In lithium-ion batteries(LIBs),separators play a vital role in lithium-ion(Li+)transport,and thus affect rate performance,battery life,and safety.Here,a new kind of multifunctional copolymer poly(acrylonitrile-co-lith...In lithium-ion batteries(LIBs),separators play a vital role in lithium-ion(Li+)transport,and thus affect rate performance,battery life,and safety.Here,a new kind of multifunctional copolymer poly(acrylonitrile-co-lithium acrylate-co-butyl acrylate)(PAAB-Li)is synthesized through soap-free emulsion polymerization,and is used to form homogeneous-covered separator based on PP matrix by a simple dip-annealing process.Compared to the bare PP separator,the modified separators with PAAB-Li enable higher ionic conductivity,higher lithium ion transference number(increased from 0.360 to 0.525),and lower interface impedance(reduced from 155Ω to 34Ω).It has been indicated that PAAB-Li functional layer significantly promotes the fast transport of Li+and improves the compatibility of the separator/electrolyte-electrode interface.The LiCo02/graphite cells with the PAAB-Li-assisted separator demonstrate excellent cycle stability and rate performance.In addition,the Li symmetric cells with the modified separator stably cycle over 800 h,indicating the functional layer effectively suppresses the lithium dendrite growth.This facile strategy can be easily applied to LIBs requiring high safety and even be scalable to Li metal batteries.Moreover,the possible mechanism of the PAAB-Li functional layer promoting fast and uniform Li+transport is discussed in this paper.展开更多
An overview of ion transport in lithium-ion inorganic solid state electrolytes is presented, aimed at exploring and de signing better electrolyte materials. Ionic conductivity is one of the most important indices of t...An overview of ion transport in lithium-ion inorganic solid state electrolytes is presented, aimed at exploring and de signing better electrolyte materials. Ionic conductivity is one of the most important indices of the performance of inorganic solid state electrolytes. The general definition of solid state electrolytes is presented in terms of their role in a working cell （to convey ions while isolate electrons）, and the history of solid electrolyte development is briefly summarized. Ways of using the available theoretical models and experimental methods to characterize lithium-ion transport in solid state elec- trolytes are systematically introduced. Then the various factors that affect ionic conductivity are itemized, including mainly structural disorder, composite materials and interface effects between a solid electrolyte and an electrode. Finally, strategies for future material systems, for synthesis and characterization methods, and for theory and calculation are proposed, aiming to help accelerate the design and development of new solid electrolytes.展开更多
Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generati...Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generation solid-state battery (SSB) because of its high specific capacity and low cost.High energy density and safe Si-based SSB,however,is plagued by large volume change that leads to poor mechanical stability and slow lithium ions transportation at the multiple interfaces between Si and SSE.Herein,we designed a self-integrated and monolithic Si/two dimensional layered T_(3)C_(2)T_(x)(MXene,T_(x) stands for terminal functional groups) electrode architecture with interfacial nitrogen engineering.During a heat treatment process,the polyacrylonitrile not only converts into amorphous carbon (a-C) that shells Si but also forms robust interfacial nitrogen chemical bonds that anchors Si and MXene.During repeated lithiation and delithiation processes,the robust interfacial engineered Si/MXene configuration enhances the mechanical adhesion between Si and MXene that improves the structure stability but also contributes to form stable solid-electrolyte interphase (SEI).In addition,the N-MXene provides fast lithium ions transportation pathways.Consequently,the Si/MXene with interfacial nitrogen engineering (denoted as Si-N-MXene) deliveres high-rate performance with a specific capacity of 1498 m Ah g^(-1) at a high current of 6.4 A g^(-1).A Si-N-MXene/NMC full cell exhibited a capacity retention of 80.5%after 200 cycles.The Si-N-MXene electrode is also applied to SSB and shows a relative stable cycling over 100 cycles,demonstrating the versatility of this concept.展开更多
As the key component of electrochemical energy storage devices, an electrode with superior ions transport pores is the important premise for high electrochemical performance. In this paper, we developed a unique solut...As the key component of electrochemical energy storage devices, an electrode with superior ions transport pores is the important premise for high electrochemical performance. In this paper, we developed a unique solution process to prepare freestanding TiO_2/graphene hydrogel electrode with tunable density and porous structures. By incorporating room temperature ionic liquids（RTILs）, even upon drying, the non-volatile RTILs that remained in the gel film would preserve the efficient ion transport channels and prevent the electrode from closely stacking, to develop dense yet porous structures. As a result, the dense TiO_2/graphene gel film as an electrode for lithium ion battery displayed a good gravimetric electrochemical performance and more importantly a high volumetric performance.展开更多
基金supported by the National 863 Program of China(No.2012AA03A602)National Key R&D Program of China(No.2017YFE0114100)+1 种基金Science and Technology Project of Guangdong Province of China(No.2019 ST115)the National Natural Science Foundation of China(No.21805240).
文摘In lithium-ion batteries(LIBs),separators play a vital role in lithium-ion(Li+)transport,and thus affect rate performance,battery life,and safety.Here,a new kind of multifunctional copolymer poly(acrylonitrile-co-lithium acrylate-co-butyl acrylate)(PAAB-Li)is synthesized through soap-free emulsion polymerization,and is used to form homogeneous-covered separator based on PP matrix by a simple dip-annealing process.Compared to the bare PP separator,the modified separators with PAAB-Li enable higher ionic conductivity,higher lithium ion transference number(increased from 0.360 to 0.525),and lower interface impedance(reduced from 155Ω to 34Ω).It has been indicated that PAAB-Li functional layer significantly promotes the fast transport of Li+and improves the compatibility of the separator/electrolyte-electrode interface.The LiCo02/graphite cells with the PAAB-Li-assisted separator demonstrate excellent cycle stability and rate performance.In addition,the Li symmetric cells with the modified separator stably cycle over 800 h,indicating the functional layer effectively suppresses the lithium dendrite growth.This facile strategy can be easily applied to LIBs requiring high safety and even be scalable to Li metal batteries.Moreover,the possible mechanism of the PAAB-Li functional layer promoting fast and uniform Li+transport is discussed in this paper.
基金supported by the National Natural Science Foundation of China(Grant No.51372228)the Shanghai Pujiang Program,China(Grant No.14PJ1403900)the Shanghai Institute of Materials Genome from the Shanghai Municipal Science and Technology Commission,China(Grant No.14DZ2261200)
文摘An overview of ion transport in lithium-ion inorganic solid state electrolytes is presented, aimed at exploring and de signing better electrolyte materials. Ionic conductivity is one of the most important indices of the performance of inorganic solid state electrolytes. The general definition of solid state electrolytes is presented in terms of their role in a working cell （to convey ions while isolate electrons）, and the history of solid electrolyte development is briefly summarized. Ways of using the available theoretical models and experimental methods to characterize lithium-ion transport in solid state elec- trolytes are systematically introduced. Then the various factors that affect ionic conductivity are itemized, including mainly structural disorder, composite materials and interface effects between a solid electrolyte and an electrode. Finally, strategies for future material systems, for synthesis and characterization methods, and for theory and calculation are proposed, aiming to help accelerate the design and development of new solid electrolytes.
基金supported by the National Natural Science Foundation of China(51902165,12004145,52072323)the Natural Science Foundation of Jiangsu Province(BK20200800)+2 种基金the Natural Science Foundation of Jiangxi Province(20192ACBL20048)the Jiangxi Provincial Natural Science Foundation(20212BAB214032)the Nanjing Science&Technology Innovation Project for Personnel Studying Abroad。
文摘Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generation solid-state battery (SSB) because of its high specific capacity and low cost.High energy density and safe Si-based SSB,however,is plagued by large volume change that leads to poor mechanical stability and slow lithium ions transportation at the multiple interfaces between Si and SSE.Herein,we designed a self-integrated and monolithic Si/two dimensional layered T_(3)C_(2)T_(x)(MXene,T_(x) stands for terminal functional groups) electrode architecture with interfacial nitrogen engineering.During a heat treatment process,the polyacrylonitrile not only converts into amorphous carbon (a-C) that shells Si but also forms robust interfacial nitrogen chemical bonds that anchors Si and MXene.During repeated lithiation and delithiation processes,the robust interfacial engineered Si/MXene configuration enhances the mechanical adhesion between Si and MXene that improves the structure stability but also contributes to form stable solid-electrolyte interphase (SEI).In addition,the N-MXene provides fast lithium ions transportation pathways.Consequently,the Si/MXene with interfacial nitrogen engineering (denoted as Si-N-MXene) deliveres high-rate performance with a specific capacity of 1498 m Ah g^(-1) at a high current of 6.4 A g^(-1).A Si-N-MXene/NMC full cell exhibited a capacity retention of 80.5%after 200 cycles.The Si-N-MXene electrode is also applied to SSB and shows a relative stable cycling over 100 cycles,demonstrating the versatility of this concept.
基金supported by grants from the National Natural Science Foundation of China(21303251)Innovation Program of Shanghai Municipal Education Commission(16SG17)the Shenzhen Science and Technology Foundation(JCYJ201419122040621)
文摘As the key component of electrochemical energy storage devices, an electrode with superior ions transport pores is the important premise for high electrochemical performance. In this paper, we developed a unique solution process to prepare freestanding TiO_2/graphene hydrogel electrode with tunable density and porous structures. By incorporating room temperature ionic liquids（RTILs）, even upon drying, the non-volatile RTILs that remained in the gel film would preserve the efficient ion transport channels and prevent the electrode from closely stacking, to develop dense yet porous structures. As a result, the dense TiO_2/graphene gel film as an electrode for lithium ion battery displayed a good gravimetric electrochemical performance and more importantly a high volumetric performance.
