The polymer-ceramic composite electrolyte is considered as one of promising electrolytes for solid-state battery.However,in previous research,ceramic particles are usually dispersed in polymer matrix and could not for...The polymer-ceramic composite electrolyte is considered as one of promising electrolytes for solid-state battery.However,in previous research,ceramic particles are usually dispersed in polymer matrix and could not form continuous Li+conductive channels.The agglomeration of ceramic particles could also lead to low ionic conductivity and poor interfacial electrode/electrolyte contact.In this paper,self-supported porous Li_(6.4)La_(3) Zr_(1.4)Ta_(0.6)O_(12)(LLZTO) electrolyte is synthesized by gelcasting process,which possesses three-dimensional(3D) interconnected pore channels and relatively high strength.The 1,3-dioxolane(DOL) could penetrate into the porous LLZTO framework for its excellent fluidity.The subsequent in situ polymerization process by thermal treatment could completely fill the internal pores and improve the interfacial contact with electrode.The resulting 3D composite electrolyte with dual continuous Li+transport channels in ceramic and polymer components exhibits high ionic conductivity of 2.8 × 10^(-4) S·cm^(-1) at room temperature and low Li/electrolyte interfacial resistance of 94 Ω·cm^(2) at 40 ℃.The corresponding Li/Li symmetric cell delivers stable voltage profiles for over 600 h under 0.1 and 0.2 mA·cm^(-2).The solid-state Li/LiFePO_(4) battery shows superior rate and cycling performance under 0.1 C and 0.2 C.This work guides the preparation of composite electrolyte with dual continuous Li+conductive paths as well as high ceramic ratio and interface modification strategy for solid-state Li metal battery.展开更多
1,3-dioxolane （DOL） was originally used to pretreat a lithium metal electrode to improve its interfacial characteristics. Electrochemical impedance spectra （EIS） meastLrements revealed that, after the DOL pretreat...1,3-dioxolane （DOL） was originally used to pretreat a lithium metal electrode to improve its interfacial characteristics. Electrochemical impedance spectra （EIS） meastLrements revealed that, after the DOL pretreatment, the lithium electrode had better interfacial stability during immersion in electrolyte and as repeated charge/discharge cycles. It was proved by SEaM that the pretreated one has smoother morphology and less dendrite after repeated charge/discharge cycles. Consequentially, benefiting from the better interface characteristics of the lithium electrode, the rechargeable lithium cell with a DOL-pretreated lithium anode had the obviously enhanced discharging performance and better cyclability.展开更多
Nine title compounds were synthesized. Their strucures were identified by means of IR, EA, 1H NMR and MS. The results from the primary biological test show that all the compounds have some activitiies of fungicide and...Nine title compounds were synthesized. Their strucures were identified by means of IR, EA, 1H NMR and MS. The results from the primary biological test show that all the compounds have some activitiies of fungicide and plant growth regulator. When R group is 2,4 Cl 2C 6H 3, compound 2 or compound 4 shows better biological activities.展开更多
1,3-dioxolane (DOL) is originally used to pretreat the lithium metal electrode in order to passivate lithium metal and improve its interface stability. Through electrochemical impedance spectra (EIS) and cathodic pola...1,3-dioxolane (DOL) is originally used to pretreat the lithium metal electrode in order to passivate lithium metal and improve its interface stability. Through electrochemical impedance spectra (EIS) and cathodic polarization measurements of pretreated and untreated electrodes, it was found that 1,3-dioxolane could form a stable passivating film on the surface of lithium electrode. And such film could enhance effectively the interfacial stability of lithium electrode, without depressing its kinetics characteristic. Consequentially, further tests of the cell-performance during repeated charge/discharge cycles showed that the cell with DOL pretreated anode had better discharging performance and longer cycle life because of the passivating and protective effects of 1,3-dioxolane pretreatment on lithium electrode.展开更多
Novel 1,3-dioxolane C-nucleoside analogues of tiazofurin 2-(2-hydroxymethyl-1,3-dioxolan-4-yl)-1,3-thiazole- 4-carboxamide as well as N-nucleoside analogues of substituted imidazoles 1-(2-hydroxymethyl-1,3-dioxolan- 4...Novel 1,3-dioxolane C-nucleoside analogues of tiazofurin 2-(2-hydroxymethyl-1,3-dioxolan-4-yl)-1,3-thiazole- 4-carboxamide as well as N-nucleoside analogues of substituted imidazoles 1-(2-hydroxymethyl-1,3-dioxolan- 4-yl)-4-nitroimidazole and 1-(2-hydroxymethyl-1,3-dioxolan-4-yl)-4,5-dicyanoimidazole were synthesized from methyl acrylate through a multistep procedure. Their structures were confirmed by IR, 1H NMR, 13C NMR spectra and elemental analysis.展开更多
Gel-based polymer electrolytes are limited by the polarity of the residual solvent,which restricts the coupling-breaking behaviour during Li^(+)conduction,resulting in the Li^(+)transport kinetics being greatly affect...Gel-based polymer electrolytes are limited by the polarity of the residual solvent,which restricts the coupling-breaking behaviour during Li^(+)conduction,resulting in the Li^(+)transport kinetics being greatly affected.Here,we designed anion competitive gel polymer electrolyte(ACPE)by introducing lithium difluoro(oxalato)borate(LiDFOB)anion into the 1,3-dioxolane(DOL)in situ polymerisation system.ACPE enhances the ionic dipole interaction between Li^(+)and the solvent molecules and synergizes with Li^(+)across the solvation site of the polymer ethylene oxide(EO)unit,combination that greatly improves the Li^(+)transport efficiency.As a result,ACPE exhibits 1.12 mS cm^(−1)ionic conductivity and 0.75 Li^(+)transfer number at room temperature.Additionally,this intra-polymer solvation sheath allows preferential desolvation of DFOB−,which contributes to the formation of kinetically stable anion-derived interphase and effectively mitigates side reactions.Our results demonstrate that the assembled Li||NCM622 solid-state battery exhibits lifespan of over 300 cycles with average Coulombic efficiency of 98.8%and capacity retention of 80.3%.This study introduces a novel approach for ion migration and interface design,paving the way for high-safety and high-energy-density batteries.展开更多
Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery asse...Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery assembly process are still the main challenges to hurdle the commercialization of SSLB.As the main component of SSLB,poly(1,3-dioxolane)(PDOL)-based solid polymer electrolytes polymerized in-situ are becoming a promising candidate solid elec-trolyte,for their high ion conductivity at room temperature,good battery elec-trochemical performances,and simple assembly process.This review analyzes opportunities and challenges of PDOL electrolytes toward practical application for polymer SSLB.The focuses include exploring the polymerization mechanism of DOL,the performance of PDOL composite electrolytes,and the application of PDOL.Furthermore,we provide a perspective on future research directions that need to be emphasized for commercialization of PDOL-based electrolytes in SSLB.The exploration of these schemes facilitates a comprehensive and profound understanding of PDOL-based polymer electrolyte and provides new research ideas to boost them toward practical application in solid-state batteries.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.52173257 and 51872159)。
文摘The polymer-ceramic composite electrolyte is considered as one of promising electrolytes for solid-state battery.However,in previous research,ceramic particles are usually dispersed in polymer matrix and could not form continuous Li+conductive channels.The agglomeration of ceramic particles could also lead to low ionic conductivity and poor interfacial electrode/electrolyte contact.In this paper,self-supported porous Li_(6.4)La_(3) Zr_(1.4)Ta_(0.6)O_(12)(LLZTO) electrolyte is synthesized by gelcasting process,which possesses three-dimensional(3D) interconnected pore channels and relatively high strength.The 1,3-dioxolane(DOL) could penetrate into the porous LLZTO framework for its excellent fluidity.The subsequent in situ polymerization process by thermal treatment could completely fill the internal pores and improve the interfacial contact with electrode.The resulting 3D composite electrolyte with dual continuous Li+transport channels in ceramic and polymer components exhibits high ionic conductivity of 2.8 × 10^(-4) S·cm^(-1) at room temperature and low Li/electrolyte interfacial resistance of 94 Ω·cm^(2) at 40 ℃.The corresponding Li/Li symmetric cell delivers stable voltage profiles for over 600 h under 0.1 and 0.2 mA·cm^(-2).The solid-state Li/LiFePO_(4) battery shows superior rate and cycling performance under 0.1 C and 0.2 C.This work guides the preparation of composite electrolyte with dual continuous Li+conductive paths as well as high ceramic ratio and interface modification strategy for solid-state Li metal battery.
基金This project was financially supported by the Foundation of Science-Technology Research Program of Guangdong Prov-ince, China (No. 2003C105006).
文摘1,3-dioxolane （DOL） was originally used to pretreat a lithium metal electrode to improve its interfacial characteristics. Electrochemical impedance spectra （EIS） meastLrements revealed that, after the DOL pretreatment, the lithium electrode had better interfacial stability during immersion in electrolyte and as repeated charge/discharge cycles. It was proved by SEaM that the pretreated one has smoother morphology and less dendrite after repeated charge/discharge cycles. Consequentially, benefiting from the better interface characteristics of the lithium electrode, the rechargeable lithium cell with a DOL-pretreated lithium anode had the obviously enhanced discharging performance and better cyclability.
基金Supported by the Natural Science Foudation of Shandong Province(No.Q 99B16 ) and the National Natural ScienceFoundation of China(No.2 0 0 75 0 13)
文摘Nine title compounds were synthesized. Their strucures were identified by means of IR, EA, 1H NMR and MS. The results from the primary biological test show that all the compounds have some activitiies of fungicide and plant growth regulator. When R group is 2,4 Cl 2C 6H 3, compound 2 or compound 4 shows better biological activities.
文摘1,3-dioxolane (DOL) is originally used to pretreat the lithium metal electrode in order to passivate lithium metal and improve its interface stability. Through electrochemical impedance spectra (EIS) and cathodic polarization measurements of pretreated and untreated electrodes, it was found that 1,3-dioxolane could form a stable passivating film on the surface of lithium electrode. And such film could enhance effectively the interfacial stability of lithium electrode, without depressing its kinetics characteristic. Consequentially, further tests of the cell-performance during repeated charge/discharge cycles showed that the cell with DOL pretreated anode had better discharging performance and longer cycle life because of the passivating and protective effects of 1,3-dioxolane pretreatment on lithium electrode.
基金Project supported by the National Natural Science Foundation of China (No. 21172049).
文摘Novel 1,3-dioxolane C-nucleoside analogues of tiazofurin 2-(2-hydroxymethyl-1,3-dioxolan-4-yl)-1,3-thiazole- 4-carboxamide as well as N-nucleoside analogues of substituted imidazoles 1-(2-hydroxymethyl-1,3-dioxolan- 4-yl)-4-nitroimidazole and 1-(2-hydroxymethyl-1,3-dioxolan-4-yl)-4,5-dicyanoimidazole were synthesized from methyl acrylate through a multistep procedure. Their structures were confirmed by IR, 1H NMR, 13C NMR spectra and elemental analysis.
基金supported by the National Natural Science Foundation of China(22008053,52002111)the Natural Science Foundation of Hebei Province(B2021208061,B2022208006,B2023208014)the Beijing Natural Science Foundation(Z200011).
文摘Gel-based polymer electrolytes are limited by the polarity of the residual solvent,which restricts the coupling-breaking behaviour during Li^(+)conduction,resulting in the Li^(+)transport kinetics being greatly affected.Here,we designed anion competitive gel polymer electrolyte(ACPE)by introducing lithium difluoro(oxalato)borate(LiDFOB)anion into the 1,3-dioxolane(DOL)in situ polymerisation system.ACPE enhances the ionic dipole interaction between Li^(+)and the solvent molecules and synergizes with Li^(+)across the solvation site of the polymer ethylene oxide(EO)unit,combination that greatly improves the Li^(+)transport efficiency.As a result,ACPE exhibits 1.12 mS cm^(−1)ionic conductivity and 0.75 Li^(+)transfer number at room temperature.Additionally,this intra-polymer solvation sheath allows preferential desolvation of DFOB−,which contributes to the formation of kinetically stable anion-derived interphase and effectively mitigates side reactions.Our results demonstrate that the assembled Li||NCM622 solid-state battery exhibits lifespan of over 300 cycles with average Coulombic efficiency of 98.8%and capacity retention of 80.3%.This study introduces a novel approach for ion migration and interface design,paving the way for high-safety and high-energy-density batteries.
基金We express our sincere appreciation to the National Natural Science Foundation of China(No.51474113(M.Jing),22279070[L.Wang]and U21A20170[X.He])the Ministry of Science and Technology of China(No.2019YFA0705703[L.Wang]).And we would like to thank the“Explorer 100”cluster system of Tsinghua National Laboratory for Information Science and Technology for facility support.
文摘Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery assembly process are still the main challenges to hurdle the commercialization of SSLB.As the main component of SSLB,poly(1,3-dioxolane)(PDOL)-based solid polymer electrolytes polymerized in-situ are becoming a promising candidate solid elec-trolyte,for their high ion conductivity at room temperature,good battery elec-trochemical performances,and simple assembly process.This review analyzes opportunities and challenges of PDOL electrolytes toward practical application for polymer SSLB.The focuses include exploring the polymerization mechanism of DOL,the performance of PDOL composite electrolytes,and the application of PDOL.Furthermore,we provide a perspective on future research directions that need to be emphasized for commercialization of PDOL-based electrolytes in SSLB.The exploration of these schemes facilitates a comprehensive and profound understanding of PDOL-based polymer electrolyte and provides new research ideas to boost them toward practical application in solid-state batteries.
