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Quantifying the solid electrolyte interphase stress induced capacity fading of lithium-ion batteries via a multiscale mechanicalelectrochemical coupling model

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Science China(Technological Sciences) 2024年第10期67卷 3168-3181页

作者： HE YaoLong XU Peng JIANG DengFeng HU HongJiu LI DaWei SHI SiQi Shanghai Institute of Applied Mathematics and Mechanics School of Mechanics and Engineering ScienceShanghai UniversityShanghai 200072China Shanghai Key Laboratory of Mechanics in Energy Engineering Shanghai UniversityShanghai 200072China Shanghai Frontier Science Center of Mechanoinformatics Shanghai UniversityShanghai 200072China School of Mechanical Engineering University of Shanghai for Science and TechnologyShanghai 200093China School of Materials Science and Engineering Shanghai UniversityShanghai 200444China Materials Genome Institute Shanghai UniversityShanghai 200444China

The solid electrolyte interphase(SEI)is widely recognized as a critical factor leading to the capacity fading of lithium-ion batteries(LIBs).Although SEI stress-related mechanical failure caused by the expansion or contraction of active materials upon cycles is well documented,previously reported SEI components and overpotential varying phenomena due to SEI stress and their effects on the electrochemical performance are poorly ***,we establish a quantitative correlation between capacity fading and the SEI stress by considering its effects on side reactions,especially SEI component evolution,in a multiscale mechanical-electrochemical coupling ***,the capacity fading behaviors of two typical cells(Li[NiMnCo]O_(2) as the cathode,and graphite and silicon as the anode,respectively)were adopted as numerical examples to demonstrate its potential utility and *** within the SEI was indeed found to play a predominant role in the capacity fading of the graphite and silicon anodes,resulting in 27%and 69%of the total capacity loss after 200 and 100 cycles at 1 C,*** study provides valuable mechanical insights into the variations of SEI properties related to the capacity degradation and SEI optimization and design for LIBs.

关键词： solid electrolyte interphase capacity fading multiscale mechanical-electrochemical coupling stress analysis

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Synthetic poly-dioxolane as universal solid electrolyte interphase for stable lithium metal anodes

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Journal of Energy Chemistry 2021年第11期30卷 172-178,I0004页

作者： Tao Chen Haiping Wu Jing Wan Mengxue Li Yucheng Zhanga Lin Sun Yuncong Liu Lili Chen Rui Wen Chao Wang Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Battery Technology BYD Shanghai Co.Ltd.Shanghai 201611China Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China

Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we report a new synthetic poly-dioxolane (PDOL) approach to constructing an artificial 'elastic' SEI to stabilize the Li/electrolyte interface and the Li deposition/dissolution behavior in a variety of electrolytes. By coating PDOL with optimized molecular weights and synthetic routes on Li metal anode, the 'elastic' SEI layer could be maintained on top of the Li metal anode to accommodate the Li deposition/dissolution. No dendrite formation was observed during the cycling process, and the interfacial side reactions were reduced significantly. Consequently, we successfully achieved 330 cycles with a CE of 98.4% in ether electrolytes and 90 cycles with a CE of 94.3% in carbonate electrolytes. Simultaneously, the Li-metal batteries with LiFePO_(4) as cathodes also exhibited improved cycling performance. This strategy could promote the development of dendrite-free metal anodes toward high-performance Li-metal batteries.

关键词： Polymer Lithium metal anodes solid electrolyte interphase Lithium-ion batteries

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In situ fluorinated solid electrolyte interphase towards long-life lithium metal anodes

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Nano Research 2020年第2期13卷 430-436页

作者： Shan-Min Xu Hui Duan Ji-Lei Shi Tong-Tong Zuo Xin-Cheng Hu Shuang-Yan Lang Min Yan Jia-Yan Liang Yu-Guo Yang Qing-Hua Kong Xing Zhang Yu-Guo Guo School of Science Beijing Jiaotong UniversityBeijing 100044China CAS Key Laboratory of Molecular Nanostructure and Nanotechmology CAS Research/Education Center for Excellence in Molecular Sciences and Beijing National Laboratory for Molecular Sciences(BNLMs)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The urgent demands for high-energy-density rechargeable batteries promote a flourishing development of Li metal ***,the uncontrollable dendrites growth and serious side reactions severely lirmit its commercial ***,an artificial LiF-rich solid electrolyte interphase(SEl)is constructed at molecular-level using one-step photopolymerization of hexafluorobutyl acrylate based solution,where the LiF is in situ generated during photopolymerization process(denoted as PHALF).The LiF-rich layercomprised flexible polymer matrix and inorganic LiF filler not only ensures intimate contact with Li anode and adapts volume fluctuations during cycling but also regulates Li deposition behavior,enabling it to suppress the dendrite growth and block side reactions between the electrolyte and Li ***,the PHALF-Li anode presents superior stable cycling performance over 500 h at 1 mA·cm^-2 for 1 mA·h·cm^-2 without dendrites growth in carbonate *** work provides a novel approach to design and build in situ artificial SEl layer for high-safety and stable Li metal anodes.

关键词： lithium metal batteries artificial in situ solid electrolyte interphase LiF

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Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano Research 2024年第8期17卷 7163-7173页

作者： Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Key Laboratory of Materials Physics of Ministry of Education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Key Laboratory of Chemical Reaction Engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China Center for High Pressure Science and Technology Advanced Research PudongShanghai 201203China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

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A review on the failure and regulation of solid electrolyte interphase in lithium batteries

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Journal of Energy Chemistry 2021年第8期30卷 306-319,I0007页

作者： Jun-Fan Ding Rui Xu Chong Yan Bo-Quan Li Hong Yuan Jia-Qi Huang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology100081 BeijingChina

solid electrolyte interphase(SEI)has been widely recognized as the most important and the least understood component in lithium *** the intrinsic instability in both chemical and mechanical,the failure of SEI is inevitable and strongly associated with the performance decay of practical working *** this Review,the failure mechanisms and the corresponding regulation strategies of SEI are ***,the fundamental properties of SEI,including the formation principles,and the typical composition and structures are briefly ***,the common SEI failure modes involving thermal failure,chemical failure,and mechanical failure are classified and discussed,*** that,the regulation strategies of SEI with respect to different failure modes are further ***,the future endeavor in further disclosing the mysteries of SEI is prospected.

关键词： solid electrolyte interphase Failure mechanism Regulation strategy Lithium batteries

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Unraveling the heterogeneity of solid electrolyte interphase kinetically affecting lithium electrodeposition on lithium metal anode

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Journal of Energy Chemistry 2023年第10期85卷 181-190,I0007页

作者： Mengyuan Zhou Yaqi Liao Longhui Li Ruoyu Xiong Guancheng Shen Yifu Chen Tianlun Huang Maoyuan Li Huamin Zhou Yun Zhang State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina Guangdong Key Laboratory of Modern Control Technology Institute of Intelligent ManufacturingGuangdong Academy of SciencesGuangzhou 510075GuangdongChina

The stability and uniformity of solid electrolyte interphase(SEI)are critical for clarifying the origin of capacity fade and safety issues for lithium metal anodes(LMA).However,understanding the interplay of SEI heterogeneity and Li electrodeposition is limited by the coupling of complex electrochemistry and mechanics ***,the correlation between the SEI failure behavior and Li deposition morphology is investigated through a quantitative electrochemical-mechanical *** local deformation and stress of SEI during Li electrodeposition identify that the heterogeneous interface between different components first *** with the well-known mechanical strength,component uniformity plays the most important role in the initial SEI failure and uneven Li deposition,and a relative component uniformity(p>0.01)represents a proper balance to ensure the stability of the naturally heterogeneous ***,the component regulation of SEI via the designed electrolyte experimentally demonstrates that improving component uniformity benefits SEI stability and the uniform Li electrodeposition for LMA,thereby increasing the capacity by~20%after 300 *** fundamental understandings and proposed strategy can be not only used to guide the SEI optimization via the electrolyte regulation,but also extended to the rational designs of artificial SEI for high-performance LMA.

关键词： Li metal anode solid electrolyte interphase Component uniformity Electrochemical-mechanical model Failure mechanism

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solid electrolyte interphase in water-in-salt electrolytes

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Science China Materials 2021年第7期64卷 1571-1579页

作者： Dezhong Liu Lixia Yuan Yunhui Huang State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The water-in-salt strategy successfully expands the electrochemical window of the aqueous electrolyte from1.23 to~3.0 V,which can lead to a breakthrough in the energy output of the aqueous battery system while maintaining the advantage of high *** expanded electrochemical window of the water-in-salt electrolytes can be ascribed to the decreased water activity and the solid electrolyte interphase formed on the *** solid electrolyte interphase in the aqueous system is not fully understood,and the basic composition,the structure,and the formation mechanism are still cloaked in *** perspective summarizes the published research with emphasis on the most possible formation mechanism and composition of the interphase layer in the aqueous *** understanding of the interphase as well as rounded assessment of the water-in-salt electrolyte in practical operating conditions is *** full understanding of the interface will guide the design of aqueous electrolytes and help to build novel aqueous batteries with high safety and high energy density.

关键词： solid electrolyte interphase water-in-salt electrolytes aqueous rechargeable Li-ion batteries

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Polar interaction of polymer host-solvent enables stable solid electrolyte interphase in composite lithium metal anodes

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Journal of Energy Chemistry 2022年第1期31卷 172-178,I0006页

作者： Peng Shi Ze-Yu Liu Xue-Qiang Zhang Xiang Chen Nan Yao Jin Xie Cheng-Bin Jin Ying-Xin Zhan Gang Ye Jia-Qi Huang Stephens IfanE L Titirici Maria-Magdalena Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Collaborative Innovation Center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy TechnologyTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032ShanxiChina Department of Materials Molecular Sciences Research HubImperial College LondonLondon W12 OBZUK epartment of Chemical Engineering Imperial College LondonSouth Kensington CampusLondon SW72AZUK

The lithium(Li) metal anode is an integral component in an emerging high-energy-density rechargeable battery.A composite Li anode with a three-dimensional(3 D) host exhibits unique advantages in suppressing Li dendrites and maintaining dimensional ***,the fundamental understanding and regulation of solid electrolyte interphase(SEI),which directly dictates the behavior of Li plating/stripping,are rarely researched in composite Li metal ***,the interaction between a polar polymer host and solvent molecules was proposed as an emerging but effective strategy to enable a stable SEI and a uniform Li deposition in a working *** carbonate molecules in electrolytes are enriched in the vicinity of a polar polyacrylonitrile(PAN) host due to a strong dipole-dipole interaction,resulting in a LiF-rich SEI on Li metal to improve the uniformity of Li deposition.A composite Li anode with a PAN host delivers 145 cycles compared with 90 cycles when a non-polar host is ***,60 cycles are demonstrated in a 1:0 Ah pouch cell without external *** work provides a fresh guidance for designing practical composite Li anodes by unraveling the vital role of the synergy between a 3 D host and solvent molecules for regulating a robust SEI.

关键词： Lithium metal Polar interaction solid electrolyte interphase Lithium plating Composite anode

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A gradient solid electrolyte interphase with high Li+conductivity induced by bisfluoroacetamide additive for stable lithium metal batteries

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Nano Research 2023年第6期16卷 8425-8432页

作者： Zhaoyang Sun Ziyue Wen Yi Chen Yue Ma Jinxiang Zhang Yuejiao Li Li Li Renjie Chen Beijing Key Laboratory of Environmental Science and Engineering School of Material Science&EngineeringBeijing Institute of TechnologyBeijing 100081China Institute of Advanced Technology Beijing Institute of TechnologyJinan 250300China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing 100081China

Stable Li metal anodes have become the driving factor for high-energy-density battery ***,uncontrolled growth of Li dendrite hinders the application of rechargeable Li metal batteries(LMBs).Here,a multifunctional electrolyte additive bisfluoroacetamide(BFA)was proposed to facilitate high-performance *** uniform and dense deposition of Li^(+) was achieved due to the reduced nucleation and plateau overpotential by the addition of ***,X-ray photoelectron spectroscopy(XPS)tests reveal a gradient solid electrolyte interface(SEI)structure on the Li metal *** voltammetry(CV)curves at different sweep speeds prove the formation of pseudocapacitance at the electrode-electrolyte interface,which accelerates the Li+transport rate and protects the electrode *** low activation energy also indicates the ability of rapid Li^(+) transportation in electrolyte ***,the Li||Li symmetric cells with 1.0 wt.%BFA electrolyte exhibit good cycling performance at 0.5 mA·cm^(−2)for over 2000 h,and Li||LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)full cells maintain a high capacity for 200 cycles at 1 C rate.

关键词： electrolytes additives solid electrolyte interphase Li dendrites Li metal batteries

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Unique double-layer solid electrolyte interphase formed with fluorinated ether-based electrolytes for high-voltage lithium metal batteries

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Journal of Energy Chemistry 2024年第1期88卷 532-542,I0012页

作者： Ruo Wang Jiawei Li Bing Han Qingrong Wang Ruohong Ke Tong Zhang Xiaohu Ao Guangzhao Zhang Zhongbo Liu Yunxian Qian Fangfang Pan Iseult Lynch Jun Wang Yonghong Deng Department of Materials Science&Engineering School of Innovation and EntrepreneurshipSouthern University of Science and TechnologyShenzhen 518055GuangdongChina School of Geography Earth and Environmental SciencesUniversity of BirminghamEdgbastonBirmingham B152TTUK Key Laboratory of Marine Environmental Corrosion and Bio-Fouling Institute of OceanologyChinese Academy of SciencesQingdao 266071ShandongChina Shenzhen CAPCHEM Technology Co. Ltd.Shenzhen 518118GuangdongChina CALB Group Co. Ltd.Changzhou 213200JiangsuChina

Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy ***,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic *** key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the ***,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation *** TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced *** Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,*** study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.

关键词： Lithium metal batteries High-voltage layered oxides Fluorinated ether-based electrolytes solid electrolyte interphase Cathode electrolyte interphase

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