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Design strategies for low temperature Aqueous electrolytes

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Nano Research Energy 2022年第1期1卷 78-89页

作者： Liwei Jiang Dejian Dong Yi-Chun Lu Electrochemical Energy and Interfaces Laboratory Department of Mechanical and Automation EngineeringThe Chinese University of Hong KongHong Kong SARChina

Low temperature aqueous batteries(LT-ABs)have attracted extensive attention recent years.The LT-ABs suffer from electrolyte freezing,slow ionic diffusion and sluggish interfacial redox kinetics at low temperature.In this review,we discuss physicochemical properties of Aqueous electrolytes in terms of phase diagram,ion diffusion and interfacial redox kinetics to guide the design of low temperature Aqueous electrolytes(LT-AEs).Firstly,the characteristics of equilibrium and non equilibrium phase diagrams are introduced to analyze the antifreezing mechanisms and propose design strategies for LT-AEs.Then,the temperature/concentration/charge carrier dependence conductivity characteristics in Aqueous electrolytes are reviewed to comprehend and regulate the ion diffusion kinetics.Moreover,we introduce interfacial studies in aqueous and non-aqueous batteries and propose potential improvement strategies for interfacial redox kinetics in LT-ABs.Finally,we summarize design strategies of LT-AEs for developing high performance LT-ABs.

关键词： Aqueous electrolytes low temperature phase diagram ionic diffusion interfacial redox kinetics

Advances in Mn‑Based Electrode Materials for aqueous Sodium‑Ion Batteries

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纳微快报:英文版 2023年第11期15卷 19-60页

作者： Changsheng Ding Zhang Chen Chuanxiang Cao Yu Liu Yanfeng Gao School of Materials Science and Engineering Shanghai UniversityShanghai 200444People’s Republic of China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050People’s Republic of China Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources Qinghai Institute of Salt LakesChinese Academy of SciencesXining 81000People’s Republic of China

aqueous sodium-ion batteries have attracted extensive attention for large-scale energy storage applications,due to abundant sodium resources,low cost,intrinsic safety of Aqueous electrolytes and eco-friendliness.The electrochemical performance of aqueous sodium-ion batteries is affected by the properties of electrode materials and electrolytes.Among various electrode materials,Mn-based electrode materials have attracted tremendous attention because of the abundance of Mn,low cost,nontoxicity,eco-friendliness and interesting electrochemical performance.Aqueous electrolytes having narrow electrochemical window also affect the electrochemical performance of Mn-based electrode materials.In this review,we introduce systematically Mn-based electrode materials for aqueous sodium-ion batteries from cathode and anode materials and offer a comprehensive overview about their recent development.These Mn-based materials include oxides,Prussian blue analogues and polyanion compounds.We summarize and discuss the composition,crystal structure,morphology and electrochemical properties of Mn-based electrode materials.The improvement methods based on electrolyte optimization,element doping or substitution,optimization of morphology and carbon modification are highlighted.The perspectives of Mn-based electrode materials for future studies are also provided.We believe this review is important and helpful to explore and apply Mn-based electrode materials in aqueous sodium-ion batteries.

关键词： Sodium-ion batteries Aqueous electrolytes Mn-based electrode materials Electrochemical performance Improvement methods

Adjusting the local solvation structures and hydrogen bonding networks for stable aqueous batteries with reduced cost

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Journal of Energy Chemistry 2022年第5期31卷 411-419页

作者： Canfu Zhang Binbin Chen Haoran Cai Renzhi Huang Yingchun Liu Huilin Pan Department of Chemistry Zhejiang UniversityHangzhou 310027ZhejiangChina

Exploring low-cost and effective approaches to extend the potentials of Aqueous electrolytes is highly desired.Herein,it is found that the activity of H_(2)O in Aqueous electrolytes could be intensively manipulated by introducing small urea and long-chain polyethylene glycol(PEG)molecules into Li TFSI-H_(2)O electrolyte systems without super salt concentration.The urea and PEG molecules could exclude partial coordinated H_(2)O out of the inner solvation shell of Li_(4) and reconstruct hydrogen-bonding network between H_(2)O and PEG molecules outside the solvation sheaths with restricted H_(2)O activity and extended electrochemical window.The bonding competitions in Aqueous electrolytes and their correlation to the electrochemical performance of full cells are studied.When the occurrence probability of H_(2)O around Li_(4)is lower than 40%,stable cycling of 3.1 V LiMn_(2)O_(4)-Li_(4)Ti_(5)O_(12) full cell is achieved,showing 73%capacity retention after 200 cycles at 1 C rate in optimal electrolytes.This work provides new avenues to understand the role of H_(2)O and explore low-cost and effective approaches for the development of nextgeneration aqueous lithium-ion batteries.

关键词： Solvation sheath H_(2)O activity Aqueous electrolytes Lithium-ion batteries

Direct observation of the CO_(2) formation and C–H consumption of carbon electrode in an aqueous neutral electrolyte supercapacitor by in-situ FTIR and Raman

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Journal of Energy Chemistry 2022年第8期31卷 488-496,I0013页

作者： Murilo M.Amaral Victor Y.Yukuhiro Rafael Vicentini Alfredo C.Peterlevitz Leonardo M.Da Silva Pablo Fernandez Hudson Zanin Advanced Energy Storage Division State University of Campinas13083-852Av.Albert Einsten 400CampinasSPBrazil Chemistry Institute State University of Campinas13083-970Josue de Castro StreetCampinasSPBrazil Department of Chemistry Laboratory of Fundamental and Applied ElectrochemistryFederal University of Jequitinhonha and Mucuri’s ValleyRodovia MGT 367km 5835000Alto da Jacuba39100-000DiamantinaMGBrazil Center for Innovation on New Energies University of Campinas13083-841 CampinasSão PauloBrazil

Electrical double-layer capacitors(EDLCs)consist of energy storage devices that present high-power and moderate energy density.The electrolyte and electrode physicochemical properties are crucial for improving their overall energy storage capabilities.Therefore,the stability of the EDLCs’materials is the primary focus of this study.Since energy storage depends on the specific capacitance,and also on the square of the maximum capacitive cell voltage(UMCV).Thus,electrodes with high specific surface area(SSA)and electrolytes with excellent electrochemical stability are commonly reported in the literature.Aqueous electrolytes are safer and green devices compared to other organic-based solutions.On the other hand,their UMCVis reduced compared to other electrolytes(e.g.,organic-based and ionic liquids).In this sense,spanning the UMCVfor aqueous-based electrolytes is a’hot topic’research.Unfortunately,the lack of protocols to establish reliable UMCVvalues has culminated in the publishing of several conflicting results.Herein,we confirm that multiwalled carbon nanotubes(MWCNTs)housed in cells degrade and produce CO_(2) under abusive polarisation conditions.It is probed by employing electrochemical techniques,in-situ FTIR and in-situ Raman spectroscopies.From these considerations,the current study uses spectro-electrochemical techniques to support the correct determination of the electrode and electrolyte stability conditions as a function of the operating electrochemical parameters.

关键词： Electrode and electrolyte stabilities In-situ FTIR CO_(2)formation Carbon degradation Supercapacitor Aqueous electrolytes Carbon nanotubes

Thermodynamic modeling and phase diagram prediction of salt lake brine systemsⅡ.aqueous Li^(+)-Na^(+)-K^(+)-SO_(4)^(2-) and its subsystems

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Chinese Journal of Chemical Engineering 2021年第6期34卷 134-149页

作者： Huan Zhou Peng Wu Wenxuan Li Xingfan Wang Kuo Zhou Qing Hao College of Chemical Engineering and Materials Science Tianjin Key Laboratory of Brine Resources and Eco-utilizationTianjin University of Science and TechnologyTianjin 300457China College of Marine and Environmental Sciences Tianjin Key Laboratory of Brine Resources and Eco-utilizationTianjin University of Science and TechnologyTianjin 300457China

It is still a challenging task to accurately and temperature-continuously express the thermodynamic properties and phase equilibrium behaviors of the salt-lake brine with multi-component,multitemperature and high concentration.The essential subsystem of sulfate type brine,aqueous Li^(+)-Na^(+)-K^(+)-SO_(4)^(2-) and its subsystems across a temperature range from 250 K to 643 K are investigated with the improved comprehensive thermodynamic model.Liquid parameters(Δg_(IJ),Δh_(IJ),and ΔC_(p,IJ))associated with the contributions of Gibbs energy,enthalpy,and heat capacity to the binary interaction parameters,i.***.the temperature coefficients of eNRTL parameters formulated with a Gibbs Helmholtz expression,are determined via multi-objective optimization method.The solid constantsΔ_(f)G_(k)°^((298.15))andΔ_(f)H_(k)°^((298.15))of11 solid species occurred in the quaternary system are rebuilt from multi-temperature solubilities.The modeling results show the accurate representation of(1)solution properties and binary phase diagram at temperature ranges from eutectic points to 643 K;(2)isothermal phase diagrams for Li_(2)SO_(4)-Na_(2)SO_(4)-H_(2)O,Li_(2)SO_(4)-K_(2)SO_(4)-H_(2)O and Na_(2)SO_(4)-K_(2)SO_(4)-H_(2)O ternary systems.The predicted results of complete structure and polythermal phase diagram of ternary systems and the isothermal phase diagrams of quaternary system excellently match with the experimental data.

关键词： Aqueous electrolytes Comprehensive thermodynamic model aqueous Li^(+)-Na^(+)-K^(+)-SO_(4)^(2-) Phase diagram Thermodynamic properties

Thermodynamic modeling and phase diagram prediction of salt lake brine systems.Ⅰ. aqueous Mg^2+–Ca^2+–Cl^- binary and ternary systems

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Chinese Journal of Chemical Engineering 2020年第9期28卷 2391-2408页

作者： Huan Zhou Xiaolong Gu Yaping Dai Jingjing Tang Jian Guo Guangbi Li Xiaoqin Bai College of Chemical Engineering and Materials Science Tianjin Key Laboratory of Marine Resources and ChemistryTianjin University of Science and TechnologyTianjin 300457China

Salt lake brine is a complex salt-water system under natural environment.Although many models can express the thermodynamic properties and phase equilibrium of electrolyte aqueous solution,the multi-temperature characteristics and predictability are still the goals of model development.In this study,a comprehensive thermodynamic model system is re-established based on the eNRTL model and some improvements:(1) new expression of long-range electrostatic term with symmetrical reference state is proposed to handle the electrolyte solution covering entire concentration range;(2) the temperature dependence of the binary interaction parameters is formulated with a Gibbs Helmholtz expression containing three temperature coefficients,the liquid parameters,which associated with Gibbs energy,enthalpy,and heat capacity contribution;and(3) liquid parameters and solid species data are regressed from properties and solubility data at full temperature range.Together the activity coefficient model,property models and parameters of liquid and solid offer a comprehensive thermodynamic model system for the typical bittern of MgCl2-CaCl2-H2 O binary and ternary systems,and it shows excellent agreement with the literature data for the ternary and binary systems.The successful prediction of complete phase diagram of ternary system shows that the model has the ability to deal with high concentration and high non-idealitv system,and the ability to extrapolate the temperature.

关键词： Aqueous electrolytes Comprehensive thermodynamic model MgCl2-CaCl2-H2O Phase diagram Thermodynamic properties

Electrolyte Solvation Structure Design for High Voltage Zinc-Based Hybrid Batteries

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Energy & Environmental Materials 2023年第4期6卷 239-247页

作者： Pauline Jaumaux Shijian Wang Shuoqing Zhao Bing Sun Guoxiu Wang Centre for Clean Energy Technology School of Mathematical and Physical SciencesFaculty of ScienceUniversity of Technology SydneyUltimo NSW 2007Australia

Zinc(Zn)metal anodes have enticed substantial curiosity for large-scale energy storage owing to inherent safety,high specific and volumetric energy capacities of Zn metal anodes.However,the aqueous electrolyte traditionally employed in Zn batteries suffers severe decomposition due to the narrow voltage stability window.Herein,we introduce N-methylformamide(NMF)as an organic solvent and modulate the solvation structure to obtain a stable organic/aqueous hybrid electrolyte for high-voltage Zn batteries.NMF is not only extremely stable against Zn metal anodes but also reduces the free water molecule availability by creating numerous hydrogen bonds,thereby accommodating high-voltage Zn‖LiMn_(2)O_(4)batteries.The introduction of NMF prevented hydrogen evolution reaction and promoted the creation of an Frich solid electrolyte interphase,which in turn hampered dendrite growth on Zn anodes.The Zn‖LiMn_(2)O_(4)full cells delivered a high average Coulombic efficiency of 99.7%over 400 cycles.

关键词： Aqueous electrolytes electrolyte solvation structures high-voltage zinc batteries hybrid batteries

Towards high power density aqueous redox flow batteries

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Nano Research Energy 2023年第1期2卷 71-87页

作者： Mengqi Gao Zhiyu Wang Dao Gen Lek Qing Wang Department of Materials Science and Engineering College of Design and EngineeringNational University of Singapore117574Singapore Institute of Materials Research and Engineering(IMRE) Agency for Science Technology and Research(A*STAR)138632Singapore

With the increasing penetration of renewable energy sources in the past decades,stationary energy storage technologies are critically desired for storing electricity generated by non-dispatchable energy sources to mitigate its impact on power grids.Redox flow batteries(RFBs)stand out among these technologies due to their salient features for large-scale energy storage.The primary obstacle to the successful industrialization and broad deployment of RFBs is now their high capital costs.A feasible route to cost reduction is to develop high-power RFBs,since the increase in power performance has a pronounced impact on the cost of RFB systems.In this review,an in-depth inspection of the power performance of RFBs is presented.Perspectives for the future development of high-power RFBs along with implementable strategies addressing both the intrinsic and extrinsic limiting factors are summarized,which are expected to provide useful references steering the further improvement in the power density of RFBs.

关键词： redox flow batteries power density Aqueous electrolytes redox kinetics polarizations