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A three-way electrolyte with ternary solvents for high-energy-density and long-cycling lithium-sulfur pouch cells

SusMat 2024年第2期4卷 1-12页

作者： Zheng Li Legeng Yu Chen-Xi Bi Xi-Yao Li JinMa Xiang Chen Xue-Qiang Zhang Aibing Chen Haoting Chen Zuoru Zhang Li-Zhen Fan Bo-Quan Li Cheng Tang Qiang Zhang Tsinghua Center for Green Chemical Engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyDepartment of Chemical EngineeringTsinghua UniversityBeijingChina School of Materials Science and Engineering Beijing Institute of TechnologyBeijingChina Institute of Advanced Materials and Technology University of Science and TechnologyBeijingChina Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuanChina Center for Next-Generation Energy Materials and School of Chemical Engineering Sungkyunkwan UniversityJangan-GuSuwon-SiGyeonggi-DoRepublic of Korea College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangChina Ordos Carbon Neutral Research and Application Co. Ltd.Kangbashi DistrictOrdos CityInner MongoliaChina Institute for Carbon Neutrality Tsinghua UniversityBeijingChina

Lithium–sulfur(Li–S)batteries promise high-energy-density potential to exceed the commercialized lithiumion batteries but suffer from limited cycling lifespan due to the side reactions between lithium polysulfides(LiPSs)and Li metal ***,a three-way electrolyte with ternary solvents is proposed to enable high-energy-density and long-cycling Li–S pouch ***,ternary solvents composed of 1,2-dimethoxyethane,di-isopropyl sulfide,and 1,3,5-trioxane are employed to guarantee smooth cathode kinetics,inhibit the parasitic reactions,and construct a robust solid electrolyte interphase,*** cycling lifespan of Li–S coin cells with 50μm Li anodes and 4.0 mg cm^(−2) sulfur cathodes is prolonged from88 to 222 cycles using the three-way ***-heterogeneous solvation structure of LiPSs and organic-rich solid electrolyte interphase are identified to improve the cycling stability of Li metal ***,a 3.0 Ah-level Li–S pouch cell with the three-way electrolyte realizes a high energy density of 405 Wh kg^(−1) and undergoes 27 *** affords a three-way electrolyte recipe for suppressing the side reactions of LiPSs and inspires rational electrolyte design for practical high-energy-density and long-cycling Li–S batteries.

关键词： lithium metal anodes lithium-sulfur batteries pouch cells solid electrolyte interphase three-way electrolyte

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Leap of Li Metal Anodes from Coin cells to pouch cells:Challenges and Progress

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Electrochemical Energy Reviews 2023年第1期6卷 39-86页

作者： Qian Wang Tiantian Lu Yuanbin Xiao Jianyang Wu Lixiang Guan Lifeng Hou Huayun Du Huan Wei Xiaoda Liu Chengkai Yang Yinghui Wei Henghui Zhou Yan Yu College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina Corrosion and Protection Engineering Technology Research Center of Shanxi Province Taiyuan 030024ShanxiChina Key Laboratory of Advanced Materials Technology College of Materials Science and EngineeringFuzhou UniversityFuzhou 350108FujianChina College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China

Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical ***,until now,there has only been limited success in improving the interfacial and structural stabilities and in realizing the highly controllable and large-scale fabrication of this emerging material;these limitations have posed great obstacles to further performing fundamental and applied studies in Li metal *** this review,we focus on summarizing the existing challenges of Li metal anodes based on the leap from coin cells to pouch cells and on outlining typical methods for designing Li metal anodes on demand;we controllably engineer their surface protection layers and structure sizes by encapsulating structured Li metal inside a variety of synthetic protection *** aim to provide a comprehensive understanding and serve as a strategic guide for designing and fabricating practicable Li metal anodes for use in pouch *** and opportunities regarding this burgeoning field are critically evaluated at the end of this review.

关键词： Li metal anode Dendrites pouch cells Air stability Energy density

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Unraveling high efficiency multi-step sodium storage and bidirectional redox kinetics synergy mechanism of cobalt-doping vanadium disulfide anode

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Journal of Energy Chemistry 2024年第7期94卷 148-157页

作者： Enzhi Li Mingshan Wang Yuanlong Feng Lin Yang Qian Li Zhenliang Yang Junchen Chen Bo Yu Bingshu Guo Zhiyuan Ma Yun Huang Jiangtao Liu Xing Li School of New Energy and Materials Southwest Petroleum UniversityChengdu 610500SichuanChina Institute of Materials China Academy of Engineering PhysicsMianyang 621908SichuanChina State Key Laboratory of Advanced Chemical Power Sources Guizhou Meiling Power Sources Co.Ltd.Zunyi 563003GuizhouChina school of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangChina

Sodium-based storage devices based on conversion-type metal sulfide anodes have attracted great atten-tion due to their multivalent ion redox reaction ***,they also suffer from sodium polysul-fides(NaPSs)shuttling problems during the sluggish Na^(+) redox process,leading to"voltage failure"and rapid capacity ***,a metal cobalt-doping vanadium disulfide(Co-VS_(2))is proposed to simulta-neously accelerate the electrochemical reaction of VS_(2) and enhance the bidirectional redox of soluble *** is found that the strong adsorption of NaPSs by V-Co alloy nanoparticles formed in situ during the conversion reaction of Co-VS_(2) can effectively inhibit the dissolution and shuttle of NaPSs,and ther-modynamically reduce the formation energy barrier of the reaction path to effectively drive the complete conversion reaction,while the metal transition of Co elements enhances reconversion kinetics to achieve high ***,Co-VS_(2) also produce abundant sulfur vacancies and unsaturated sulfur edge defects,significantly improve ionic/electron diffusion ***,the Co-VS_(2) anode exhibits ultrahigh rate capability(562 mA h g^(-1) at 5 A g^(-1)),high initial coulombic efficiency(~90%)and 12,000 ultralong cycle life with capacity retention of 90%in sodium-ion batteries(SIBs),as well as impressive energy/power density(118 Wh kg^(-1)/31,250 W kg^(-1))and over 10.000 stable cycles in sodium-ion hybrid capacitors(SIHCs).Moreover,the pouch cell-type SIHC displays a high-energy density of 102 Wh kg^(-1) and exceed 600 stable *** work deepens the understanding of the electrochemical reaction mechanism of conversion-type metal sulfide anodes and provides a valuable solution to the shuttlingofNaPSs inSIBsandSIHCs.

关键词： Sodium-ionbatteries Sodium-ion hybrid capacitors pouch cells Vanadium disulfide Shuttle effect

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Revealing the Multifunctional Electrocatalysis of Indium-Modulated Phthalocyanine for High-Performance Lithium-Sulfur Batteries

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Energy & Environmental Materials 2024年第1期7卷 1-8页

作者： Yang Guo Zhaoqing Jin Jianhao Lu Zilong Wang Zihao Song Anbang Wang Weikun Wang Yaqin Huang Beijing Key Laboratory of Electrochemical Process and Technology for Materials Key Laboratory of Biomedical Materials of Natural MacromoleculesMinistry of EducationBeijing University of Chemical TechnologyBeijing 100029China Research Institute of Chemical Defense Beijing Key Laboratory of Advanced Chemical Energy Storage Technology and MaterialsBeijing 100191China

The sluggish kinetics of complicated multiphase conversions and the severe shuttling effect of lithium polysulfides(LiPSs)significantly hinder the applications of Li-S battery,which is one of the most promising candidates for the next-generation energy storage ***,a bifunctional electrocatalyst,indium phthalocyanine self-assembled with carbon nanotubes(InPc@CNT)composite material,is proposed to promote the conversion kinetics of both reduction and oxidation processes,demonstrating a bidirectional catalytic effect on both nucleation and dissolution of Li_(2)S *** theoretical calculation shows that the unique electronic configuration of InPc@CNT is conducive to trapping soluble polysulfides in the reduction process,as well as the modulation of electron transfer dynamics also endows the dissolution of Li_(2)S in the oxidation reaction,which will accelerate the effectiveness of catalytic conversion and facilitate sulfur ***,the InPc@CNT modified separator displays lower overpotential for polysulfide transformation,alleviating polarization of electrode during *** integrated spectroscopy analysis,HRTEM,and electrochemical study reveal that the InPc@CNT acts as an efficient multifunctional catalytic center to satisfy the requirements of accelerating charging and discharging ***,the Li-S battery with InPc@CNT-modified separator obtains a discharge-specific capacity of 1415 mAh g^(-1)at a high rate of 0.5 ***,the 2 Ah Li-S pouch cells deliver 315 Wh kg^(-1)and achieved 80%capacity retention after 50 cycles at 0.1 C with a high sulfur loading of 10 mg cm^(-2).Our study provides a practical method to introduce bifunctional electrocatalysts for boosting the electrochemical properties of Li-S batteries.

关键词： bidirectional catalyst indium phthalocyanine lithium-sulfur batteries pouch cells

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Post lithium-sulfur battery era:challenges and opportunities towards practical application

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Science China Chemistry 2024年第1期67卷 106-121页

作者： Jiahang Chen Yang Zhang Jun Yang Yanna Nuli Jiulin Wang State Key Laboratory of Chemistry and Utilization of Carbon-Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China Department of Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Lithium-sulfur(Li-S)batteries have been regarded as a promising next-generation energy storage system owing to the high theoretical energy density and natural abundance of *** fundamental researches have pushed the flourishing development on electrochemical behaviors in recent 20 *** is time to evolve into post-Li-S battery era with the pursuit towards practical *** the landmark leap,numerous new challenges appear under harsh conditions,such as high sulfur loading,low cathode density,lean electrolyte and limited lithium ***,we summarize the considerable parameters of pouch Li-S cells and review the pioneering studies focused on the cathode structure,conversion kinetics,electrode interphase and battery *** interwoven relationship of these key points is concluded and discussed,which provides guidance to future researches aiming to safe and long-lifespan Li-S batteries with high energy density.

关键词： lithium-sulfur batteries practical application harsh conditions energy density pouch cells

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12.6μm-Thick Asymmetric Composite Electrolyte with Superior Interfacial Stability for Solid-State Lithium-Metal Batteries

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Nano-Micro Letters 2024年第9期16卷 397-409页

作者： Zheng Zhang Jingren Gou Kaixuan Cui Xin Zhang Yujian Yao Suqing Wang Haihui Wang Beijing Key Laboratory for Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510000People’s Republic of China

Solid-state lithium metal batteries(SSLMBs)show great promise in terms of high-energy-density and high-safety ***,there is an urgent need to address the compatibility of electrolytes with high-voltage cathodes/Li anodes,and to minimize the electrolyte thickness to achieve highenergy-density of ***,we develop an ultrathin(12.6μm)asymmetric composite solid-state electrolyte with ultralight areal density(1.69 mg cm^(−2))for *** electrolyte combining a garnet(LLZO)layer and a metal organic framework(MOF)layer,which are fabricated on both sides of the polyethylene(PE)separator separately by tape *** PE separator endows the electrolyte with flexibility and excellent mechanical *** LLZO layer on the cathode side ensures high chemical stability at high *** MOF layer on the anode side achieves a stable electric field and uniform Li flux,thus promoting uniform Li^(+)*** to the well-designed structure,the Li symmetric battery exhibits an ultralong cycle life(5000 h),and high-voltage SSLMBs achieve stable cycle *** assembled pouch cells provided a gravimetric/volume energy density of 344.0 Wh kg^(−1)/773.1 Wh L^(−1).This simple operation allows for large-scale preparation,and the design concept of ultrathin asymmetric structure also reveals the future development direction of SSLMBs.

关键词： Solid-state lithium metal batteries Composite solid-state electrolyte Ultrathin asymmetric structure pouch cells

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Dynamic Multi-Physics Behaviors and Performance Loss of Cylindrical Batteries Upon Low-Velocity Impact Loading

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ENERGY & ENVIRONMENTAL MATERIALS 2024年第6期7卷 184-192页

作者： Huang, Qingdan Bai, Yang Luo, Han Jia, Yikai Zhang, Chao Northwestern Polytech Univ Sch Civil Aviat Xian 710072 Peoples R China Key Lab Impact Protect & Safety Assessment Civil A Taicang 215400 Peoples R China Northwestern Polytech Univ Sch Aeronaut Xian 710072 Peoples R China EVE Energy Co Ltd Huizhou 516006 Peoples R China

In challenging operational environments, Lithium-ion batteries (LIBs) inevitably experience mechanical stresses, including impacts and extrusion, which can lead to battery damage, failure, and even the occurrence of fire and explosion incidents. Consequently, it is imperative to investigate the safety performance of LIBs under mechanical loads. This study is grounded in a more realistic coupling scenario consisting of electrochemical cycling and low-velocity impact. We systematically and experimentally uncovered the mechanical, electrochemical, and thermal responses, damage behavior, and corresponding mechanisms under various conditions. Our study demonstrates that higher impact energy results in increased structural stiffness, maximum temperature, and maximum voltage drop. Furthermore, heightened impact energy significantly influences the electrical resistance parameters within the internal resistance. We also examined the effects of State of Charge (SOC) and C-rates. The methodology and experimental findings will offer insights for enhancing the safety design, conducting risk assessments, and enabling the cascading utilization of energy storage systems based on LIBs. In this study, the impact of low-velocity impacts on the performance and safety of LIBs is explored. Various conditions, such as impact energy, State of Charge (SOC), and C-rates, systematically reveal mechanical, electrochemical, and thermal responses, as well as damage behaviors. The study demonstrates that higher energy leads to increased structural stiffness, maximum temperature, and maximum voltage drop. Additionally, heightened impact energy and SOC significantly influence electrochemical parameters, including charging capacity and internal resistance. image

关键词： cycling performance damaged battery lithium-ion battery low-velocity impact mechanical safety LITHIUM-ION BATTERY SHORT-CIRCUIT MECHANICAL-BEHAVIOR pouch cells COMPUTATIONAL MODEL ELECTRIC VEHICLES THERMAL-BEHAVIOR STRAIN-RATE DEFORMATION OVERCHARGE

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Boosting High-Voltage Practical Lithium Metal Batteries with Tailored Additives

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Nano-Micro Letters 2024年第12期16卷 23-41页

作者： Jinhai You Qiong Wang Runhong Wei Li Deng Yiyang Hu Li Niu Jingkai Wang Xiaomei Zheng Junwei Li Yao Zhou Jun-Tao Li College of Energy Xiamen UniversityXiamen 361005People’s Republic of China Magnetism Key Laboratory of Zhejiang Province College of Materials and ChemistryChina Jiliang UniversityHangzhou 310018People’s Republic of China Laboratory for Soft Matter and Biophysics Department of Physics and AstronomyKU Leuven3001 LeuvenBelgium State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China Department of Chemical Engineering KU LeuvenCelestijnenlaan 200F3001 LeuvenBelgium College of Chemistry and Chemical Engineering Northwest Normal UniversityLanzhou 730070GansuPeople’s Republic of China

The lithium(Li)metal anode is widely regarded as an ideal anode material for high-energy-density ***,uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency(CE),limiting its broader ***,an ether-based electrolyte(termed FGN-182)is formulated,exhibiting ultra-stable Li metal anodes through the incorporation of LiFSI and LiNO3 as dual *** synergistic effect of the dual salts facilitates the formation of a highly robust SEI film with fast Li+transport ***,Li||Cu half cells exhibit an average CE reaching up to 99.56%.In particular,pouch cells equipped with high-loading lithium cobalt oxide(LCO,3 mAh cm^(-2))cathodes,ultrathin Li chips(25μm),and lean electrolytes(5 g Ah-1)demonstrate outstanding cycling performance,retaining 80%capacity after 125 *** address the gas issue in the cathode under high voltage,cathode additives 1,3,6-tricyanohexane is incorporated with FGN-182;the resulting high-voltage LCO||Li(4.4 V)pouch cells can cycle steadily over 93 *** study demonstrates that,even with the use of ether-based electrolytes,it is possible to simultaneously achieve significant improvements in both high Li utilization and electrolyte tolerance to high voltage by exploring appropriate functional additives for both the cathode and anode.

关键词： Li metal anode Li dendrites LiNO_(3) 1,3,6-tricyanohexane pouch cells

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High-performance localized high-concentration electrolytes by diluent design for long-cycling lithium metal batteries

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Chinese Chemical Letters 2024年第4期35卷 244-247页

作者： Zhe Wang Li-Peng Hou Qian-Kui Zhang Nan Yao Aibing Chen Jia-Qi Huang Xue-Qiang Zhang College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China

Electrolyte design is essential for stabilizing lithium metal anodes and localized high-concentration electrolyte(LHCE) is a promising one. However, the state-of-the-art LHCE remains insufficient to ensure long-cycling lithium metal anodes. Herein, regulating the solvation structure of lithium ions in LHCE by weakening the solvating power of diluents is proposed for improving LHCE performance. A diluent,1,1,2,2,3,3,4,4-octafluoro-5-(1,1,2,2-tetrafluoroethoxy) pentane(OFE), with weaker solvating power is introduced to increase the proportion of aggregates(an anion interacts with more than two lithium ions,AGG-n) in electrolyte compared with the commonly used 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether(TTE). The decomposition of AGG-n in OFE-based LHCE intensifies the formation of anion-derived solid electrolyte interphase and improves the uniformity of lithium deposition. Lithium metal batteries with OFE-based LHCE deliver a superior lifespan of 190 cycles compared with 90 cycles of TTE-based LHCE under demanding conditions. Furthermore, a pouch cell with OFE-based LHCE delivers a specific energy of 417 Wh/kg and undergoes 49 cycles. This work provides guidance for designing high-performance electrolytes for lithium metal batteries.

关键词： Lithium metal anodes Electrolyte Diluents Solid electrolyte interphase pouch cells

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Highly soluble organic nitrate additives for practical lithium metal batteries

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Carbon Energy 2023年第1期5卷 16-24页

作者： Zhe Wang Li-Peng Hou Zheng Li Jia-Lin Liang Ming-Yue Zhou Chen-Zi Zhao Xiaoyuan Zeng Bo-Quan Li Aibing Chen Xue-Qiang Zhang Peng Dong Yingjie Zhang Jia-Qi Huang Qiang Zhang Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijingPR China College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangPR China School of Materials Science and Engineering Beijing Institute of TechnologyBeijingPR China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijingPR China National and Local Joint Engineering Laboratory for Lithium-Ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunmingPR China

The stability of lithium metal anodes essentially dictates the lifespan of high-energy-density lithium metal *** nitrate(LiNO_(3))is widely recognized as an effective additive to stabilize lithium metal anodes by forming LiN_(x)O_(y)-containing solid electrolyte interphase(SEI).However,its poor solubility in electrolytes,especially ester electrolytes,hinders its applications in lithium metal ***,an organic nitrate,isosorbide nitrate(ISDN),is proposed to replace LiNO_(3).ISDNhas a high solubility of 3.3M in ester electrolytes due to the introduction of organic segments in the *** decomposition of ISDN generates LiN_(x)O_(y)-rich SEI,enabling uniform lithium *** lifespan of lithium metal batteries with ISDN significantly increases from 80 to 155 cycles under demanding ***,a lithium metal pouch cell of 439Whkg^(−1) delivers 50 *** work opens a new avenue to develop additives by molecular modifications for practical lithium metal batteries.

关键词： electrolyte additives lithium metal anodes organic nitrate pouch cells solid electrolyte interphase

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