Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving...Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.展开更多
Practical implementations of rechargeable lithium(Li)metal batteries have long been plagued by multiple problems of Li anode,such as Li dendrite growth,large volume change,low Coulombic efficiency.Here,we report a pro...Practical implementations of rechargeable lithium(Li)metal batteries have long been plagued by multiple problems of Li anode,such as Li dendrite growth,large volume change,low Coulombic efficiency.Here,we report a protein-enabled film that can provide effective protection for Li metal.The protective film with an integrated design of high flexibility,strong adhesion and high Li-ion transference number(0.80)is fabricated by incorporating denatured zein(corn protein)with polyethylene oxide(PEO)acting as an age nt for sustaining the denatured protein chains against refolding via the intermolecular interactions between them.Thus,a conformable zein-enabled protective film(zein@PEO)with simultaneous en hancement in flexibility,modulus and adhesion strength is gen erated to offer both functi ons of self-adapting and anion-anchoring abilities.The results show that the zein@PEO film is able to accommodate the volume change,reduce the side reactions,and homogenize the ion deposition.Benefiting from these significant properties/fu nctions,the Li/Cu cell with the zein@PEO film delivers prolonged cycle life for over 500 hours with stable performance.Paired with LiMn_(2)O_(4) cathode,the capacity,cycle stability and rate performance of the cell are remarkably improved as well,demonstrati ng the effectiveness in stabilizing Li metal batteries.展开更多
Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundame...Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.展开更多
All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional l...All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.展开更多
Objective This study examines the sequential mediating roles of body pain and self-reported health in the association between sleep duration and self-reported life satisfaction among elderly Chinese adults.Methods Dat...Objective This study examines the sequential mediating roles of body pain and self-reported health in the association between sleep duration and self-reported life satisfaction among elderly Chinese adults.Methods Data from the fifth wave of the China Health and Retirement Longitudinal Survey(CHARLS)were used to analyse the relationships between sleep duration and body pain,self-reported health,and life satisfaction through logistic regression and Restricted Cubic Spline(RCS)analyses.The sequential mediation effects of body pain and self-reported health status were examined via chain mediation analysis.Results Logistic regression analysis showed that sleeping fewer than 6 hours or 6-7 hours was linked to higher risks of body pain,poor health,and dissatisfaction with life compared to sleeping 7-8 hours(all P<0.05).Additionally,those sleeping more than 9 hours also had increased risks of poor health and dissatisfaction with life compared to those sleeping 7-8 hours(all P<0.05).Chain mediation analysis showed that body pain and self-reported health status sequentially mediated 46.15%of the association between sleep duration and life satisfaction.Conclusion Body pain and self-reported health may shape the relationship between sleep duration and life satisfaction in elderly Chinese adults.展开更多
Polymer electrolytes are attractive materials towards achieving safe,flexible and high-performance energy storage devices( ESDs) such as lithium ion batteries( LIBs). Conventional polymer electrolytes are confronted w...Polymer electrolytes are attractive materials towards achieving safe,flexible and high-performance energy storage devices( ESDs) such as lithium ion batteries( LIBs). Conventional polymer electrolytes are confronted with big challenges to achieve high ionic conductivity,good mechanical properties,excellent biocompatibility and environmental friendliness. In this context,natural polymeric materials have appealing merits of multi-functionality,ease of accessibility,good mechanical strength,etc. making them promising candidates to substitute conventional polymer electrolytes. Recently,the rational design and fabrication of advanced natural bio-based polymer electrolytes have made important progresses. In this review, we summarize recent developments in terms of polymer electrolytes using natural polymers for several application purposes. This review also involves the merits and demerits of the different natural polymers that have been investigated thus far. The insights on state-of-the-art for natural polymer electrolytes and possible solutions for further improvement of them are discussed as well in this review.展开更多
The microstructures on electrode level are crucial for battery performance, but the ambiguous understanding of both electrode microstructures and their structuring process causes critical challenges in controlling and...The microstructures on electrode level are crucial for battery performance, but the ambiguous understanding of both electrode microstructures and their structuring process causes critical challenges in controlling and evaluating the electrode quality during fabrication. In this review, analogous to the cell microenvironment well-known in biology, we introduce the concept of ‘‘active material microenvironment”(ME@AM)that is built by the ion/electron transport structures surrounding the AMs, for better understanding the significance of the electrode microstructures. Further, the scientific significance of electrode processing for electrode quality control is highlighted by its strong links to the structuring and quality control of ME@AM. Meanwhile, the roles of electrode rheology in both electrode structuring and structural characterizations involved in the entire electrode manufacturing process(i.e., slurry preparation, coating/printing/extrusion, drying and calendering) are specifically detailed. The advantages of electrode rheology testing on in-situ characterizations of the electrode qualities/structures are emphasized. This review provides a glimpse of the electrode rheology engaged in electrode manufacturing process and new insights into the understanding and effective regulation of electrode microstructures for future high-performance batteries.展开更多
The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and...The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and beyond.Herein,by learning from the pencil-writing process,a facile solid-ink rubbing technology(SIR-tech)is invented to address the above challenge.The solid-ink is exampled by rational combination of liquid metal and graphite particles.By harnessing the synergistic effects between rubbing and adhesion,controllable metallic skin is successfully formed onto metals,woods,ceramics,and plastics without limitation in size and shape.Moreover,outperforming pure liquid-metal coating,the composite metallic skin by SIR-tech is very robust due to the self-lamination of graphite nanoplate exfoliated by liquid-metal rubbing.The critical factors controlling the structures-properties of the composite metallic skin have been systematically investigated as well.For applications,the SIR-tech is demonstrated to fabricate high-performance composite current collectors for next-generation batteries without traditional metal foils.Meanwhile,advanced skin-electrodes are further demonstrated for stable triboelectricity generation even under temperature fluctuation from-196 to 120℃.This facile and highly-flexible SIR-tech may work as a powerful platform for the studies on functional coatings by liquid metals and beyond.展开更多
Development of ＂green＂ multi-functional air filters with features such as excellent filtration efficiency eco-friendliness, and environmental stability are critically required to address the increasing concerns of p...Development of ＂green＂ multi-functional air filters with features such as excellent filtration efficiency eco-friendliness, and environmental stability are critically required to address the increasing concerns of polluted air. Natural proteins, such as soy protein and gelatin, are attractive candidates as multi-functional air-filtration materials owing to the rich functional groups; however, these bio-materials are vulnerable to moisture, which limits their broad application in practice. In this work, a hydrophobic protein of zein derived from abundant corn is modified for the first time to produce high-performance nanofilters via electrospinning. The zein nanofabrics are fabricated with the aid of a non-toxic solvent and co-electrospinning agent, poly（ethylene oxide）. The results reveal that the zein-based nanofabrics show high efficiency for the simultaneous removal of particulate matters of different sizes ranging from 0.1 to 10 btm （〉 99.5%） and certain gaseous toxic chemicals （〉 70%）. In addition, the zein nanofabrics show excellent moisture-resistance and good adhesion to the cellulose paper towel used as the air-filter substrate. This study demonstrates that nanofabrics based on hydrophobic natural proteins such as zein are promising materials for developing multi-functional ＂green＂ air filters.展开更多
基金the financial support from the National Natural Science Foundation of China(52203123 and 52473248)State Key Laboratory of Polymer Materials Engineering(sklpme2024-2-04)+1 种基金the Fundamental Research Funds for the Central Universitiessponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.
基金supported by NSF CBET 1929236the support on microscopy characterizations from the Franceschi Microscopy & Imaging Center at Washington State University.
文摘Practical implementations of rechargeable lithium(Li)metal batteries have long been plagued by multiple problems of Li anode,such as Li dendrite growth,large volume change,low Coulombic efficiency.Here,we report a protein-enabled film that can provide effective protection for Li metal.The protective film with an integrated design of high flexibility,strong adhesion and high Li-ion transference number(0.80)is fabricated by incorporating denatured zein(corn protein)with polyethylene oxide(PEO)acting as an age nt for sustaining the denatured protein chains against refolding via the intermolecular interactions between them.Thus,a conformable zein-enabled protective film(zein@PEO)with simultaneous en hancement in flexibility,modulus and adhesion strength is gen erated to offer both functi ons of self-adapting and anion-anchoring abilities.The results show that the zein@PEO film is able to accommodate the volume change,reduce the side reactions,and homogenize the ion deposition.Benefiting from these significant properties/fu nctions,the Li/Cu cell with the zein@PEO film delivers prolonged cycle life for over 500 hours with stable performance.Paired with LiMn_(2)O_(4) cathode,the capacity,cycle stability and rate performance of the cell are remarkably improved as well,demonstrati ng the effectiveness in stabilizing Li metal batteries.
基金financial support from the National Natural Science Foundation of China(52203123)the Sichuan Science and Technology Program(2023NSFSC0991)+2 种基金the State Key Laboratory of Polymer Materials Engineering(sklpme 2023-1-05 and sklpme 2024-2-04)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.
基金National Natural Science Foundation of China (52203123)Sichuan Science and Technology Program (2023NSFSC0991)+2 种基金State Key Laboratory of Polymer Materials Engineering (sklpme-2023-1-05 and sklpme-2024-2-04)Fundamental Research Funds for the Central UniversitiesThis research was also partially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
基金supported by This work was supported by the Ministry of Science and Technology of the People’s Republic of China(STI2030-Major Projects2021ZD0201900)。
文摘Objective This study examines the sequential mediating roles of body pain and self-reported health in the association between sleep duration and self-reported life satisfaction among elderly Chinese adults.Methods Data from the fifth wave of the China Health and Retirement Longitudinal Survey(CHARLS)were used to analyse the relationships between sleep duration and body pain,self-reported health,and life satisfaction through logistic regression and Restricted Cubic Spline(RCS)analyses.The sequential mediation effects of body pain and self-reported health status were examined via chain mediation analysis.Results Logistic regression analysis showed that sleeping fewer than 6 hours or 6-7 hours was linked to higher risks of body pain,poor health,and dissatisfaction with life compared to sleeping 7-8 hours(all P<0.05).Additionally,those sleeping more than 9 hours also had increased risks of poor health and dissatisfaction with life compared to those sleeping 7-8 hours(all P<0.05).Chain mediation analysis showed that body pain and self-reported health status sequentially mediated 46.15%of the association between sleep duration and life satisfaction.Conclusion Body pain and self-reported health may shape the relationship between sleep duration and life satisfaction in elderly Chinese adults.
基金Sponsored by the USDA NIFA(Grant o.2015-67021-22911)the National Science Foundation CMMI(Grant No.1463616)
文摘Polymer electrolytes are attractive materials towards achieving safe,flexible and high-performance energy storage devices( ESDs) such as lithium ion batteries( LIBs). Conventional polymer electrolytes are confronted with big challenges to achieve high ionic conductivity,good mechanical properties,excellent biocompatibility and environmental friendliness. In this context,natural polymeric materials have appealing merits of multi-functionality,ease of accessibility,good mechanical strength,etc. making them promising candidates to substitute conventional polymer electrolytes. Recently,the rational design and fabrication of advanced natural bio-based polymer electrolytes have made important progresses. In this review, we summarize recent developments in terms of polymer electrolytes using natural polymers for several application purposes. This review also involves the merits and demerits of the different natural polymers that have been investigated thus far. The insights on state-of-the-art for natural polymer electrolytes and possible solutions for further improvement of them are discussed as well in this review.
基金the financial support from the National Natural Science Foundation of China and the start-up projectthe Sichuan-University-Dazhou Joint project(00309053A2037)+1 种基金the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘The microstructures on electrode level are crucial for battery performance, but the ambiguous understanding of both electrode microstructures and their structuring process causes critical challenges in controlling and evaluating the electrode quality during fabrication. In this review, analogous to the cell microenvironment well-known in biology, we introduce the concept of ‘‘active material microenvironment”(ME@AM)that is built by the ion/electron transport structures surrounding the AMs, for better understanding the significance of the electrode microstructures. Further, the scientific significance of electrode processing for electrode quality control is highlighted by its strong links to the structuring and quality control of ME@AM. Meanwhile, the roles of electrode rheology in both electrode structuring and structural characterizations involved in the entire electrode manufacturing process(i.e., slurry preparation, coating/printing/extrusion, drying and calendering) are specifically detailed. The advantages of electrode rheology testing on in-situ characterizations of the electrode qualities/structures are emphasized. This review provides a glimpse of the electrode rheology engaged in electrode manufacturing process and new insights into the understanding and effective regulation of electrode microstructures for future high-performance batteries.
基金the financial support from the National Natural Science Foundation of China (52125301 and 52203123)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘The development of a durable metallic coating on diverse substrates is both intriguing and challenging,particularly in the research of metal-conductive materials for applications such as batteries,soft electronics,and beyond.Herein,by learning from the pencil-writing process,a facile solid-ink rubbing technology(SIR-tech)is invented to address the above challenge.The solid-ink is exampled by rational combination of liquid metal and graphite particles.By harnessing the synergistic effects between rubbing and adhesion,controllable metallic skin is successfully formed onto metals,woods,ceramics,and plastics without limitation in size and shape.Moreover,outperforming pure liquid-metal coating,the composite metallic skin by SIR-tech is very robust due to the self-lamination of graphite nanoplate exfoliated by liquid-metal rubbing.The critical factors controlling the structures-properties of the composite metallic skin have been systematically investigated as well.For applications,the SIR-tech is demonstrated to fabricate high-performance composite current collectors for next-generation batteries without traditional metal foils.Meanwhile,advanced skin-electrodes are further demonstrated for stable triboelectricity generation even under temperature fluctuation from-196 to 120℃.This facile and highly-flexible SIR-tech may work as a powerful platform for the studies on functional coatings by liquid metals and beyond.
文摘Development of ＂green＂ multi-functional air filters with features such as excellent filtration efficiency eco-friendliness, and environmental stability are critically required to address the increasing concerns of polluted air. Natural proteins, such as soy protein and gelatin, are attractive candidates as multi-functional air-filtration materials owing to the rich functional groups; however, these bio-materials are vulnerable to moisture, which limits their broad application in practice. In this work, a hydrophobic protein of zein derived from abundant corn is modified for the first time to produce high-performance nanofilters via electrospinning. The zein nanofabrics are fabricated with the aid of a non-toxic solvent and co-electrospinning agent, poly（ethylene oxide）. The results reveal that the zein-based nanofabrics show high efficiency for the simultaneous removal of particulate matters of different sizes ranging from 0.1 to 10 btm （〉 99.5%） and certain gaseous toxic chemicals （〉 70%）. In addition, the zein nanofabrics show excellent moisture-resistance and good adhesion to the cellulose paper towel used as the air-filter substrate. This study demonstrates that nanofabrics based on hydrophobic natural proteins such as zein are promising materials for developing multi-functional ＂green＂ air filters.
