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Sulfolane-Graphite Incompatibility and Its Mitigation in Li-ion Batteries

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Energy & Environmental Materials 2022年第3期5卷 906-911页

作者： Qinfeng Zheng Guanjie Li Xiongwen Zheng lidan xing Kang Xu Weishan Li Engineering Research Center of MTEES(Ministry of Education) Research Center of BMET(Guangdong Province)Engineering Lab.of OFMHEB(Guangdong Province)Key Lab.of ETESPG(GHEI)and Innovative Platform for ITBMD(Guangzhou Municipality)School of Chemistry and EnvironmentSouth China Normal UniversityGuangzhou 510006China Battery Science Branch Sensor and Electron Devices DirectorateU.S.Army Research LaboratoryAdelphiMD 20783USA

The non-flammability and high oxidation stability of sulfolane(SL)make it an excellent electrolyte candidate for lithium-ion batteries(LIBs).However,its incompatibility with graphitic anode prevents the realization of these *** understand how this incompatibility arises on molecular level so that it can be suppressed,we combined theoretical calculation and experimental characterization and reveal that the primary Li^(+) solvation sheath in SL is depleted of fluorine *** reduction,SL in such fluorine-poor solvation sheath generates insoluble dimer with poor electronic insulation,hence leading to slow but sustained parasitic *** fluorine content in Li^(+)-SL solvation sheath is increased via salt concentration,a high stability LiF-rich interphase on graphite can be *** new understanding of the failure mechanism of graphite in SL-based electrolyte is of great significance in unlocking many possible electrolyte solvent candidates for the high-voltage cathode materials for next-generation LIBs.

关键词： graphite anode interphasial incompatibility mechanism lithium-ion batteries sulfolane

Phase Transformation of Lithium-rich Oxide Cathode in Full Cell and its Suppression by Solid Electrolyte Interphase on Graphite Anode

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Energy & Environmental Materials 2020年第1期3卷 19-28页

作者： Wenqiang Tu Yucheng Wen Changchun Ye lidan xing Kang Xu Weishan Li School of Chemistry and Environment South China Normal UniversityGuangzhou 510006China National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)and Key Lab.of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006China Electrochemistry Branch Sensor and Electron Devices DirectoratePower and Energy DivisionU.S.Army Research LaboratoryAdelphi MD 20783USA

Lithium-rich oxide is one of the most promising cathodes that meet high energy density requirement for batteries of the future, but its phase transformation from layer to spinel structure caused by the lattice instability presents severe challenge to cycling stability and the actually accessible capacity. The currently available approaches to suppress this undesired irreversible process often resort to limit the high voltages that lithium-rich oxide is exposed to. However, cycling stability thus improved is at the expense of the eventual energy output. In this work, we identified a new mechanism that is directly responsible for the lithium-rich oxide phase transformation and established a clear correlation between the successive consumption of Li+on anode due to incessant interphase repairing and the over-delithiation of lithium-rich oxide cathode. This new mechanism enables a simple but effective solution to the cathode degradation, in which an electrolyte additive is used to build a dense and protective interphase on anode with the intention to minimize Li depletion at cathode. The application of this new interphase effectively suppresses both electrolyte decomposition at anode and the phase transformation of lithium-rich oxide cathode, leading to high capacity and cycling stability.

关键词： electrolyte additive graphite-based battery lithium-rich oxide cathode phase transformation suppression

Suppression of Co(Ⅱ)ion deposition and hazards:Regulation of SEI film composition and structure

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Journal of Energy Chemistry 2024年第2期89卷 259-265,I0007页

作者： Jiaqi Zhan Mingzhu Liu Yutian Xie Jiarong He Hebing Zhou lidan xing Weishan Li 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)Key Lab.of ETESPG(GHEI)Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina

Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and transition metal ions in the ***,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in ***,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline Li F,effectively inhibits the undesired Li^(+)/Co^(2+)ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic ***,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interphacial stability of the graphite *** findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guidance for designing next-generation electrolytes.

关键词： Lithium-ion batteries Transition metal ions SEI film Composition and structure

Enhanced interphasial stability of hard carbon for sodium-ion battery via film-forming electrolyte additive

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Nano Research 2023年第3期16卷 3823-3831页

作者： Wenguang Zhang Fanghong Zeng Huijuan Huang Yan Yu Mengqing Xu lidan xing Weishan Li Engineering Research Center of MTEES(Ministry of Education) Research Center of BMET(Guangdong Province)Engineering Lab.of OFMHEB(Guangdong Province)Key Lab.of ETESPG(GHEI)and Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006China Hefei National Laboratory for Physical Sciences at the Microscale Department of Materials Science and EngineeringCAS Key Laboratory of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei 230026China

Although the operating mechanism of sodium-ion battery(SIB)resembles that of lithium-ion battery,common film-forming additive for lithium-ion battery does not play its role in ***,it is essential to tailor new additives for *** carbon(HC),as the most used anode material of SIB,has the disadvantage of interphasial instability,especially under the condition of long-term *** incessant accumulation of electrolyte decomposition products leads to a significant increase in interphasial impedance and a sharp decline in discharge *** this work,N-phenyl-bis(trifluoromethanesulfonimide)(PTFSI)was proposed as a novel film-forming electrolyte additive,which effectively enhances the long-term cycling performance for HC anode in *** passivation film generated from the preferential reduction of PTFSI improves the capacity retention of HC/Na half-cell from 0%to 68%after 500 ***,the enhanced interphasial stability of HC anode results in a 52%increase in capacity retention of HC/Na_(3)V_(2)(PO_(4))_(3)full-cells after 100 cycles.

关键词： hard carbon anode interphasial stability N-phenyl-bis(trifluoromethanesulfonimide) sodium-ion battery

Outstanding performances of graphite||NMC622 pouch cells enabled by a non-inert diluent

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Journal of Energy Chemistry 2023年第6期81卷 593-602,I0013页

作者： Qinqin Cai Hao Jia Guanjie Li Zhangyating Xie Xintao Zhou Zekai Ma lidan xing Weishan Li Engineering Research Center of MTEES(Ministry of Education) Research Center of BMET(Guangdong Province)Engineering Lab.of OFMHEB(Guangdong Province)Key Lab.of ETESPG(GHEI)and Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina

Although high salt concentration electrolyte(HCE)can construct effective Li F-rich interphase film and solve the interphasial instability issue of graphite anode,its high cost,high viscosity and poor wettability with electrode materials limit its large-scale ***,localized high concentration electrolyte(LHCE)is obtained by introducing an electrochemically inert diluent into HCE to avoid the above-mentioned problems while maintaining the high interphasial stability of HCE with graphite *** traditional inert diluents,1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluropropyl ether(TTE)with electrochemical activity is introduced into propylene carbonate(PC)-based HCE to obtain LHCE-2(1 M LiPF_(6),PC:DMC:TTE=1:1:6.1)*** and theoretical simulation results show that TTE participates in the oxidation decomposition and film-forming reaction at the NCM622 cathode surface,conducting a cathode electrolyte interphase(CEI)rich in organic fluorides with excellent electron insulation ability,high structural stability and low interphasial *** to the outstanding interphasial properties induced by LHCE-2,the graphite||NMC622 pouch cell reaches a capacity retention of 80%after 500 cycles at 1 C under room *** at sub-zero temperatures,the capacity released by the cell with LHCE-2 electrolyte is significantly higher than that of HCE and conventional EC-based ***,the LHCE-2 electrolyte inherits the advantages of TTE flame-resistant,thus improving the safety of the battery.

关键词： Lithium-ion batteries Propylene carbonate Localized high-concentration electrolyte Non-Inert diluent Graphite||NMC622 pouch cells

Revealing the critical effect of solid electrolyte interphase on the deposition and detriment of Co(Ⅱ) ions to graphite anode

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Journal of Energy Chemistry 2022年第6期31卷 389-396,I0011页

作者： Qiming Xie Jiawei Chen lidan xing Xianggui Zhou Zekai Ma Binhong Wu Yilong Lin Hebing Zhou Weishan Li China National and Local Joint Engineering Research Center of MPTES in High Energy andSafety LIBs Engineering Research Center of MTEES(Ministry of Education)Research Center of BMET(Guangdong Province).Schoolof Chemistry.South China Normal University.Guangzhou 510006.Guangdong.China

"Dissolution,migration,and deposition"of transition metal ions (TMIs) result in capacity degradation of lithium-ion batteries (LIBs).Understanding such detrimental mechanism of TMIs is critical to the development of LIBs with long cycle *** most previous works,TMIs were directly introduced into the electrolyte to investigate such a detrimental *** these cases,the TMIs are deposited directly on the fresh anode ***,in the practical battery system,the TMIs are deposited on the anode covered with solid electrolyte interphase (SEI) *** the pre-presence of SEI film on anode surface influences the deposition and detriment of TMIs is *** this work,the deposition of Co element on graphite anode with and without SEI film were systematically *** results clearly show that,in comparison with that of fresh graphite (SEI-free),the presence of SEI film aggravates the deposition of Co ions due to the Li^(+)–Co^(2+) ion exchange between the SEI and Co^(2+)-containing electrolyte without the driving of the electric field,leading to faster capacity fading of graphite ***,how to regulate electrolytes and film-forming additives to design the components of SEI and prevent its exchange with TMIs,is a crucial way to inhibit the deposition and detriment of TMIs on graphite anode.

关键词： Lithium-ion batteries Transition metal ions Ion exchange Graphite anode SEI film

Protective electrode/electrolyte interphases for high energy lithium-ion batteries with p-toluenesulfonyl fluoride electrolyte additive

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Journal of Energy Chemistry 2021年第1期30卷 361-371,I0012页

作者： Yanxia Che Xiuyi Lin lidan xing Xiongcong Guan Rude Guo Guangyuan Lan Qinfeng Zheng Wenguang Zhang 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)and Key Lab.of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006GuangdongChina

High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte additive to enhance the cycling performances of graphite/LiNi0.6Co0.2Mn0.2O2 pouch *** comparison with the baseline electrolyte,a small dose of pTSF can significantly improve the cyclic stability of the *** calculations together with experimental results indicate that pTSF would be oxidized and reduced to construct protective interphase film on the surfaces of LiNi0.6Co0.2Mn0.2O2 cathode and graphite anode,*** S-containing surface films derived from pTSF effectively mitigate the decomposition of electrolyte,reduce the interphasial impedance,as well as prevent the dissolution of transition metal ions from Ni-rich cathode upon cycling at high *** finding is beneficial for the practical application of high energy density graphite/LiNi0.6Co0.2Mn0.2O2 cells.

关键词： Lithium-ion batteries Electrolyte additive P-toluenesulfonyl fluoride Electrode/electrolyte interphase Graphite/LiNi0.6Co0.2Mn0.2O2

Innovative discontinuous-SEI constructed in ether-based electrolyte to maximize the capacity of hard carbon anode

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Journal of Energy Chemistry 2023年第4期79卷 459-467页

作者： Fanghong Zeng lidan xing Wenguang Zhang Zhangyating Xie Mingzhu Liu Xiaoyan Lin Guangxia Tang Changyong Mo Weishan Li Engineering Research Center of MTEES(Ministry of Education) Research Center of BMET(Guangdong Province)Engineering Lab.of OFMHEB(Guangdong Province)Key Lab.of ETESPG(GHEI)and Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina

Compared with graphite,the lower sodiation potential and larger discharge capacity of hard carbon(HC)makes it the most promising anode material for sodium-ion *** ether-based electrolyte rather than conventional carbonate-based electrolyte,HC achieves superior electrochemical ***,the mechanism by which ether-based electrolyte improves the properties of HC is still controversial,primarily focusing on whether it forms solid electrolyte interphase(SEI)*** this work,according to the sodium storage mechanisms in HC at low voltage(<0.1 V),including Na^(+)-diglyme co-interaction into the carbon layer(SEI forbidden)and desolvated Na^(+)insertion in the irregular carbon holes(SEI required),the NaPF6concentration in ether-based electrolyte was regulated,so as to construct a discontinuous-SEI on the surface of the HC anode,which significantly enhances the electrochemical performances of ***,with 0.2 M NaPF6ether-based electrolyte,HC deliverers a discharge capacity of 459.7 mA h g^(-1)at 0.1 C and stays at 357.2 mA h g^(-1)after 500 cycles at 1 C,which is substantially higher than that of higher/lower salt concentration electrolytes.

关键词： Sodium ion battery Hard carbon Ether-based electrolyte SEI/SEI-free

Inhibiting manganese(Ⅱ)from catalyzing electrolyte decomposition in lithium-ion batteries

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Journal of Energy Chemistry 2022年第2期31卷 1-8页

作者： Xuehuan Luo lidan xing Jenel Vatamanu Jiawei Chen Jiakun Chen Mingzhu Liu Cun Wang Kang Xu Weishan Li Engineering Research Center of MTEES(Ministry of Education) Research Center of BMET(Guangdong Province)Engineering Lab.of OFMHEB(Guangdong Province)Key Lab.of ETESPG(GHEI)and Innovative Platform for ITBMD(Guangzhou Municipality)School of Chemistry and EnvironmentSouth China Normal UniversityGuangzhou 510006GuangdongChina Battery Science Branch Sensor and Electron Devices DirectorateU.S.Army Research LaboratoryAdelphiMD 20783United States

A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified *** order to deactivate the catalytic activity of such manganese(II)ion,1-aza-12-crown-4-ether(A12C4)with cavity size well matched manganese(Ⅱ)ion is used in this work as electrolyte *** and experimental results show that stable complex forms between A12C4 and manganese(II)ions in the electrolyte,which does not affect the solvation of Li *** strong binding effect of A12C4 additive reduces the charge density of manganese(II)ion and inhibits its destruction of the PF_(6)^(-)structure in the electrolyte,leading to greatly improved thermal stability of manganese(II)ions-containing *** addition to bulk electrolyte,A12C4 additive also shows capability in preventing Mn^(2+) from degrading SEI on graphite *** bulk and interphasial stability introduced by A12C4 leads to significantly improved cycling performance of LIBs.

关键词： Manganese(Ⅱ)ions Electrolyte decomposition 1-Aza-12-crown-4-ether Thermal stability