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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

Degradation of platinum electrocatalysts for methanol oxidation by lead contamination

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Chinese Chemical Letters 2023年第2期34卷 610-612页

作者： Zihao li Xianggui Zhou Subhash Singh Xiaoming Wei Chunlei Guo weishan li School of Physics and Optoelectronics South China University of TechnologyGuangzhou 510640China The Institute of Optics University of RochesterRochesterNew York 14627United States School of Chemistry South China Normal UniversityGuangzhou 510006China

Platinum exhibits high electrocatalytic activity toward various reactions but might be poisoned by some species. This communication reports a new finding that the electrocatalytic activity of platinum for methanol oxidation will be largely lost in a lead-contaminated environment. This activity loss is demonstrated in an electrochemical cell using a lead counter electrode for measuring the activity of platinum electrode towards methanol oxidation. The recorded methanol oxidation current in this cell is significantly decreased compared with that using a platinum counter electrode. The possible mechanism is related to the adsorption of trace lead ions from the lead counter electrode, as confirmed by comparing the calculated binding energies of platinum and lead ions with oxygen ion. This report is of great importance for reliably designing and efficiently managing direct methanol fuel cells, because trace lead might be present in various components in the fuel cell systems or in air and attention should be paid to its negative effect.

关键词： Activity degradation Platinum electrocatalyst Lead contamination Methanol oxidation Binding energy

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

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

Recent Advances of Electroplating Additives Enabling lithium Metal Anodes to Applicable Battery Techniques

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Energy & Environmental Materials 2021年第3期4卷 284-292页

作者： Xianshu Wang Weicong Mai Xiongcong Guan Qi liu Wenqiang Tu weishan li Feiyu Kang Baohua li Shenzhen Key Laboratory on Power Battery Safety and Shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China School of Materials Science and Engineering Tsinghua UniversityBeijing 100084China School of Chemistry 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

lithium(li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of li metal ***,the intractable dendritic li deposition during cycling greatly restrains the large-scale applications of li metal *** advances have been explored to address this issue,among which a specific class of electrolyte additives for electroplating is deeply impressive,as they are economic and *** from the conventional additives that construct solid electrolyte interphase(SEI)layer on anodes,they make dendrite-free li metal anodes feasible through altering li plating *** this research news article,the interlinked principles between industrial electroplating and li deposition are firstly *** featured effects of electroplating additives on regulating li plating morphology are also summarized and mainly divided into three categories:co-deposition with li cation,coordination with li cation,and leveling effect of li ***,the mechanism exploration or derivative use of electroplating additive for dendrite suppression and potential research directions are proposed,with emphasizing that industrial electroplating might enable li metal anode to scalable battery techniques and spread to metal battery systems beyond li.

关键词： electroplating additives lithium metal anodes co-deposition coordination leveling effect

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

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

Highly improved cyclic stability of Ni-rich/li batteries with succinic anhydride as electrolyte additive and underlying mechanism

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Journal of Energy Chemistry 2023年第3期78卷 80-90,I0003页

作者： Shu Yang Guanjie li Xiaoyan lin Changyong Mo Xianggui Zhou lijiao Quan Kuan Zhou Suli li Hai Wang weishan li School of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina Zhuhai CosMX Battery Co. LtdZhuhai 519180GuangdongChina 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

lithium-metal battery based on Ni-rich cathode provides high energy density but presents poor cyclic stability due to the unstable electrode/electrolyte interfaces on both cathode and *** this work,we report a new strategy to address this *** is found that the cyclic stability of Ni-rich/li battery can be significantly improved by using succinic anhydride(SA) as an electrolyte ***,the capacity retention of liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)/li cell is improved from 14% to 83% after 200cycles at 1 C between 3.0 and 4.35 V by applying 5% *** underlying mechanism of SA contribution is understood by comparing the effects of malic anhydride(MA) and citraconic anhydride(CA), both of which share a similar molecular structure to SA but show different *** anode side,SA can but MA and CA cannot form a protective solid electrolyte interphase(SEI) on li *** cathode side,three anhydrides can suppress the formation of hydrogen fluoride from electrolyte oxidation decomposition,but SA behaves ***,MA shows adverse effects on the interface stability of li anode and NCM811 cathode,which originates from its high *** the acidity of MA can be mitigated by substituting a methyl for one H atom at its C=C bond,the substituent CA cannot compete with SA in cyclic stability improvement of the cell,because the SEI resulting from CA is not as robust as that from SA,which is related to the binding energy of the SEI *** understanding reveals the importance of the electrolyte acidity on the Ni-rich cathode and the robustness of the SEI on li anode,which is helpful for rationally designing new electrolyte additives to further improve the cyclic stability of high-energydensity Ni-rich/li batteries.

关键词： lithium-metal battery Ni-rich cathode Electrolyte additives Succinic Anhydride Cyclic stability

Recent research progresses in ether-and ester-based electrolytes for sodium-ion batteries

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InfoMat 2019年第3期1卷 376-389页

作者： Zeheng lin Qingbing Xia Wanlin Wang weishan li Shulei Chou Institute for Superconducting and Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongNorth WollongongNew South WalesAustralia School of Chemistry and Environment South China Normal UniversityGuangzhouChina National and Local Joint Engineering Research Center of MPTES in High Energy and Safety liBs Engineering Research Center of MTEES(Ministry of Education)Key Laboratory of ETESPG(GHEI)South China Normal UniversityGuangzhouChina

Owing to the natural abundance and low cost of sodium resources,sodium-ion batteries(SIBs)have drawn considerable attention for state-of-the-art power storage devices over the last few *** enable advanced SIBs with a brighter future,great effort has been made,not only through optimizing the electrode materials,but also with rationally designing various electrolyte *** the available electrolyte systems,organic electrolytes,especially those based on esters as well as ethers,are the most promising ones for practical application in the foreseeable future,due to their numerous inherent *** review is concerned with the recent research progresses on organic electrolytes for SIBs,focusing on etherbased and ester-based ones.

关键词： electrolyte additives organic electrolytes sodium salts sodium-ion batteries