains in carbon by inhibiting iron aggregation.The purification process creates a well-developed mass transfer channel for Fe-N-G. Consequently,Fe-N-G delivers a half-wave potential of 0.859 V in ORR and an overpotential of 344 m V at10 m A cm^(-2)in OER. During long-term operation, the graphitic layers protect edge Fe-Nx sites from demetallation in ORR and synergize with Fe OOH species endowing Fe-N-G with enhanced OER activity.Density functional theory calculations reveal that the edge Fe-Nx site is superior to the in-plane Fe-Nx site in terms of OH* dissociation in ORR and OOH* formation in OER. The constructed ZAB based on Fe-N-G cathode shows a higher peak power density of 133 m W cm^(-2)and more stable cycling performance than Pt/C + RuO2counterparts. This work provides a novel strategy to obtain high-efficiency bifunctional oxygen electrocatalysts through space mediation.

关键词： Bifunctionality EdgeFe-Nxsites Oxygen catalysis Graphitic domains zinc-air batteries

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