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Tackling application limitations of high-safetyγ-butyrolactone electrolytes:Exploring mechanisms and proposing solutions

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Journal of Energy chemistry 2024年第6期93卷 193-201,I0005页

作者： Haojun Wu Zhangyating Xie Guanjie Li Lei Zheng Zhiwei Zhao Jiarong He Yanbin Shen Jiahao Hu Zhangquan Peng Guiming Zhong Lidan Xing Weishan Li School of chemistry South China Normal UniversityGuangzhou 510006GuangdongChina National and Local Joint Engineering Research center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Research Center of BMET(Guangdong Province)and Key Lab.of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006GuangdongChina laboratory of Advanced Spectroelectrochemistry and Li-ion Batteries Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina i-Lab CAS Center for Excellence in NanoscienceSuzhou Institute of Nano-Tech and Nano-Bionics(SINANO)Chinese Academy of SciencesSuzhou 215123JiangsuChina School of chemical Engineering Faculty of SciencesEngineering and TechnologyThe University of AdelaideSA 5005Australia

Developing wide-temperature and high-safety lithium-ion batteries(LIBs)presents significant challenges attributed to the absence of suitable solvents possessing broad liquid range and non-flammability properties.γ-Butyrolactone(GBL)has emerged as a promising solvent;however,its incompatibility with graphite anode has hindered its *** limitation necessitates a comprehensive investigation into the underlying mechanisms and potential *** this study,we achieve a molecular-level understanding of the perplexing interphase formation process by employing in-situ spectroelectrochemical techniques and density function *** findings reveal that,even at high salt concentrations,GBL consistently occupies the primary Li^(+)solvation sheath,leading to extensive GBL decomposition and the formation of a high-impedance and inorganic-poor solid-electrolyte interphase(SEI)*** to manipulating solvation structures,our research demonstrates that the utilization of filmforming additives with higher reduction potential facilitates the pre-establishment of a robust SEI film on the graphite *** approach effectively inhibits GBL decomposition and significantly enhances the battery's *** study provides the first reported intrinsic understanding of the unique GBLgraphite incompatibility and offers valuable insights for the development of wide-temperature and high-safety LIBs.

关键词： γ-Butyrolactone/Graphite incompatibility Unique solvation structure SEI film Lithium-ion batteries

Progress in in-situ electrochemical nuclear magnetic resonance for battery research

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Magnetic Resonance Letters 2024年第2期4卷 13-21页

作者： Yong Jiang Mengmeng Zhao Zhangquan Peng Guiming Zhong laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of chinese Academy of Sciences Beijing100049China Tianmu Lake Institute of Advanced Energy Storage Technologies co. Ltd.Liyang213300China

A thorough understanding of the fundamental electrochemical and chemical processes in batteries is crucial to advancing energy density and power ***,the characterizations of such processes are ***-situ electrochemical nuclear magnetic resonance(Ec-NMR)offers the capability to collect real-time data during battery operation,furnishing insights into the local structures and ionic dynamics of materials by monitoring changes in the chemical environment around the ***-NMR also has the advantages of being both quantitative and *** paper systematically reviews the design of Ec-NMR approach,and delves into the applications and progress of Ec-NMR concerning battery reaction mechanisms,failure mechanisms,and overall battery *** review culminates in a comprehensive summary of the perspective and challenges associated with Ec-NMR.

关键词： In-situ NMR Reaction mechanism Failure mechanism Battery systems Ionic dynamics

Misfit strains inducing voltage decay in LiMn_(y)Fe_(1-y)PO_(4)/c

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Journal of Energy chemistry 2022年第5期31卷 206-212页

作者： chun Luo Yao Jiang Xinxin Zhang chuying Ouyang Xiaobin Niu Liping Wang School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina c innovation laboratory Contemporary Amperex Technology Ltd.(21C LAB)Ningde 352100FujianChina

LiMn_(y)Fe_(1-y)PO_(4) is considered a promising cathode material for next-generation lithium-ion batteries(LIBs) due to its high energy density and low cost. Its energy density degradation is often ascribed to the capacity loss during cycling. However, in this study, we find that the energy density degradation mainly roots in voltage decay. We have synthesized a series of LiMn_(y)Fe_(1-y)PO_(4) /c(0.5 ≤ y ≤ 0.8) and find this voltage decay is correlated with the Mn content. A high amount Mn leads to a heavier voltage ***-situ X-ray diffraction(XRD) and high-resolution transmission electron microscopy(HRTEM) reveal the nature of this effect, which show a mismatch along the b-axis of-2.68%(charge) and +3.4%(discharge), a volume misfit of-4.41%(charge) and +4.54%(discharge) between Li_(x)Mn_(y)Fe_(1-y)PO_(4) and Mn_(y)Fe_(1-y)PO_(4) during phase transitions. The resultant misfit strains during Li+insertion compared to extraction result in structural degradations, such as amorphization and impurity(Mn F3) accumulation after cycling. The voltage decay can be alleviated by kinetic relaxations and recovered by a wild reannealing. This work demonstrates effective strategies to improve the energy density and cycling performance of LiMn_(y)Fe_(1-y)PO_(4) /c,providing good references for other LIB cathodes, such as the Li-rich cathodes.

关键词： Olivine cathodes LiMn_(y)Fe_(1-y)PO_(4)/c Voltage decay Misfit strains Structural degradation

Fluorinated soft carbon as an ultra-high energy density potassium-ion battery cathode enabled by a ternary phase K_(x)Fc

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Journal of Energy chemistry 2023年第2期77卷 38-44,I0002页

作者： Pengyu chen Bojun Wang Zhenrui Wu Xiaobin Niu chuying Ouyang Hong Li Liping Wang School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina School of Engineering The University of British ColumbiaKelowna V1V 1V7Canada c innovation laboratory Contemporary Amperex Technology Ltd.(21C LAB)Ningde 352100FujianChina Key laboratory for Renewable Energy Institute of PhysicsChinese Academy of SciencesBeijing 100190China

Fluorinated carbons(cFx)have been widely applied as lithium primary batteries due to their ultra-high energy *** will be a great promise if cFx can be *** this study,we rationally tune the c-F bond strength for the alkaline intercalated cFx via importing an electronegative weaker element K instead of *** forms a ternary phase K_(x)Fc instead of two phases(LiF+c)in lithium-ion ***,we choose a large layer distance and more defects cFx,namely fluorinated soft carbon,to accommodate ***,we enable cFx rechargeable as a potassium-ion battery *** detail fluorinated soft carbon cF_(1.01) presents a reversible specific capacity of 339 mA h g^(-1)(797 Wh kg^(-1))in the 2nd cycle and maintains 330 mA h g^(-1)(726 Wh kg^(-1))in the 15th *** study reveals the importance of tuning chemical bond stability using different alkaline ions to endow batteries with *** work provides good references for focusing on developing reversible electrode materials from popular primary cell configurations.

关键词： Fluorinated carbon High energy density battery Potassium-ion battery conversion reaction K-free cathode

An ultra-low concentration electrolyte with fluorine-free bulky anions for stable potassium metal batteries

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Nano Research 2023年第6期16卷 8290-8296页

作者： Qinguang Liu Mei Geng Ting Yu Li Zhang changdong Wu Jie Liu Shulin Zhao Qingxin Yang Robin Song Jingjuan Ye Fenfen Wang Yuping Wu Dengji Xiao Yuhui chen State Key laboratory of Materials-Oriented chemical Engineering and School of Energy Science and EngineeringNanjing Tech UniversityNanjing 211816China Jiangsu Sunpower co. Ltd.Taixing 225411China

Potassium metal battery is a promising alternative to Li-ion battery for large-scale energy storage due to the abundant potassium resources and high energy ***,it suffers from rapid capacity fading and safety issues due to the uncontrolled dendrite ***,we design a fluorine-free ultra-low concentration electrolyte(ULcE)with the super bulky[BPh_(4)]^(−) anions for stable potassium metal *** this special electrolyte,the migration rate of K+in the electrolyte is about six times faster than that of the[BPh_(4)]^(−) anions because of the super bulky structure of the[BPh_(4)]^(−) anions,thus resulting in a high K^(+)transference number of *** high transference number can effectively make up for the deficiency of K^(+)in ULcE for ensuring the normal operation of the potassium metal *** addition,the improved transference number can also promote the uniform distribution of K^(+)flux on the surface of the K metal anode,resulting in uniform K *** a result,this electrolyte achieves a high K plating/stripping coulombic efficiency of 92.6%over 200 cycles and a stable discharging/charging for 100 cycles under the full battery configuration(K used as the anode and perylene-3,4,9,10-tetracarboxylic dianhydride used as the cathode).

关键词： potassium metal batteries ultra-low concentration electrolyte high transference number

Air-stability of sodium-based layered-oxide cathode materials

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Science china chemistry 2022年第6期65卷 1076-1087页

作者： Hu-Rong Yao Lituo Zheng Sen Xin Yu-Guo Guo Fujian Provincial Key laboratory of Quantum Manipulation and New Energy Materials College of Physics and EnergyFujian Normal UniversityFuzhou350117China cAS Key laboratory of Molecular Nanostructure and Nanotechnology Institute of ChemistryChinese Academy of Sciences(CAS)Beijing100190China Fujian Provincial collaborative innovation center for Advanced High-Field Superconducting Materials and Engineering Fuzhou350117China University of chinese Academy of Sciences Beijing100049China c innovation laboratory Contemporary Amperex Technology Ltd.(CATL)Ningde352100China

Sodium-ion batteries have the potential to be an alternative to lithium-ion batteries especially for applications such as large-scale grid energy storage. The development of suitable cathode materials is crucial to the commercialization of sodium-ion ***-based layered-type transition metal oxides are promising candidates as cathode materials as they offer decent energy density and are easy to be synthesized. Unfortunately, most layered oxides suffer from poor air-stability, which greatly increases the cost of manufacturing and handling. The air-sensitivity severely limits the development and commercial application of sodium-ion batteries. A review that summarizes the latest understanding and solutions of air-sensitivity is desired. In this review,the background and fundamentals of sodium-based layered-type cathode materials are presented, followed by a discussion on the latest research on air-sensitivity of these materials. The mechanism is complex and involves multiple chemical and physical reactions. Various strategies are shown to alleviate some of the corresponding problems and promote the feasible application of sodium-ion batteries, followed by an outlook on current and future research directions of air-stable cathode materials. It is believed that this review will provide insights for researchers to develop practically relevant materials for sodium-ion batteries.

关键词： sodium-ion batteries layered oxide cathodes air-sensitivity mechanism and strategies

Boosting Li-ion storage in Li2MnO_(3) by unequal-valent Ti4+-substitution and interlayer Li vacancies building

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chinese chemical Letters 2023年第4期34卷 564-569页

作者： Yu Tian Yuling Zhao Fanqi Meng Kaicheng Zhang Yanyuan Qi Yujie Zeng congcong cai Yuli Xiong Zelang Jian Yang Sun Lin Gu Wen chena School of Materials Science and Engineering Key laboratory of Advanced technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Materials Shenzhen Campus of Sun Yat-sen UniversityShenzhen 518107China c innovation laboratory Contemporary Amperex Technology Ltd.(CATL)Ningde 352100China Institute of Physics Chinese Academy of SciencesBeijing 100190China Sanya Science and Education innovation Park of Wuhan University of technology Wuhan 430070China

Lithium rich layered oxide(LRLO) has been considered as one of the promising cathodes for lithium-ion batteries(LIBs). The high voltage and large capacity of LRLO depend on Li2MnO_(3)phase. To ameliorate the electrochemical performance of Li2MnO_(3), also written as Li(Li1/3Mn2/3)O_(2), we propose a strategy to substitute Mn4+and Li+in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO_(3)by inhibiting the excessive oxidation of O_(2)-above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O_(2)with high interlayer Li vacancies, which presents a high capacity(290 m Ah/g at 10 m A/g) and stable cycling performance(84% over 60 cycles at 50 m A/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.

关键词： Lithium-ion batteries Li2MnO_(3) Unequal-valent Ti4+-substitution Interlayer Li vacancies Activated Mn3+/4+redox

Li^(+)Solvation Mediated Interfacial Kinetic of Alloying Matrix for Stable Li Anodes

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Energy & Environmental Materials 2023年第2期6卷 70-80页

作者： Xingyi Wang Kailin Luo Lixin Xiong Tengpeng Xiong Zhendong Li Jie Sun Haiyong He chuying Ouyang Zhe Peng Ningbo Institute of Materials technology and Engineering Chinese Academy of SciencesNingbo 315201China Department of Physics Laboratory of Computational Materials PhysicsJiangxi Normal UniversityNanchang 330022China 21c innovation laboratory Contemporary Amperex Technology Ltd.(CATL)Ningde 352100China

Severe lithium(Li)dendrite growth caused by the uneven overpotential deposition is a formidable challenge for high energy density Li metal batteries(LMBs).Herein,we investigate a synergetic interfacial kinetic to regulate Li deposition behavior and stabilize Li metal *** constructing Li alloying matrix with a bi-functional silver(Ag)-Li_(3)N blended interface,fast Li^(+)conductivity and high Li affinity can be achieved simultaneously,resulting in both decreased Li nucleation and mass transfercontrolled *** these properties,a more important feature is demonstrated herein;that is,the inward diffusion depth of the Li adatoms inside of the Ag site can be restricted by the Li^(+)solvation structure in a highly coordinating *** latter feature can ensure the durability of the operational Ag sites,thereby elongating the Li protection ability of the Ag-Li_(3)N interface *** work provides a deep insight into the synergetic effect of functional alloying structure and Li^(+)solvation mediated interfacial kinetic on Li metal protection.

关键词： Li^(+)solvation structure Li-Ag alloy lithium metal anode lithium metal batteries SEI

Recent Progress in and Perspectives on Emerging Halide Superionic conductors for All‑Solid‑State Batteries

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Electrochemical Energy Reviews 2023年第1期6卷 234-279页

作者： Kaiyong Tuo chunwen Sun Shuqin Liu School of chemical and Environmental Engineering China University of Mining&Technology(Beijing)Beijing 100083China 21c innovation laboratory Contemporary Amperex Technology Ltd.(21C LAB)Ningde 352100FujianChina

Rechargeable all-solid-state batteries(ASSBs)are considered to be the next generation of devices for electrochemical energy *** development of solid-state electrolytes(SSEs)is one of the most crucial subjects in the field of energy storage *** newly emerging halide SSEs have recently been intensively studied for application in ASSBs due to their favorable combination of high ionic conductivity,exceptional chemical and electrochemical stability,and superior mechanical *** this review,a critical overview of the development,synthesis,chemical stability and remaining challenges of halide SSEs is *** design strategies for optimizing the ionic conductivity of halide SSEs,such as element substitution and crystal structure design,are summarized in ***,the associated chemical stability issues in terms of solvent compatibility,humid air stability and corresponding degradation mechanisms are *** particular,advanced in situ/operando characterization techniques applied to halide-based ASSBs are *** addition,a comprehensive understanding of the interface issues,cost issues,and scalable processing challenges faced by halide-based ASSBs for practical application is ***,future perspectives on how to design high-performance electrode/electrolyte materials are given,which are instructive for guiding the development of halide-based ASSBs for energy conversion and storage.

关键词： Halide solid-state electrolytes Synthesis Ionic conductivity chemical stability In situ/operando characterization All-solid-state batteries