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Insights into interfacial speciation and deposition morphology evolution at Mg-electrolyte interfaces under practical conditions

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Journal of Energy Chemistry 2020年第9期29卷 299-307,I0009页

作者： Zihao Song Zhonghua Zhang Aobing Du Shamu Dong Guicun Li Guanglei Cui College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101ShandongChina

Rechargeable magnesium(Mg)battery technologies show the promise of low cost,less safety concerns and relatively higher energy *** the critical issues on the Mg stripping/plating performance as well as the Mg metal anode-electrolyte interfacial chemistry is one great importance under the practical areal capacity and rate *** this work,we systematically investigate the electrochemistry of Mg stripping/plating processes within four distinctive Mg-ion electrolytes and the Mg anodeelectrolyte interfacial chemistry under practical *** results show that the cycle life of Mg//Cu asymmetric cells using these above electrolytes is significantly shortened(less than 10 cycles)when tested at a practical areal capacity of 10 mAh cm^-*** optical and electron microscopic analyses reveal that the gradual growth of the Mg deposits is susceptible to detachment from the copper substrate,where the initial nucleation process might *** spite of showing an interconnected particle-like morphology,the Mg deposits could easily penetrate the porous separator,leading to cell *** co-deposition of metallic Al is revealed from surface region to bulk,while the Cl-containing species exist in the near surface of Mg *** work not only highlights the critical impacts of areal capacity on the performances of Mg stripping/plating process,but calls for further efforts to eliminating the safety concerns of Mg anode under practical conditions.

关键词： magnesium battery Interfacial chemistry magnesium stripping/plating Aluminum co-deposition

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Design of metal-organic frameworks for improving pseudo-solid-state magnesium-ion electrolytes:Open metal sites,isoreticular expansion,and framework topology

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Journal of Materials Science & Technology 2023年第13期144卷 15-27页

作者： Yun Zheng Junpo Guo De Ning Yike Huang Wen Lei Jing Li Jianding Li Götz Schuck Jingjun Shen Yan Guo Qi Zhang Hao Tian Hou Ian Huaiyu Shao Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeMacao 999078China Centre for Photonics Information and Energy Materials Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and TechnologyWuhan 430081China School of Science Huzhou UniversityHuzhou 313000China Helmholtz-Center Berlin for Materials and Energy Albert-Einstein-StreetBerlin 1512489Germany Cancer Center and Institute of Translational Medicine Faculty of Health SciencesUniversity of MacaoMacao 999078China

The design criteria for metal-organic frameworks(MOFs)have been established by evaluating the rela-tionship between their key characteristics and magnesium-ion conductivity based on three types of sec-ondary building blocks(Zn_(4)O(CO_(2))_(6):MOF-5 and MOF-177;Cu_(2)(CO_(2))4:MOF-199,MOF-143,MOF-14,and MOF-399;Cu_(2)O_(2)(CO_(2))2:Cu-MOF-74)to achieve pseudo-solid-state magnesium-ion *** found that open-metal sites and channel layouts play a pivotal role in promoting magnesium-ion transport dy-namics at reduced activation energy,transforming MOF scaffolds into ionic-channel analogs.X-ray ab-sorption spectroscopy combined with Raman and Fourier-transform infrared spectroscopy predicted the chemical environment,solvents,and anions that occupied coordinatively unsaturated metal *** chemical compositions of electrolytes determined by^(1)H-NMR(nuclear magnetic resonance)and organic elemental analysis confirmed that isoreticular expansion increases the molar percentage of charge carri-ers,providing high *** current research systematically reveals the impacts of different MOF characteristics on ionic conduction performance,paving the way for the construction of a new class of fast and selective multivalent-ion pseudo-solid electrolytes.

关键词： magnesium conduction magnesium battery Metal-organic frameworks Solid-state electrolytes Reticular chemistry

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A rapid solid-state synthesis of electrochemically active Chevrel phases （Mo6T8; T = S, Se） for rechargeable magnesium batteries

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Nano Research 2017年第12期10卷 4415-4435页

作者： Partha Saha Prashanth H. Jampani Moni K. Datta Daeho Hong Bharat Gattu Prasad Patel Karan S. Kadakia Ayyakkannu Manivannan Prashant N. Kumta Department of Bioengineering Swanson School of Engineering University of Pittsburgh Pittsburgh PA 15261 USA U.S. Department of Energy National Energy Technology Laboratory Morgantown WV26507 USA Mechanical Engineering and Materials Science Swanson School of Engineering University of Pittsburgh Pittsburgh PA 15261 USA Chemical and Petroleum Engineering Swanson School of Engineering University of Pittsburgh Pittsburgh PA 15261 USA School of Dental Medicine University of Pittsburgh Pittsburgh PA 15251 USA Center for Complex Engineered Multifunctional Materials University of Pittsburgh Pittsburgh PA 15261 USA Present address: Department of Ceramic Engineering Nationallnstitute ofTechnology-Rourkela Odisha-769008 India

High energy mechanical milling （HEMM） of a stoichiometric mixture of molybdenum and metal chalcogenides （CuT and MOT2; T = S, Se） followed by heat treatment at elevated temperatures was successfully applied to synthesize Chevrel phases （Cu2Mo6T8; T = S, Se） as positive electrodes for rechargeable magnesium batteries. Differential scanning calorimetry （DSC）, thermogravimetric analyses （TGA）, X-ray diffraction （XRD）, and scanning electron microscopy （SEM） were used to understand the phase formation following milling and heat treatment. CuS and Mo were observed to react at 714-800 K and formed an intermediate ternary Chevrel phase （Cu1.83Mo3S4）, which further reacted with residual Mo and MoS2 to form the desired Cu2MosSs. Quantitative XRD analysis shows the formation of a -96%-98% Chevrel phase at 30 min following the milling and heat treatment. The electrochemical performance of de-cuprated Mo6S8 and Mo6Ses phases were evaluated by cyclic voltammetry （CV）, galvanostatic cycling, and electrochemical impedance spectroscopy （EIS）. The results of the CV and galvanostatic cycling data showed the expected anodic/cathodic behavior and a stable capacity after the first cycle with the formation of MgxMo6T8 （T = S, Se; 1 ≤ x 〈 2）. EIS at -0.1 V intervals for the Mo6Ss electrode during the first and second cycle shows that partial Mg-ion trapping resulted in an increase in charge transfer resistance Re. In contrast, the interfacial resistance Ri remained constant, and no significant trapping was evident during the galvanostatic cycling of the Mo6,Se8 electrode. Importantly, the ease of preparation, stable capacity, high Coulombic efficient35 and excellent rate capabilities render HEMM a viable route to laboratory-scale production of Chevrel phases for use as positive electrodes for rechargeable magnesium batteries.

关键词： magnesium battery Chevrel phase high energy mechanicalmilling electrochemical properties

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Electrochemical reactivity of In-Pb solid solution as a negative electrode for rechargeable Mg-ion batteries

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Journal of Energy Chemistry 2021年第4期30卷 124-128页

作者： Lucie Blondeau Suzy Surble Eddy Foy Hicham Khodja Magali Gauthier UniversitéParis-Saclay CEACNRSNIMBELEEL91191Gif-sur-YvetteFrance UniversitéParis-Saclay CEACNRSNIMBELAPA-IRAMAT91191Gif-sur-YvetteFrance

A composite In-Pb:carbon was successfully synthetized by a two-step mechanochemical synthesis in order to obtain an adequate particles size and structure to investigate the electrochemical reactivity of the In-Pb solid solution towards Mg.A potential synergetic coupling of electroactive elements In and Pb was examined using electrochemical and ex situ X-ray diffraction *** potential profile of the solid solution indicates the formation of Mg_(2)Pb and Mg ***,the diffraction study suggests a peculiar electrochemically-driven amorphization of Mg In during the magnesiation,in strong contrast to Mg In crystallization in In-based and In Bi-based electrodes reported in the *** In and Pb favors the amorphization of Mg In and a high first magnesiation capacity of about 550 m Ah g^(-1),but is thereafter detrimental to the material’s *** results emphasize the possible influence of electrochemically-driven amorphization and crystallization processes on electrochemical performance of battery materials.

关键词： magnesium battery Negative electrode Alloy Amorphization

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