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Decouple charge transfer reactions in the Li-ion battery

Journal of Energy Chemistry 2024年第5期92卷 759-798页

作者： Yuxuan Bai Qiu-An Huang Kai Wu Jiujun Zhang Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444China Ningde contemporary Innovation Laboratory Contemporary Amperex Technology Co.LimitedNingde 352100FujianChina

In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is required.Although electrochemical impedance spectroscopy(EIS)is regarded as a powerful diagnosis tool,it is not a direct but an indirect measurement.With respect to this,some critical questions need to be answered:(i)why EIS can reflect the kinetics of charge transfer reactions;(ii)what the inherent logical relationship between impedance models under different physical scenes is;(iii)how charge transfer reactions compete with each other at multiple scales.This work aims at answering these questions via developing a theory framework so as to mitigate the blindness and uncertainty in unveiling charge transfer reactions in LIBs.To systematically answer the above questions,this article is organized into a three-in-one(review,tutorial,and research)type and the following contributions are made:(i)a brief review is given for impedance model development of the LIBs over the past half century;(ii)an open source code toolbox is developed based on the unified impedance model;(iii)the competive mechanisms of charge transfer reactions are unveiled based on the developed EIS-Toolbox@LIB.This work not only clarifies theoretical fundamentals,but also provides an easy-to-use open source code for EIS-Toolbox@LIB to optimize fast charge/discharge,mitigate cycle aging,and improve energy/power density.

关键词： Electrochemical impedance spectroscopy Unified impedance model Charge transfer reactions Solid/electrolyte diffusion Porous electrode EIS-Toolbox@LIB

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Lithium-ion and solvent co-intercalation enhancing the energy density of fluorinated graphene cathode

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Journal of Energy Chemistry 2024年第2期89卷 208-215,I0006页

作者： Hao Wang Jie Jiang Pengyu Chen Zhenrui Wu Xiaobin Niu Chuying Ouyang Jian Liu Liping Wang School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina School of Engineering Faculty of Applied ScienceThe University of British ColumbiaKelowna V1V 1V7Canada 21C Innovation Laboratory Contemporary Amperex Technology Ltd.(21C LAB)Ningde 352100FujianChina

Fluorinated carbons CF_xhold the highest theoretical energy density(e.g.,2180 W h kg^(-1)when x=1)among all cathode materials of lithium primary batteries.However,the low conductivity and severe polarization limit it to achieve its theory.In this study,we design a new electrolyte,namely 1 M LiBF_(4)DMSO:DOL(1:9 vol.),achieving a high energy density in Li/CF_xprimary cells.The DMSO with a small molecular size and high donor number successfully solvates Li^(+)into a defined Li^(+)-solvation structure.Such solvated Li^(+)can intercalate into the large-spacing carbon layers and achieve an improved capacity.Consequently,when discharged to 1.0 V,the CF_(1.12)cathode demonstrates a specific capacity of 1944 m A h g^(-1)with a specific energy density of 3793 W h kg^(-1).This strategy demonstrates that designing the electrolyte is powerful in improving the electrochemical performance of CF_(x) cathode.

关键词： Fluorinated carbon Conversion reaction High-energy-density primary battery Li^(+)-solvation structure Solvent co-intercalation

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Mechanical behavior analysis of high power commercial lithium-ion batteries

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Chinese Journal of Chemical Engineering 2023年第6期58卷 315-322页

作者： Ruicheng Shen Shaojun Niu Guobin Zhu Kai Wu Honghe Zheng College of Energy Soochow UniversitySuzhou 215006China contemporary amperex technology limited Ningde 352100China

In application,lithium-ion cells undergo expansion during cycling.The mechanical behavior and the impact of external stress on lithium-ion battery are important in vehicle application.In this work,18 Ah high power commercial cell with Li Ni_(0.5)Co_(0.2)Mn_(0.3)O_(2)/graphite electrode were adopted.A commercial compress machine was applied to monitor the mechanical characteristics under different stage of charge(SOC),lifetime and initial external force.The dynamic and steady force was obtained and the results show that the dynamic force increases as the SOC increasing,obviously.During the lifetime with high power driving mode,different external force is shown to have a great impact on the long-term cell performance,with higher stresses result in higher capacity decay rates and faster impedance increases.A proper initial external force(900 N)provides lower impedance increasing.Postmortem analysis of the cells with2000 N initial force suggests a close correlation between electrochemistry and mechanics in which higher initial force leads to higher direct current internal resistance(DCIR)increase rate.In addition,for the cell with higher external force,deformation of the cathode and thicker solid electrolyte interface(SEI)film on the surface of anode and separator are observed.Porosity reduction and closure was also verified after cycles which is an obstacle to the lithium ion transferring.The largest cause of the observed capacity decline was the loss of active lithium through autopsy analysis.In addition,for the cell with higher external force,deformation of the cathode and thicker SEI film on the surface of anode and separator are observed.Porosity reduction and closure was also verified after cycles which is an obstacle to the lithium ion transferring.The largest cause of the observed capacity decline was the loss of active lithium through autopsy analysis.

关键词： Lithium-ion batteries External mechanical pressure Capacity fade Static pressure Dynamic pressure

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The feasibility for natural graphite to replace artificial graphite in organic electrolyte with different film-forming additives

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Chinese Journal of Chemical Engineering 2023年第4期56卷 58-69页

作者： Shaojun Niu Guobin Zhu Kai Wu Honghe Zheng College of Energy Soochow UniversitySuzhou 215006China contemporary amperex technology limited Ningde 352100China

The feasibility for natural graphite(NG)to replace artificial graphite(AG)in organic electrolytes with different additives are investigated.Although the strong film-forming additives contributes to form robust solid electrolyte interphase(SEI)film on graphite particle surface,great differences in gas evolution,lithium inventory loss and other side reactions are observed.Lithium bis(oxalato)borate(Li BOB)and fluoroethylene carbonate(FEC)are found more effective and the combination shows to be more promising.In the optimized electrolyte,natural graphite anode exhibits excellent long-term cycling capability.After 800 cycles at high temperature,the capacity retention is comparable to that using artificial graphite.The mechanisms for the capacity-fading of the full cells with AG and NG anode are investigated by ICP,SEM and polarization studies.The results shows that NG electrode consumes more active lithium due to the rough surface and larger volume expansion.The rapid capacity-fading in the initial 100 cycles is related to the instability of the SEI film aroused from large volume expansion.The systematic analysis is inspiriting for the development of high performance lithium ion batteries with reduced cost.

关键词： Lithium ion batteries Natural graphite Electrolyte additive Solid electrolyte interphase

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An intercalation-type Li-free cathode with energy density exceeding 550 Wh kg-1

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National Science Review 2023年第3期10卷 56-57页

作者： Kai Wu Wenwei Luo Bo Xu contemporary amperex technology limited(CATL) Department of Physics Jiangxi Normal University

The development of all-solid-state technologyinvolving Li-free transition-metalbased cathodes and Li-metal anodes has become an emerging trend with regard to solving the energy and safety bottleneck of current Li-ion ...

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Prelithiation Enhances Cycling Life of Lithium-Ion Batteries:A Mini Review

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Energy & Environmental Materials 2023年第6期6卷 1-9页

作者： Xiaomei Liu Ze Wu Leqiong Xie Li Sheng Jianhong Liu Li Wang Kai Wu Xiangming He Institute of Nuclear and New Energy technology Tsinghua UniversityBeijing 100084China contemporary amperex technology Co. LimitedNinde 352100China

During the last decade,the rapid development of lithium-ion battery(LIB)energy storage systems has provided significant support for the efficient operation of renewable energy stations.In the coming years,the service life demand of energy storage systems will be further increased to 30 years from the current 20 years on the basis of the equivalent service life of renewable energy stations.However,the life of the present LIB is far from meeting such high demand.Therefore,research on the next-generation LIB with ultra-long service life is imminent.Prelithiation technology has been widely studied as an important means to compensate for the initial coulombic efficiency loss and improve the service life of LIBs.This review systematically summarized the different prelithiation methods from anode and cathode electrodes.Moreover,the large-scale industrialization challenge and the possibility of the existing prelithiation technology are analyzed,based on three key parameters:industry compatibility,prelithiation efficiency,and energy density.Finally,the future trends of improvement in LIB performance by other overlithiated cathode materials are presented,which gives a reference for subsequent research.

关键词： cycle life lithium compensation lithium-ion battery prelithiation

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Degradation mechanism of high-voltage single-crystal LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode material

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Chinese Physics B 2023年第12期32卷 618-622页

作者：柳娜 contemporary amperex technology Co. LimitedNingde 352000China

Layered cathode materials have been successfully commercialized and applied to electric vehicles.To further improve improve the energy density of these marterials is still the main efforts in the market.Therefore,developing high-voltage LiNi_(x)Co_(y)Mn_(z)O_(2)(x+y+z=1,NCM)to achieve high energy density is particularly important.However,under high voltage cycling,NCM often exhibits rapid capacity degradation,which can be attributed to oxygen release,structural phase transition and particle cracking.In this work,the representative single-crystal LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM523)was studied under various high charge cut-off voltages.Analysis by x-ray diffraction(XRD),transmission electron microscope(TEM)and electron back scatter diffraction(EBSD)measurements indicated that the rock-salt phase is formed on the surface of the particles after high voltage cycling,which is responsible for the increase of impedance and the rapid decay of capacity.Therefore,inhibiting the formation of rock-salt phase is believed an effective strategy to address the failure of NCM under high voltages.These findings provide effective guidance for the development of high-voltage NCM.

关键词： high voltage Li-ion battery phase transition LiNi_(x)Co_(y)Mn_(z)O_(2)

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Bending and wave propagation analysis of axially functionally graded beams based on a reformulated strain gradient elasticity theory

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Applied Mathematics and Mechanics(English Edition) 2023年第10期44卷 1803-1820页

作者： Shaopeng WANG Jun HONG Dao WEI Gongye ZHANG Jiangsu Key Laboratory of Engineering Mechanics School of Civil EngineeringSoutheast UniversityNanjing 210096China contemporary amperex technology Co. Ltd.Ningde 352100Fujian ProvinceChina

A new size-dependent axially functionally graded(AFG) micro-beam model is established with the application of a reformulated strain gradient elasticity theory(RSGET). The new micro-beam model incorporates the strain gradient, velocity gradient,and couple stress effects, and accounts for the material variation along the axial direction of the two-component functionally graded beam. The governing equations and complete boundary conditions of the AFG beam are derived based on Hamilton's principle. The correctness of the current model is verified by comparing the static behavior results of the current model and the finite element model(FEM) at the micro-scale. The influence of material inhomogeneity and size effect on the static and dynamic responses of the AFG beam is studied. The numerical results show that the static and vibration responses predicted by the newly developed model are different from those based on the classical model at the micro-scale. The new model can be applied not only in the optimization of micro acoustic wave devices but also in the design of AFG micro-sensors and micro-actuators.

关键词： Timoshenko beam theory reformulated strain gradient elastic theory(RSGET) axially functionally graded(AFG)material Hamilton's principle

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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 decay.In-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

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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 storage.The development of solid-state electrolytes(SSEs)is one of the most crucial subjects in the field of energy storage chemistry.The 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 deformability.In this review,a critical overview of the development,synthesis,chemical stability and remaining challenges of halide SSEs is given.The design strategies for optimizing the ionic conductivity of halide SSEs,such as element substitution and crystal structure design,are summarized in detail.Moreover,the associated chemical stability issues in terms of solvent compatibility,humid air stability and corresponding degradation mechanisms are discussed.In particular,advanced in situ/operando characterization techniques applied to halide-based ASSBs are highlighted.In addition,a comprehensive understanding of the interface issues,cost issues,and scalable processing challenges faced by halide-based ASSBs for practical application is provided.Finally,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

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