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“In-N-out” design enabling high-content triethyl phosphate-based non-flammable and high-conductivity electrolytes for lithium-ion batteries

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Science China Chemistry 2024年第2期67卷 724-731页

作者： Mengchuang Liu Fenfen Ma Zicheng Ge Ziqi Zeng Qiang Wu Hui Yan Yuanke Wu Sheng Lei Yanli Zhu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan430074China GuSu Laboratory of Materials Suzhou215123China Institute of Metal Research Chinese Academy of SciencesShenyang110000China State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China

Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended *** use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of ***,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content *** mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate *** a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.

关键词： lithium-ion batteries graphite anode high-phosphate-content electrolytes non-flammable electrolyte excellent ion conductivity standard concentration

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Multi-core-shell-structured LiFePO_(4)@Na_(3)V_(2)(PO_(4))_(3)@C composite for enhanced low-temperature performance of lithium-ion batteries

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Rare Metals 2021年第4期40卷 828-836页

作者： Xing-Xing Gu Shuang Qiao Xiao-Lei Ren Xing-Yan Liu You-Zhou He Xiao-Teng Liu Tie-Feng Liu Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and ResourcesChongqing Technology and Business UniversityChongqing 400067China Faculty of Engineering and Environment Northumbria UniversityNewcastle upon Tyne NE18STUK GRINM Group Co. Ltd.Beijing 100088China College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China

In this work,a multi-core-shell-structured LiFePO_(4)@Na_(3) V_(2)(PO_(4))_(3)@C(LFP@NVP@C) composite was successfully designed and prepared to address inferior low-temperature performance of LiFePO_(4) cathode for lithium-ion *** electron microscopy(TEM) confirms the inner NVP and outer carbon layers coexisted on the surface of LFP *** evaluated at low-temperature operation,LFP@NVP@C composite exhibits an evidently enhanced electrochemical performance in term of higher capacity and lower polarization,compared with LFP@*** at-10℃ with 0.5 C,LFP@NVP@C delivers a discharge capacity of ca.96.9 mAh-g^(-1) and discharge voltage of ca.3.3 V,which is attributed to the beneficial contribution of NVP *** ICON-structured NVP with an open framework for readily insertion/desertion of Li+ will effectively reduce the polarization for the electrochemical reactions of the designed LFP@NVP@C composite.

关键词： LiFePO_(4)@Na_(3)V_(2)(PO_(4))_(3)@C composite Multi-core-shell Low-temperature lithium-ion batteries

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Li4SiO4-coated LiNi0.5Mn1.5O4 as the high performance cathode materials for lithium-ion batteries

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Frontiers in Energy 2017年第3期11卷 374-382页

作者： Shifeng YANG Wenfeng REN Jian CHEN Advanced Rechargeable Battery Laboratory Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 University of Chinese Academy of Sciences Beijing 100049 China Advanced Rechargeable Battery Laboratory Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China

The preparation of Li4SiO4-coated LiNi0.5Mn1.5O4 materials by sintering the SiO2-coated nickel-manganese oxides with lithium salts using abundant and low-cost sodium silicate as the silicon source was reported. The samples were characterized by X-ray diffraction, scanning electron microscopy and transmission electron microscopy. It was found that a uniform and complete SiO2 coating layer could be obtained at a suitable pH value of 10, which transformed to a good LiaSiO4 coating layer afterwards. When used as the cathode materials for lithium-ion batteries, the Li4SiO4-coated LiNi0.5Mn1.5O4 samples deliver a better electrochemical performance in terms of the discharge capacity, rate capability, and cycling stability than that of the pristine material. It can still deliver 111.1 mAh/g at 20 C after 300 cycles, with a retention ratio of 93.1% of the stable capacity, which is far beyond that of the pristine material （101.3 mAh/g, 85.6%）.

关键词： lithium-ion batteries cathode material LiNi0.5Mn1.5O4 lithium-ion conductor coating

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Constructing the bonding between conductive agents and active materials/binders stabilizes silicon anode in lithium-ion batteries

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Journal of Energy Chemistry 2023年第5期80卷 23-31,I0002页

作者： Jie Tang Jiawang Zhou Xingyu Duan Yujie Yang Xinyi Dai Fuzhong Wu Guizhou High-level Institution Key Laboratory of High-Performance Battery Materials Guizhou UniversityGuiyang 550025GuizhouChina

Silicon(Si)anode has been considered a promising candidate due to its remarkable theoretical capacity but it was plagued by severe pulverization because of the inherent huge volume *** electrode stability is an effective approach to improve electrochemical ***,a stable Si anode was established by an innovative construction of the bonding between conductive agents and active materials/*** a result,the strong interaction of electrode components not only effectively alleviates the volume expansion of Si but also achieves a stable interface by generating the beneficial solid electrolyte interphase(SEI)*** to the deliberate scheme of the electrode,the Si anode exhibits sterling electrochemical ***,the device of the electrode is not only effective for other binders but also for other anode materials with high volume variation,thus shedding light on the rational design of electrodes for high-energy-density lithium-ion batteries.

关键词： lithium-ion batteries Si MXene SEI Structural stability

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lithium-ion insertion kinetics of Na-doped Li2TiSiO5 as anode materials for lithium-ion batteries

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Journal of Materials Science & Technology 2020年第22期54卷 18-25页

作者： Yueni Mei Yuyu Li Fuyun Li Yaqian Li Yingjun Jiang Xiwei Lan Songtao Guo Xianluo Hu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Li2TiSiO5 receives much interest recently in lithium-ion battery anodes because of its attractive Liinsertion/extraction potential at 0.28 V(vs. Li+/Li), which bridges the potential gap between graphite and Li4 Ti5 O12. However, Li2TiSiO5 suffers from the low intrinsic electronic conductivity and sluggish Liion transfer kinetics. In this work, we report lithium-ion insertion kinetics of Li2TiSiO5 by Na doping,achieving high-rate capability. Rietveld refinement of X-ray diffraction results reveals that Na doping can enlarge the space of Li slabs, thus reducing the Li-ion transfer barrier and enhancing the Li-ion diffusion kinetics. According to first-principles calculations, Na doping can tune the band structure of Li2TiSiO5 from indirect to direct band, leading to improved electronic conductivity and electrochemical performance. In particular, the Na-doped Li2TiSiO5(Li1.95 Na(0.05)TiSiO5) electrode exhibits outstanding rate capability with a high capacity of 101 m A h g^(-1) at 5 A g^(-1) and superior cyclability with a reversible capacity of 137 m A h g^(-1) under 0.5 A g^(-1) over 150 cycles.

关键词： lithium-ion batteries Li2TiSiO5 Anode lithium-ion diffusion Na doping

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Controllable construction of La_(2)Li_(0.5)Co_(0.5)O_(4)multifunctional“armor”to stabilize Li-rich layered oxide cathode for highperformance lithium-ion batteries

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Nano Research 2023年第7期16卷 10634-10643页

作者： Xiaoyang Deng Mi Li Zizai Ma Xiaoguang Wang Institute of New Carbon Materials College of Materials Science and EngineeringTaiyuan University of TechnologyTaiyuan 030024China Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan 030024China College of Chemistry Taiyuan University of TechnologyTaiyuan 030024China

lithium-rich manganese-based cathodes(LR)are valuable cathode materials for the next generation of lithium-ion batteries(LIBs)with high-energy ***,the fast voltage/capacity decay on cycling is the major obstacle for the practical application induced by the less-than-ideal anionic redox reactions and structure ***,in order to tackle these challenges,a perovskite-like La_(2)Li_(0.5)Co_(0.5)O_(4)(LLCO)material is selected as protective surface to stabilize the Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2)(LR)substrate through wet chemical coating *** structure/phase characterizations and electrochemical tests exhibit that the LLCO can not only minish the oxygen evolution and enhance the structure stability,but also restrain the electrolyte corrosion and increase the mechanical strength of cathode ***,the coated LLCO with high electronic/ionic conductivity dramatically accelerates the energy storage kinetic,thereby displaying the improved rate ***,the optimized LR@LLCO sample(1LLCO)exhibits a high capacity of 250.6 mAh·g^(-1)after 100 cycles at 0.1 C and excellent capacity retention of 82.6%after 200 cycles at 2 *** work provides a new idea for the modification of LR cathodes toward commercial high-performance LIBs.

关键词： lithium-rich manganese-based oxide lithium-ion batteries surface modification electrochemical performance

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High-Safety Anode Materials for Advanced lithium-ion batteries

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Energy & Environmental Materials 2024年第5期7卷 1-19页

作者： Kai Yuan Yu Lin Xiang Li Yufeng Ding Peng Yu Jian Peng Jiazhao Wang HuaKun Liu Shixue Dou Wuhan Institute of Marine Electric Propulsion Wuhan 430000China State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongInnovation CampusSquires WayNorth WollongongNew South Wales 2522Australia Institute of Energy Materials Science(IEMS) University of Shanghai for Science and TechnologyShanghai 200093China

lithium-ion batteries(LIBs)play a pivotal role in today's society,with widespread applications in portable electronics,electric vehicles,and smart *** LIBs predominantly utilize graphite anodes due to their high energy density and *** anodes face challenges,however,in extreme safety-demanding situations,such as airplanes and passenger *** lithiation of graphite can potentially form lithium dendrites at low temperatures,causing short ***,the dissolution of the solid-electrolyte-interphase on graphite surfaces at high temperatures can lead to intense reactions with the electrolyte,initiating thermal *** review introduces two promising high-safety anode materials,Li_(4)Ti_(5)O_(12)and TiNb_(2)O_(7).Both materials exhibit low tendencies towards lithium dendrite formation and have high onset temperatures for reactions with the electrolyte,resulting in reduced heat generation and significantly lower probabilities of thermal ***_(4)Ti_(5)O_(12)and TiNb_(2)O_(7)offer enhanced safety characteristics compared to graphite,making them suitable for applications with stringent safety *** review provides a comprehensive overview of Li_(4)Ti_(5)O_(12)and TiNb_(2)O_(7),focusing on their material properties and practical *** aims to contribute to the understanding and development of high-safety anode materials for advanced LIBs,addressing the challenges and opportunities associated with their implementation in real-world applications.

关键词： anodes electrode materials lithium-ion batteries thermal runaway

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A review on the critical challenges and progress of SiO_(x)-based anodes for lithium-ion batteries

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International Journal of Minerals,Metallurgy and Materials 2022年第4期29卷 876-895页

作者： Nana Yao Yu Zhang Xianhui Rao Zhao Yang Kun Zheng KonradŚwierczek Hailei Zhao School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083China Faculty of Energy and Fuels AGH University of Science and Technologyal.A.Mickiewicza 30Krakow30-059Poland Beijing Key Lab of New Energy Materials and Technology Beijing 100083China

With the advantages of abundant resources,high specific capacity,and relatively stable cycling performance,silicon suboxides(SiO_(x) ,x<2)have been recently suggested as promising anodes for next-generation lithium-io... 详细信息

With the advantages of abundant resources,high specific capacity,and relatively stable cycling performance,silicon suboxides(SiO_(x) ,xion lithium-ion batteries(LIBs).SiO_(x) exhibits superior storage capability because of the presence of silicon and smaller volume change upon charge/discharge than Si owing to the buffering effect of the initial lithiation products of inert lithium oxide and lithium silicates,enabling a stable cycle life of ***,significant improvements such as overcoming issues related to volume changes in cycling and initial irreversible capacity loss and enhancing the ionic and electronic charge transport in poorly conducting SiO_(x) electrodes,are still needed to achieve the satisfactory performance required for commercial *** review summarizes recent progress on the cycling performance and initial coulombic efficiency of SiO_(x) .Advances in the design of particle morphology and composite composition,prelithiation and prereduction methods,and usage of electrolyte additives and optimized electrode binders are *** on the promising research directions that might lead to further improvement of the electrochemical properties of SiO_(x) -based anodes are *** paper can serve as a basis for the research and development of high-energy-density LIBs.

关键词： silicon suboxides preparation structural optimization anode lithium-ion batteries

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Enhancing electrochemical capacity and interfacial stability of lithium-ion batteries through side reaction modulation with ultrathin carbon nanotube film and optimized lithium cobalt oxide particle size

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Nano Research 2024年第8期17卷 7230-7241页

作者： Wei Xi Xiaogang Xia Jiacheng Zhu Dehua Yang Sishen Xie Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Advanced Passivation Technology Lab College of Physics Science and TechnologyHebei UniversityBaoding 071002China

lithium cobalt oxide(LCO),the first commercialized cathode active material for lithium-ion batteries,is known for high voltage and ***,its application has been limited by relatively low capacity and stability at high *** particle size is considered one of the most straightforward and effective strategies to enhance ion transfer,thus increasing the rate ***,side reactions are simultaneously enhanced as the specific surface area ***,we investigate the impact of LCO particles with varying size distributions and optimize the particle *** modulate the side reactions associated with particle size reduction,an ultrathin carbon nanotube film(UCNF)is introduced to coat the cathode *** this simple process and optimized particle size,the rate performance improves significantly,normal commercial LCO achieves 118 mA·h·g^(−1)at 3.0–4.3 V and 20 C(0.72 mA·h·cm^(−2)),corresponding to power density of 8732 W·kg^(−1).This method is applied to high voltage as well,152 mA·h·g^(−1)at 3.0–4.6 V and 20 C(0.99 mA·h·cm^(−2))was achieved with high-voltage LCO(HVLCO),corresponding to power density of 11,552 W·kg^(−1).The cycling stability is also enhanced,with the capacity retention maintaining more than 96%after 100 cycles at 0.1 *** the first time,UCNF is demonstrated to suppress the excessive decomposition of the electrolytes and solvents by blocking electron injection/extraction between LCO and electrolyte *** findings provide a simple method for improving LCO rate performance,especially at high C-rates.

关键词： lithium-ion batteries lithium cobalt oxides carbon nanomaterials side reactions

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A novel order-reduced thermal-coupling electrochemical model for lithium-ion batteries

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Chinese Physics B 2024年第5期33卷 637-654页

作者：谢奕展王舒慧王震坡程夕明 School of Mechanical Engineering Beijing Institute of TechnologyBeijing 100081China National Engineering Research Center for Electric Vehicles Beijing Institute of TechnologyBeijing 100081China The Hong Kong University of Science and Technology (Guangzhou) Sustainable Energy and Environment Thrust and Guangzhou MunicipalKey Laboratory of Materials InformaticsGuangzhou 511400China

Although the single-particle model enhanced with electrolyte dynamics(SPMe)is simplified from the pseudo-twodimensional(P2D)electrochemical model for lithium-ion batteries,it is difficult to solve the partial differential equations of solid–liquid phases in real-time ***,working temperatures have a heavy impact on the battery ***,a thermal-coupling SPMe is ***,a lumped thermal model is established to estimate battery *** order of the SPMe model is reduced by using both transfer functions and truncation techniques and merged with Arrhenius equations for thermal *** polarization voltage drop is then modified through the use of test data because its original model is unreliable ***,the coupling-model parameters are extracted using genetic *** results demonstrate that the proposed model produces average errors of about 42 mV under 15 constant current conditions and 15 mV under nine dynamic conditions,*** new electrochemicalthermal coupling model is reliable and expected to be used for onboard applications.

关键词： lithium-ion batteries order-reduced electrochemical models SPMe thermal-coupling model transient polarization voltage drop

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