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Understanding of the charge storage mechanism of MnO_(2)-based aqueous zinc-ion batteries:Reaction processes and regulation strategies

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Journal of Energy Chemistry 2023年第7期82卷 423-463,I0010页

作者： Nan Zhang Yu-Rui Ji Jian-Cang Wang Peng-Fei Wang Yan-Rong Zhu Ting-Feng Yi School of Materials Science and Engineering Northeastern UniversityShenyang 110819LiaoningChina Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province School of Resources and MaterialsNortheastern University at QinhuangdaoQinhuangdao 066004HebeiChina

Though secondary aqueous Zn ion batteries(AZIBs)have been received broad concern in recent years,the development of suitable cathode materials of AZIBs is still a big challenge.The MnO_(2) has been deemed as one of most hopeful cathode materials of AZIBs on account of some extraordinary merits,such as richly natural resources,low toxicity,high discharge potential,and large theoretical capacity.However,the crystal structure diversity of MnO_(2) results in an obvious various of charge storage mechanisms,which can cause great differences in electrochemical performance.Furthermore,several challenges,including intrinsic poor conductivity,dissolution of manganese and sluggish ion transport dynamics should be conquered before real practice.This work focuses on the reaction mechanisms and recent progress of MnO_(2)-based materials of AZIBs.In this review,a detailed review of the reaction mechanisms and optimal ways for enhancing electrochemical performance for MnO_(2)-based materials is proposed.At last,a number of viewpoints on challenges,future development direction,and foreground of MnO_(2)-based materials of aqueous zinc ions batteries are put forward.This review clarifies reaction mechanism of MnO_(2)-based materials of AZIBs,and offers a new perspective for the future invention in MnO_(2)-based cathode materials,thus accelerate the extensive development and commercialization practice of aqueous zinc ions batteries.

关键词： Aqueous zinc-ion battery MnO_(2) charge storage mechanism Optimization strategy

High-Resolution Mass Spectroscopy for Revealing the charge storage mechanism in Batteries: Oxamide Materials as an Example

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Energy & Environmental Materials 2023年第4期6卷 195-202页

作者： Chenyang Zhang Yuan Chen Kun Fan Guoqun Zhang Jincheng Zou Huichao Dai Yanbo Gao Xiaobo Wang Minglei Mao Chengliang Wang School of Optical and Electronic Information Wuhan National Laboratory for Optoelectronics(WNLO)Optics Valley LaboratoryHuazhong University of Science and TechnologyWuhan 430074China Wenzhou Advanced Manufacturing Technology Research Institute Huazhong University of Science and TechnologyWenzhou 325035China

The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challenging,which limits the development of advanced electrode materials.Herein,high-resolution mass spectroscopy(HR-MS)is employed to detect the evolution of organic electrode materials during the redox process and reveal the charge storage mechanism,by using small molecular oxamides as an example,which have ortho-carbonyls and are therefore potential electrochemical active materials for batteries.The HR-MS results adequately proved that the oxamides could reversibly store lithium ions in the voltage window of 1.5–3.8 V.Upon deeper reduction,the oxamides would decompose due to the cleavage of the C–N bonds in oxamide structures,which could be proved by the fragments detected by HR-MS,^(1)H NMR,and the generation of NH_(3)after the reduction of oxamide by Li.This work provides a strategy to deeply understand the charge storage mechanism of organic electrode materials and will stimulate the further development of characterization techniques to reveal the charge storage mechanism for developing high-performance electrode materials.

关键词： charge storage mechanism high-resolution mass spectroscopy organic batteries organic electrodes oxamides

charge storage mechanism of MOF-derived Mn2O3 as high performance cathode of aqueous zinc-ion batteries

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Journal of Energy Chemistry 2021年第1期30卷 277-283,I0009页

作者： Min Mao Xingxing Wu Yi Hu Qunhui Yuan Yan-Bing He Feiyu Kang Tsinghua Shenzhen International Graduate School Division of Energy&EnvironmentTsinghua UniversityShenzhen 518055GuangdongChina Laboratory of Advanced Materials Department of Materials Science and EngineeringTsinghua UniversityBeijing 100084China State Key Laboratory of Advanced Welding and Joining and School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055GuangdongChina

Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most important cathode materials of ZIB.In this paper,α-Mn2O3 used as cathode of ZIB is synthesized via Metal-Organic Framework(MOF)-derived method,which delivers a high specific capacity of225 mAh g^(-1) at 0.05 A g^(-1) and 92.7 mAh g^(-1) after 1700 cycles at 2 A g^(-1).The charge storage mechanism of α-Mn2O3 cathode is found to greatly depend on the discharge current density.At lower current density discharging,the H+ and Zn2+ are successively intercalated into the α-Mn2O3 before and after the "turning point" of discharge voltage and their discharging products present obviously different morphologies changing from flower-like to large plate-like products.At a higher current density,the low-voltage plateau after the turning point disappears due to the decrease of amount of Zn2+ intercalation and the H+intercalation is dominated in α-Mn2 O3.This study provides significant understanding for future design and research of high-performance Mn-based cathodes of ZIB.

关键词： Zinc ion batteries α-Mn2O3 Metal-organic framework(MOF) charge storage mechanism

charge storage mechanism of copper hexacyanoferrate nanocubes for supercapacitors

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Chinese Chemical Letters 2020年第5期31卷 1213-1216页

作者： Zhaoxia Song Wei Liu Xiaofei Wei Quan Zhou Hongda Liu Zheng Zhang Guichang Liu Zhongfu Zhao Department of Chemical Engineering College of Life ScienceDalian Minzu UniversityDalian 116600China School of Chemical Engineering Dalian University of TechnologyDalian 116024China

The widely accepted theory concerning the electrochemical energy storage mechanism of copper hexacyanoferrate(CuHCF)for supercapacitors is that CuHCF stores charge by the reversible redox processes of Fe^3+/Fe2+couple and Cu cations are electrochemically inactive.In this work,CuHCF nanocubes(CuHCF-NC)were synthesized in the presence of potassium citrate and its electrochemical properties were tentatively studied in 1 mol/L Na2 SO4 aqueous electrolyte.Good supercapacitive performance was exhibited.The combined analyses of cyclic voltammogram(CV)and X-ray photoelectron spectroscopy(XPS)disclosed that the CuHCF nanocubes underwent the redox reactions of Fe^3+/Fe2+and Cu^2+/Cu+couples to store charges.The Cu^2+/Cu+redox couple was activated due to the strong coordination interaction between the carboxylate groups of citrate ions and surface Cu cations.

关键词： Copper hexacyanoferrate Supercapacitor Electrode material charge storage mechanism Redox couple

Electrochemical Proton storage:From Fundamental Understanding to Materials to Devices

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Nano-Micro Letters 2022年第8期14卷 1-23页

作者： Tiezhu Xu Di Wang Zhiwei Li Ziyang Chen Jinhui Zhang Tingsong Hu Xiaogang Zhang Laifa Shen Jiangsu Key Laboratory of Electrochemical Energy storage Technologies College of Material Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 211106People’s Republic of China

Simultaneously improving the energy density and power density of electrochemical energy storage systems is the ultimate goal of electrochemical energy storage technology.An effective strategy to achieve this goal is to take advantage of the high capacity and rapid kinetics of electrochemical proton storage to break through the power limit of batteries and the energy limit of capacitors.This article aims to review the research progress on the physicochemical properties,electrochemical performance,and reaction mechanisms of electrode materials for electrochemical proton storage.According to the different charge storage mechanisms,the surface redox,intercalation,and conversion materials are classified and introduced in detail,where the influence of crystal water and other nanostructures on the migration kinetics of protons is clarified.Several reported advanced full cell devices are summarized to promote the commercialization of electrochemical proton storage.Finally,this review provides a framework for research directions of charge storage mechanism,basic principles of material structure design,construction strategies of full cell device,and goals of practical application for electrochemical proton storage.

关键词： Electrochemical proton storage Rapid kinetics charge storage mechanism Material design Device construction

Enhancing charge storage of O-doped perovskite fluorides via in-situ electrochemical oxidation for high-performance potassium-ion capacitors

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Journal of Materials Science & Technology 2023年第27期158卷 111-120页

作者： Jing Zhao Zicheng Cai Yue Fan Yunan Wang Yu Song Jie Liu Shuangwen Li Di Guo Xiaoxia Liu Department of Chemistry Northeastern UniversityShenyang 110819China School of Resources and Civil Engineering Northeastern UniversityShenyang 110819China National-local Joint Engineering Research Center of High-efficient Exploitation Technology for Refractory Iron Ore Resources Shenyang 110819China School of Materials Engineering North China Institute of Aerospace EngineeringLangfang 065000China

Potassium ion capacitors(PICs)are regarded as promising large-scale aqueous energy storage systems.However,due to the poor K^(+)transport kinetics and the structural instability of the cathode materials,the key issues of limited energy density and poor cyclic stability are obstacles to the in-depth growth of PICs.Herein,a novel O-doped perovskite fluoride is demonstrated via an in-situ electrochemical oxidation strategy as the cathode for PICs,introducing additional defects that improve the capacitance and facilitate the reaction kinetics of the electrode.During the electrochemical oxidation process,it is discovered that the perovskite fluoride crystal tends to transform into disordered O-doped KMnF 3(K_(x)MnF_(y)O_(z)),realizing a structural reconstruction at the electrode material/electrolyte interface.The First-principles calculations based on density functional theory(DFT)are performed to confirm that the improved electrical conduc-tivity and low ionic adsorption energy may be ascribed to the substitution of oxygen for fluorine.The obtained K_(1.14)MnF_(1.17)O_(1.26) cathode achieves a high specific capacitance of 694 F g^(-1) at 1 A g^(-1),as well as high capacitance retention of 91.3%after 10,000 charge/discharge cycles in mild K_(2)SO_(4) electrolyte.This study provides an effective strategy to improve the capacitive performance of perovskite fluoride cathode materials in electrochemical energy storage.

关键词： Perovskite fluorides O-doped Potassium-ion capacitors charge storage mechanism

Mechanistic understanding of the charge storage processes in FeF_(2) aggregates assembled with cylindrical nanoparticles as a cathode material for lithium-ion batteries by in situ magnetometry

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Carbon Energy 2022年第6期4卷 1011-1020页

作者： Zhengqiang Hu Fengling Zhang Huanyu Liang Hao Zhang Huaizhi Wang Tiansheng Wang Renbin Liu Jie Liu Yadong Li Xiaotong Dong Lianyu Bao Zhuan Liang Yaqun Wang Shishen Yan Qiang Li Hongsen Li Center for Marine Observation and Communications College of PhysicsQingdao UniversityQingdaoShandongChina College of Electrical Engineering and Automation Shandong University of Science and TechnologyQingdaoShandongChina State Key Laboratory of Crystal Materials School of PhysicsShandong UniversityJinanShandongChina

Transition metal fluorides(TMFs)cathode materials have shown extraordinary promises for electrochemical energy storage,but the understanding of their electrochemical reaction mechanisms is still a matter of debate due to the complicated and continuous changing in the battery internal environment.Here,we design a novel iron fluoride(FeF_(2))aggregate assembled with cylindrical nanoparticles as cathode material to build FeF_(2) lithium-ion batteries(LIBs)and employ advanced in situ magnetometry to detect their intrinsic electronic structure during cycling in real time.The results show that FeF_(2) cannot be involved in complete conversion reactions when the FeF_(2) LIBs operate between the conventional voltage range of 1.0–4.0 V,and that the corresponding conversion ratio of FeF_(2) can be further estimated.Importantly,we first demonstrate that the spin-polarized surface capacitance exists in the FeF_(2) cathode by monitoring the magnetic responses over various voltage ranges.The research presents an original and insightful method to examine the conversion mechanism of TMFs and significantly provides an important reference for the future artificial design of energy systems based on spinpolarized surface capacitance.

关键词： charge storage mechanism FeF_(2)cathode materials in situ magnetometry lithium-ion batteries

Iron anode-based aqueous electrochemical energy storage devices: Recent advances and future perspectives

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Interdisciplinary Materials 2022年第1期1卷 116-139页

作者： Jian Jiang Jinping Liu Chongqing Key Lab for Advanced Materials and Clean Energies of Technologies School of Materials and EnergySouthwest UniversityChongqingChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of ChemistryChemical Engineering and Life ScienceWuhan University of TechnologyWuhanChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbinChina

The ever-growing demands for green and sustainable power sources for ap-plications in grid-scale energy storage and portable/wearable devices have enabled the continual development of advanced aqueous electrochemical energy storage(EES)systems.Aqueous batteries and supercapacitors made of iron-based anodes are one of the most promising options due to the remark-able electrochemical features and natural abundance,pretty low cost and good environmental friendliness of ferruginous species.Though impressive ad-vances in developing the state-of-the-art ferruginous anodes and designing various full-cell aqueous devices have been made,there still remain key issues and challenges on the way to practical applications,which urgently need discussing to put forwards possible solutions.In this review,rather than focusing on the detailed methods to optimize the iron anode,electrolyte,and device performance,we first give a comprehensive review on the charge storage mechanisms for ferruginous anodes in different electrolyte systems,as well as the newly developed iron-based aqueous EES devices.The deep in-sights,involving the inherent failure mechanisms and corresponding modification/optimization strategies toward iron anodes for the development of high-performance aqueous EES devices,will then be discussed.The advances in applying iron-based aqueous EES devices for emerging fields such as flexible/wearable electronics and functionalized building materials will be further outlined.Last,future research trends and perspectives for maximizing the potential of current iron anodes and devices as well as exploiting brand-new iron-based aqueous EES systems are put forward.

关键词： aqueous batteries battolyser charge storage mechanism hybrid supercapacitors iron anode

Electrochemically activated nickel-cobalt double hydroxide for aqueous ammonium-zinc hybrid battery

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Nano Research 2023年第2期16卷 2495-2501页

作者： Qing Pan Peng Hei Yu Song Jianming Meng Chang Liu Xiao-Xia Liu Department of Chemistry Northeastern UniversityShenyang 110819China National Frontiers Science Center for Industrial Intelligence and Systems Optimization Northeastern UniversityShenyang 110819China Key Laboratory of Data Analytics and Optimization for Smart Industry(Northeastern University) Ministry of EducationShenyang 110819China

Aqueous rechargeable ammonium-ion(NH^(4+))batteries(AAIBs)with ammonium ions as charge carriers possess many advantages,yet the relatively low discharge capacities(e.g.,storage properties of an electrochemically activated NiCo double hydroxide(A-NiCo-DH)in neutral ammonium acetate electrolyte for the first time.The activation process extracts the interlayer anions(NO3from the host material,providing additional cation accommodation sites for charge storage.The introduced H vacancies in A-−)NiCo-DH could activate the O sites,leading to the enhanced cation adsorption capability for the electrode.Therefore,A-NiCo-DH exhibits a high discharge capacity of 280.6 mAh·g^(−1)at 0.72 A·g^(−1)with good rate capability.Spectroscopy studies suggest A-NiCo-DH experiences a NH4+/H+coinsertion mechanism.A NH4+-Zn hybrid cell is assembled using A-NiCo-DH as the cathode and Zn foil as the anode,respectively.The device delivers an energy density of 306 Wh·kg^(−1)at the power density of 745.8 W·kg^(−1)(based on the active mass of A-NiCo-DH).This work provides a new NH_(4)^(+)storage material and would push forward the development of aqueous NH4+-based batteries.

关键词： Ni-Co double hydroxide electrochemical activation charge storage mechanism high capacity ammonium-ion battery