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Enhancing zinc-air battery performance by constructing threedimensional N-doped carbon coating multiple valence Co and MnO heterostructures

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Nano Research 2024年第6期17卷 5104-5113页

作者： Qi Liu Panzhe Qiao Miaomiao Tong Ying Xie Xinxin Zhang Kuo Lin Zhijian Liang Lei Wang Honggang Fu Key Laboratory of Superlight Materials and Surface Technology of the Ministry of Education of the People’s Republic of China Harbin Engineering UniversityHarbin 150080China Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of China Heilongjiang UniversityHarbin 150080China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China

Developing highly-efficient bifunctional oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)electrocatalysts is crucial for the widespread application of rechargeable zn-air batteries(ZABs).Herein,an efficiency electrodeposition and pyrolytic strategy to synthesize the three-dimensional(3D)N-doped carbon coating multiple valence Co and MnO heterostructures supported on carbon cloth substrate(Co-MnO@NC/CC).It contains Co-Co,Co-N,and Co-O bonds,which synergistically enhance the oxygen reaction activity with MnO.It exhibits a working potential of 1.473 V at 10 mA·cm^(−2)for OER and onset potential of 0.97 V for ORR.Theory calculations demonstrate that the synergy between cobalt and manganese species could optimize the d-band center and reduce the energy barrier of Co-MnO@NC/CC for both OER and ORR processes.Besides,the MnO acts as the main OER active site could significantly optimize the energy barrier of O*→OOH*,thus further promoting the OER activity.It can be directly used as the air-cathode for both liquid-state and solid-state ZABs,which could afford a small voltage gap of 0.75 V at 10 mA·cm^(−2),a high power density of 172.5 mW·cm^(−2)and a long-term durability for 400 h,surpassing those of the Pt/C+RuO_(2)-based ZAB.Importantly,the assembled batteries show potential applications in portable devices.

关键词： heterostructure synergy valence cobalt manganese oxide zn-air battery

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Light-assisted rechargeable zinc-air battery:Mechanism,progress,and prospects

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Journal of Energy Chemistry 2024年第4期91卷 178-193页

作者： Jiangchang Chen Jinlong Luo Youlin Xiang Yingjian Yu College of Physics Science and Technology Kunming UniversityKunming 650214YunnanChina

Exploring effective energy storage systems is critical to alleviate energy scarcity.Rechargeable zinc-air batteries are promising energy storage devices.However,conventional rechargeable zinc-air battery systems face many challenges associated with electrolytes and electrodes,causing inferior electrochemistry performance.The light-assisted strategy represents a novel and innovative approach to conventional zinc-air battery technology that uses only electrical energy.This strategy effectively combines both light and electrical energy conversion/storage mechanisms.In addition,light-assisted rechargeable zinc-air batteries can achieve photocharging with or without applied electrical bias by partially using solar energy and the acceleration of oxygen reduction/evolution reaction kinetics.In this paper,the working mechanism and structural design of the light-assisted rechargeable zinc-air batteries are introduced based on the theory of photoelectrochemistry and its characteristics.Then,the latest advances in electrolyte and photocathode design strategies are discussed in detail.The performance enhancement of aqueous light-assisted rechargeable zinc-air batteries using photoelectric materials is explained.Finally,a summary and outlook on the further modification of properties of light-assisted rechargeable zinc-air batteries,especially the photovoltaic electrode catalyst design strategies,are illustrated.This review provides insights and guidance for the design of high-performance light-assisted rechargeable zn-air batteries for next-generation energy storage devices.

关键词： zn-air battery Light-assisted Electrolyte Catalyst Semiconductor

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WC/Co_(7)Fe_(3)heterojunction embedded in N,P co-doped hierarchical carbon enables rechargeable/flexible zn-air battery

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Nano Research 2023年第2期16卷 2519-2527页

作者： Huimin Mao Xiaobin Liu Siqi Wu Yixin Fu Guishan Liu Guizhong Zhou Lei Wang Key Laboratory of Eco-chemical Engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingQingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042China Chaofeng Steel Structure Group Co. Ltd.Hangzhou 311215China

Rational design and synthesis of bifunctional oxygen electrocatalysts with high activity and stability are key challenges in the development of rechargeable zn-air batteries(ZABs).In this paper,tungsten carbide(WC)and Co_(7)Fe_(3)embedded in N,P co-doped hierarchical carbon(WC/Co_(7)Fe_(3)-NPHC)was prepared by using zeolite imidazolate frameworks as precursor.Density functional theory demonstrates that the mutual adjustment among the WC,Co_(7)Fe_(3),and N,P co-doped carbon at the three-phase heterojunction interface makes the catalyst possess moderate adsorption strength,and greatly improves the conductivity and electron transfer rate of the catalyst.As a result,the WC/Co_(7)Fe_(3)-NPHC exhibits a low overall oxygen redox potential difference of 0.72 V,while the ZAB assembled by WC/Co_(7)Fe_(3)-NPHC as an air cathode exhibits ultra-long cycle stability of over 550 h.Futhermore,WC/Co_(7)Fe_(3)-NPHC can keep good charge and discharge stability at different bending angles when applied to flexible solid ZAB.

关键词： heterojunction hierarchical structure bifunctional oxygen electrocatalyst zn-air battery

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Confinement synthesis of bimetallic MOF-derived defect-rich nanofiber electrocatalysts for rechargeable zn-air battery

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Nano Research 2022年第10期15卷 9000-9009页

作者： Xing Chen Jie Pu Xuhui Hu Le An Jianjun Jiang Yujun Li School of Mechanical Engineering Northwestern Polytechnical UniversityXi’an 710072China Frontiers Science Center for Flexible Electronics Institute of Flexible ElectronicsNorthwestern Polytechnical UniversityXi’an 710072China College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China

zn-air batteries with high energy density and safety have acquired enormous attention,while the practical application is hindered by the sluggish kinetics of the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR).In this work,a threedimensional(3D)defect-rich bifunctional electrocatalyst(CoFe/N CNFs)comprising irregular hollow CoFe nanospheres in Ndoped carbon nanofibers is presented,which is fabricated from CoFe ZIFs-derived(ZIF:zeolitic-imidazolate framework)polymer nanofibers precursor.The CoFe ZIFs with tunable particle size and composition are constructed using a confined synthesis strategy.Moreover,the Kirkendall diffusion process is available for forming the irregular hollow CoFe nanospheres,and the decomposition of polyvinylpyrrolidone(PVP)results in forming the defective carbon nanofibers,which provide more efficient active sites and enhance the electrocatalytic properties toward both OER and ORR.The optimized CoFe/N CNFs exhibit superior bifunctional activities,outperforming that of the benchmark Pt/C+RuO_(2) catalyst.As a result,the CoFe/N CNFs as an air-cathode endow the rechargeable zn-air battery with an excellent power density of 149 mW·cm^(−2),energy density of 875 Wh·kg^(−1),and cycling stability.This work provides a new strategy to develop bifunctional electrocatalysts with desired nanostructure and regulated performance toward energy applications.

关键词： defect-rich electrocatalyst hollow structure carbon fiber metal-organic framework zn-air battery

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Hierarchically porous Co@N-doped carbon fiber assembled by MOF-derived hollow polyhedrons enables effective electronic/mass transport:An advanced 1D oxygen reduction catalyst for zn-air battery

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Journal of Energy Chemistry 2023年第1期76卷 117-126,I0004页

作者： Yifei Zhang Quanfeng He Zihao Chen Yuqing Chi Junwei Sun Ding Yuan Lixue Zhang Industrial Research Institute of Nonwovens&Technical Textiles College of Textiles&ClothingQingdao UniversityQingdao 266071ShandongChina College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071ShandongChina College of Chemistry and Chemical Engineering Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)Xiamen UniversityXiamen 361005FujianChina

Developing advanced oxygen reduction reaction(ORR)electrocatalysts with rapid mass/electron transport as well as conducting relevant kinetics investigations is essential for energy technologies,but both still face ongoing challenges.Herein,a facile approach was reported for achieving the highly dispersed Co nanoparticles anchored hierarchically porous N-doped carbon fibers(Co@N-HPCFs),which were assembled by core-shell MOFs-derived hollow polyhedrons.Notably,the unique one-dimensional(1D)carbon fibers with hierarchical porosity can effectively improve the exposure of active sites and facilitate the electron transfer and mass transfer,resulting in the enhanced reaction kinetics.As a result,the ORR performance of the optimal Co@N-HPCF catalysts remarkably outperforms that of commercial Pt/C in alkaline solution,reaching a limited diffusion current density(J)of 5.85 m A cm^(-2)and a half-wave potential(E_(1/2))of 0.831 V.Particularly,the prepared Co@N-HPCF catalysts can be used as an excellent air-cathode for liquid/solid-state zn-air batteries,exhibiting great potentiality in portable/wearable energy devices.Furthermore,the reaction kinetic during ORR process is deeply explored by finite element simulation,so as to intuitively grasp the kinetic control region,diffusion control region,and mixing control region of the ORR process,and accurately obtain the relevant kinetic parameters.This work offers an effective strategy and a reliable theoretical basis for the engineering of first-class ORR electrocatalysts with fast electronic/mass transport.

关键词： Oxygen reduction catalyst Metal-organic frameworks Carbon nanofiber Hierarchically porous structure Diffusion kinetics zn-air battery

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Hierarchical porous yolk-shell Co-N-C nanocatalysts encaged in graphene nanopockets for high-performance zn-air battery

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Nano Research 2023年第7期16卷 8893-8901页

作者： Yisi Liu Zongxu Li Shizhu Wang Jinnan Xuan Dongbin Xiong Lina Zhou Jianqing Zhou Jun Wang Yahui Yang Yue Du Institute for Advanced Materials Hubei Normal UniversityHuangshi 435002China Jiangsu Key Laboratory of Materials and Technology for Energy Conversion College of Material Science and EngineeringNanjing University of Aeronautics and AstronauticsNanjing 210016China National&Local Joint Engineering Laboratory for New Petro-chemical Materials and Fine Utilization of Resources College of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China

The rational design and preparation of promising cathode electrocatalysts with excellent activity and strong stability for metal-air batteries is a huge challenge.In this work,we innovate an approach of combining solvothermal with high-temperature pyrolysis utilizing zeolitic imidazolate framework(ZIF)-8 and ZIF-67 as the template to synthesize a novel hybrid material of hierarchical porous yolk-shell Co-N-C polyhedron nanocatalysts engaged in graphene nanopocket(yolk-shell Co-N-C@GNP).The obtained catalyst exhibits prominent bifunctional electrocatalytic performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)in the alkaline condition,in which the half-wave potential is 0.86 V for ORR,and the over-potential for OER is 0.42 V at 10 mA·cm^(-2).The rechargeable aqueous zn-air battery fabricated with yolk-shell Co-N-C@GNP cathode deliveries an open circuit voltage(OCV)of 1.60 V,a peak power density of 236.2 mW·cm^(-2),and excellent cycling stability over 94 h at 5 mA·cm^(-2).The quasi-solid-state zn-air battery(ZAB)using yolk-shell Co-N-C@GNP displays a high OCV of 1.40 V and a small voltage gap of 0.88 V in continuous cycling tests at 2 mA·cm^(-2).This work provides a valuable thought to focus attention on the design of high-efficient bifunctional catalysts with hierarchical porous yolk-shell framework and high-density metal active sites for metal-air battery technologies.

关键词： zeolitic imidazolate framework(ZIF)-67@ZIF-8 yolk-shell graphene nanopocket Bi-functional catalysts zn-air battery

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Regulating electronic structure of CoN_(4)with axial Co-S for promoting oxygen reduction and zn-air battery performance

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Nano Research 2023年第4期16卷 4211-4218页

作者： Chang Chen Zhiqiang Chen Junxi Zhong Xin Song Dongfang Chen Shoujie Liu Weng-Chon Cheong Jiazhan Li Xin Tan Chang He Jiaqi Zhang Di Liu Qiuhua Yuan Chen Chen Qing Peng Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Beijing Key Laboratory of Research and Application for Aerospace Green Propellants Beijing Institute of Aerospace Testing TechnologyBeijing 100048China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China State Key Laboratory of Automtive Safety and Energy Tsinghua UniversityBeijing 100084China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacao 999078China

Regulating the coordination environment of transition-metal based materials in the axial direction with heteroatoms has shown great potential in boosting the oxygen reduction reaction(ORR).The coordination configuration and the regulation method are pivotal and elusive.Here,we report a combined strategy of matrix-activization and controlled-induction to modify the CoN_(4)site by axial coordination of Co-S(Co1N_(4)-S_(1)),which was validated by the aberration-corrected electron microscopy and X-ray absorption fine structure analysis.The optimal Co1N_(4)-S_(1)exhibits an excellent alkaline ORR activity,according to the half-wave potential(0.897 V vs.reversible hydrogen electrode(RHE)),Tafel slope(24.67 mV/dec),and kinetic current density.Moreover,the Co1N_(4)-S_(1)based zn-air battery displays a high power density of 187.55 mW/cm^(2)and an outstanding charge-discharge cycling stability for 160 h,demonstrating the promising application potential.Theoretical calculations indicate that the better regulation of CoN_(4)on electronic structure and thus the highly efficient ORR performance can be achieved by axial Co-S.

关键词： electronic structure regulation axial Co-S coordination single-atom Co oxygen reduction zn-air battery

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Lattice confined Ru single sites in hollow Co_(9)S_(8)polyhedron triggering Co-S-Ru catalytic centers for rechargeable zn-air battery

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Nano Research 2023年第5期16卷 6701-6709页

作者： Xuan Liu Siru Chen Huicheng Wang Anmin Liu Shizheng Wen Liwei Mi Yanqiang Li School of Chemical Engineering Dalian University of TechnologyPanjin CampusPanjin 124221China School of Material and Chemical Engineering Center for Advanced Materials ResearchZhongyuan University of TechnologyZhengzhou 450007China School of Materials Science and Engineering North China University of Water Resources and Electric PowerZhengzhou 450045China School of Physics and Electronic Electrical Engineering Huaiyin Normal UniversityHuai’an 223300China

Single-atom catalysts with precise structure and tunable coordination nature provide opportunities for developing novel catalytic centers and understanding reaction mechanisms.Herein,hollow Co_(9)S_(8)polyhedrons with lattice-confined Ru single atoms(Ru-Co_(9)S_(8))are fabricated.Aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy verify the isolated Ru atoms are confined in Co_(9)S_(8)to form Co-S-Ru catalytic centers.Theoretical calculations indicate that the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)energy barriers are extensively reduced,the d-band center of Co_(9)S_(8)downshifts from the Fermi level,therefore boosting the desorption of O-containing intermediates.Consequently,the Ru-Co_(9)S_(8)exhibits an ultralow overpotential of 163 mV at 10 mA·cm^(−2)for OER and could catalyze a rechargeable zn-air battery with a high-power density of 92.0 mW·cm^(−2).This work provides a promising approach for designing novel bifunctional catalytic active centers for energy conversion.

关键词： electrocatalysis single-atom catalysts lattice confinement bifunctional catalysts zn-air battery

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Atomically dispersed Fe-Ni dual sites in heteroatom doped carbon tyres for efficient oxygen electrocatalysis in rechargeable zn-air battery

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能源化学:英文版 2023年第8期83卷 264-274,I0008页

作者： Zili Wang Caiyun Li Yukun Liu Yu Wu Sen Zhang Chao Deng Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationCollege of chemistry and chemical engineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina College of Material Science and Chemical Engineering Harbin Engineering UniversityHarbin 150001HeilongjiangChina

The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs) attractive for oxygen electrocatalysis. The catalytic activities of DACs are largely decided by their surrounding micro-environment and supporting substrates. Modulating the micro-environment as well as engineering the efficient support is challenging tasks. Moreover, both are critical to optimizing the performance of DACs. Herein, a novel bio-cooperative strategy is developed to synthesize Fe Ni-DAC wherein Fe-Ni dual-atom sites are embedded in the N, P codoped tyre shaped carbon matrix. The configuration matching of Fe-Ni dual centers together with the local electronic engineering of N, P heteroatoms synergistically boost the catalytic activity on the oxygen reaction. Furthermore, the central-hollow highlyporous carbon matrix not only gives rise to a large amount of active sites, but also facilitates fast kinetics.Taking advantage of both the DAC and the substrate, the Fe Ni-NPC hollow tyre(HT) catalyst scores high in both oxygen reduction and evolution reactions, which exhibits the narrow potential difference and excellent durability. The aqueous zn-air full battery(ZAB) integrating the Fe Ni-NPC HT air cathode has a high power density and a good stability over long-term cycling. Moreover, the flexible solid-state ZAB assembled with the polymer electrolyte obtains the high reliability over a wide range of temperatures or under diverse outside deformations. Therefore, this work offers a new green approach to prepare highly efficient DACs with built-in modulated micro-environment and tailor-made substrates. Moreover,it also paves a new way to develop highly-pliable power source for flexible electronics.

关键词： FeNi dual sites P,N codoped carbon Bio-assisted stategy zn-air battery

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Vacancy-modified bimetallic FeMoS_(x)/CoNiP_(x) heterostructure array for efficient seawater splitting and zn-air battery

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Journal of Energy Chemistry 2023年第6期81卷 533-542,I0012页

作者： Ansheng Wang Shan Gao Jiaguo Yan Chunning Zhao Meng Yu Weichao Wang Integrated Circuits and Smart System Lab(Shenzhen) Renewable Energy Conversion and Storage CenterTianjin Key Laboratory of Photo-Electronic Thin Film Device and TechnologyCollege of Electronic Information and Optical EngineeringNankai UniversityTianjin 300071China Department of Physical Science and Technology Ningbo UniversityNingbo 315211ZhejiangChina Division of Oilfield Chemicals China Oilfield Services LimitedTianjin 300452China

The development of highly efficient OER catalysts with superior durability for seawater electrolysis and zn-air battery is important but challenging.Herein,the vacancy-modified heterostructured bimetallic Fe Mo S_(x)/Co Ni P_(x)OER electrocatalyst is exploited.Benefiting from the electron redistribution and reaction kinetics modulation resulting from vacancy introduction and heterojunction formation,it yields ultralow OER overpotentials of 196,276,303 m V in 1 M KOH and 197,318,348 m V in 1 M KOH+seawater at 10,500,1000 m A cm^(-2),respectively,surviving 600 h at 800 m A cm^(-2)without obvious decay.Further,FeMoS_(x)/CoNiP_(x)-based zn-air battery not only affords the high peak power density of 214.5 m W cm^(-2)but also exhibits the small voltage gap of 0.698 V and long lifetime of 500 h at 10 m A cm^(-2),overmatching overwhelming majority of reported advanced catalysts.It is revealed experimentally that the OER process on rationally designed Fe Mo S_(x)/Co Ni P_(x)follows the adsorbate evolution mechanism and the ratedetermining step shifts from^(*)OOH formation in individual building blocks to^(*)OOH deprotonation process in FeMoS_(x)/CoNiP_(x),providing the directly proof of how the vacancy introduction and heterojunction formation affect the reaction kinetics.

关键词： Vacancy Heterojunction Oxygen evolution reaction Seawater splitting zn-air battery

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