The rapid improvement in the gel polymer electrolytes(GPEs)with high ionic conductivity brought it closer to practical applications in solid-state Li-metal batteries.The combination of solvent and polymer enables quas...The rapid improvement in the gel polymer electrolytes(GPEs)with high ionic conductivity brought it closer to practical applications in solid-state Li-metal batteries.The combination of solvent and polymer enables quasi-liquid fast ion transport in the GPEs.However,different ion transport capacity between solvent and polymer will cause local nonuniform Li+distribution,leading to severe dendrite growth.In addition,the poor thermal stability of the solvent also limits the operating-temperature window of the electrolytes.Optimizing the ion transport environment and enhancing the thermal stability are two major challenges that hinder the application of GPEs.Here,a strategy by introducing ion-conducting arrays(ICA)is created by vertical-aligned montmorillonite into GPE.Rapid ion transport on the ICA was demonstrated by 6Li solid-state nuclear magnetic resonance and synchrotron X-ray diffraction,combined with computer simulations to visualize the transport process.Compared with conventional randomly dispersed fillers,ICA provides continuous interfaces to regulate the ion transport environment and enhances the tolerance of GPEs to extreme temperatures.Therefore,GPE/ICA exhibits high room-temperature ionic conductivity(1.08 mS cm^(−1))and long-term stable Li deposition/stripping cycles(>1000 h).As a final proof,Li||GPE/ICA||LiFePO_(4) cells exhibit excellent cycle performance at wide temperature range(from 0 to 60°C),which shows a promising path toward all-weather practical solid-state batteries.展开更多
The development of metallic lithium anode is restrained by lithium dendrite growth during cycling.The solid polymer electrolyte with high mechanical strength and lithium ion conductivity could be applied to inhibit li...The development of metallic lithium anode is restrained by lithium dendrite growth during cycling.The solid polymer electrolyte with high mechanical strength and lithium ion conductivity could be applied to inhibit lithium dendrite growth.To prepare the high-performance solid polymer electrolyte,the environment-friendly and cheap bacterial cellulose(BC)is used as filler incorporating with PEO-based electrolyte owing to good mechanical properties and Li salts compatibility.PEO/Li TFSI/BC composite solid polymer electrolytes(CSPE)are prepared easily by aqueous mixing in water.The lithium ion transference number of PEO/Li TFSI/BC CSPE is 0.57,which is higher than PEO/Li TFSI solid polymer electrolyte(SPE)(0.409).The PEO/Li TFSI/BC CSPE exhibits larger tensile strength(4.43 MPa)than PEO/Li TFSI SPE(1.34 MPa).The electrochemical window of composite electrolyte is widened 1.43 V by adding BC.Density functional theory calculations indicate that flex of PEO chains around Li atoms is suppressed,suggesting the enhanced lithium ion conductivity.Frontier molecular orbitals results suggest that an unfavorable intermolecular charge transfer lead to achieve higher potential for BC composite electrolyte.All solid-state Li metal battery with PEO/Li TFSI/BC CSPE delivers longer cycle life for 600 cycles than PEO/Li TFSI SPE battery(50 cycles).Li symmetrical battery using PEO/Li TFSI/BC CSPE could be stable for 1160 h.展开更多
Nano Research volume 13,pages2289–2298(2020)Cite this article 347 Accesses 1 Altmetric Metrics details Abstract Sodium-ion batteries(SIBs)are promising power sources due to the low cost and abundance of battery-grade...Nano Research volume 13,pages2289–2298(2020)Cite this article 347 Accesses 1 Altmetric Metrics details Abstract Sodium-ion batteries(SIBs)are promising power sources due to the low cost and abundance of battery-grade sodium resources,while practical SIBs suffer from intrinsically sluggish diffusion kinetics and severe volume changes of electrode materials.Metal-organic framework(MOFs)derived carbonaceous metal compound offer promising applications in electrode materials due to their tailorable composition,nanostructure,chemical and physical properties.Here,we fabricated hierarchical MOF-derived carbonaceous nickel selenides with bi-phase composition for enhanced sodium storage capability.As MOF formation time increases,the pyrolyzed and selenized products gradually transform from a single-phase Ni3Se4 into bi-phase NiSex then single-phase NiSe2,with concomitant morphological evolution from solid spheres into hierarchical urchin-like yolk-shell structures.As SIBs anodes,bi-phase NiSex@C/CNT-10h(10 h of hydrothermal synthesis time)exhibits a high specific capacity of 387.1 mAh/g at 0.1 A/g,long cycling stability of 306.3 mAh/g at a moderately high current density of 1 A/g after 2,000 cycles.Computational simulation further proves the lattice mismatch at the phase boundary facilitates more interstitial space for sodium storage.Our understanding of the phase boundary engineering of transformed MOFs and their morphological evolution is conducive to fabricate novel composites/hybrids for applications in batteries,catalysis,sensors,and environmental remediation.展开更多
Highly stretchable and transparent ionic conducting materials have enabled new concepts of electronic devices denoted as iontronics,with a distinguishable working mechanism and performances from the conventional elect...Highly stretchable and transparent ionic conducting materials have enabled new concepts of electronic devices denoted as iontronics,with a distinguishable working mechanism and performances from the conventional electronics.However,the existing ionic conducting materials can hardly bear the humidity and temperature change of our daily life,which has greatly hindered the development and real-world application of iontronics.Herein,we design an ion gel possessing unique traits of hydrophobicity,humidity insensitivity,wide working temperature range(exceeding 100℃,and the range covered our daily life temperature),high conductivity(10^(-3)~10^(-5) S/cm),extensive stretchability,and high transparency,which is among the bestperforming ionic conductors ever developed for flexible iontronics.Several ion gel-based iontronics have been demonstrated,including large-deformation sensors,electroluminescent devices,and ionic cables,which can serve for a long time under harsh conditions.The designed material opens new potential for the real-world application progress of iontronics.展开更多
基金This work was supported partially by the National Natural Science Foundation of China(No.51973171)China Postdoctoral Science Foundation(No.2019M663687)+1 种基金National Natural Science Foundation of China(No.52105587),the Foundation of State Key Laboratory of Organic-Inorganic Composites(oic-202001003)the University Joint Project-Key Projects of Shaanxi Province(No.2021GXLH-Z-042).
文摘The rapid improvement in the gel polymer electrolytes(GPEs)with high ionic conductivity brought it closer to practical applications in solid-state Li-metal batteries.The combination of solvent and polymer enables quasi-liquid fast ion transport in the GPEs.However,different ion transport capacity between solvent and polymer will cause local nonuniform Li+distribution,leading to severe dendrite growth.In addition,the poor thermal stability of the solvent also limits the operating-temperature window of the electrolytes.Optimizing the ion transport environment and enhancing the thermal stability are two major challenges that hinder the application of GPEs.Here,a strategy by introducing ion-conducting arrays(ICA)is created by vertical-aligned montmorillonite into GPE.Rapid ion transport on the ICA was demonstrated by 6Li solid-state nuclear magnetic resonance and synchrotron X-ray diffraction,combined with computer simulations to visualize the transport process.Compared with conventional randomly dispersed fillers,ICA provides continuous interfaces to regulate the ion transport environment and enhances the tolerance of GPEs to extreme temperatures.Therefore,GPE/ICA exhibits high room-temperature ionic conductivity(1.08 mS cm^(−1))and long-term stable Li deposition/stripping cycles(>1000 h).As a final proof,Li||GPE/ICA||LiFePO_(4) cells exhibit excellent cycle performance at wide temperature range(from 0 to 60°C),which shows a promising path toward all-weather practical solid-state batteries.
基金supported partialy by the National Natural Science Foundation of China(No.51973171)Young Talent Support Plan of Xi’an Jiaotong University and Innovation Capability Support Program of Shaanxi(No.2018PT-28,2019PT-05)
文摘The development of metallic lithium anode is restrained by lithium dendrite growth during cycling.The solid polymer electrolyte with high mechanical strength and lithium ion conductivity could be applied to inhibit lithium dendrite growth.To prepare the high-performance solid polymer electrolyte,the environment-friendly and cheap bacterial cellulose(BC)is used as filler incorporating with PEO-based electrolyte owing to good mechanical properties and Li salts compatibility.PEO/Li TFSI/BC composite solid polymer electrolytes(CSPE)are prepared easily by aqueous mixing in water.The lithium ion transference number of PEO/Li TFSI/BC CSPE is 0.57,which is higher than PEO/Li TFSI solid polymer electrolyte(SPE)(0.409).The PEO/Li TFSI/BC CSPE exhibits larger tensile strength(4.43 MPa)than PEO/Li TFSI SPE(1.34 MPa).The electrochemical window of composite electrolyte is widened 1.43 V by adding BC.Density functional theory calculations indicate that flex of PEO chains around Li atoms is suppressed,suggesting the enhanced lithium ion conductivity.Frontier molecular orbitals results suggest that an unfavorable intermolecular charge transfer lead to achieve higher potential for BC composite electrolyte.All solid-state Li metal battery with PEO/Li TFSI/BC CSPE delivers longer cycle life for 600 cycles than PEO/Li TFSI SPE battery(50 cycles).Li symmetrical battery using PEO/Li TFSI/BC CSPE could be stable for 1160 h.
基金This work was financially supported by the National Natural Science Foundation of China(51773165,51973171)Innovation Capability Support Program of Shaanxi(2018PT-28,2019PT-05).
文摘锂硫电池因具有2600 Wh kg–1的高能量密度,而备受人们关注.但由于硫的负荷和利用率低,阻碍了硫的商品化.在此,本文设计了纤维素基石墨烯-碳复合气凝胶(CCA)自支撑电极来提高锂硫电池的性能. CCA具有低密度(0.018 g cm–3)、大比表面积(657.85 m2g–1)、高孔隙率(96%)、显著的电解质吸附(42.25倍)等独特的物理结构,有助于提高硫的质量负荷和利用率.与Al(约49%)相比, CCA表现出优良的硫利用效率(86%),在9.11 mgS负荷下可达到8.60 mAh cm–2的大面积容量,有助于实现锂硫电池的商业化进程.同时,由于其灵活性和对电响应信号的高灵敏度, CCA表现出优异的脉冲传感应用潜力.
基金supported partially by the National Natural Science Foundation of China (51973171, 51873170)the Young Talent Support Plan of Xi’an Jiaotong University。
基金This research was supported by the National Natural Science Foundation of China(No.51773165)Project of National Defense Science and Technology Innovation Special Zone(No.JZ-20171102)+3 种基金Shaanxi Post-doctoral Foundation(No.2016BSHYDZZ20)Key Laboratory Construction Program of Xi’an Municipal Bureau of Science and Technology(No.201805056ZD7CG40)Innovation Capability Support Program of Shaanxi(No.2018PT-28,2019PT-05)The numerical calculations in this paper have been done on the supercomputing system in the Supercomputing Center of Wuhan University.A.K.C.thanks the Ras al Khaimah Centre for Advanced Materials for financial support.J.H.thanks the financial support(No.DE190100803)。
文摘Nano Research volume 13,pages2289–2298(2020)Cite this article 347 Accesses 1 Altmetric Metrics details Abstract Sodium-ion batteries(SIBs)are promising power sources due to the low cost and abundance of battery-grade sodium resources,while practical SIBs suffer from intrinsically sluggish diffusion kinetics and severe volume changes of electrode materials.Metal-organic framework(MOFs)derived carbonaceous metal compound offer promising applications in electrode materials due to their tailorable composition,nanostructure,chemical and physical properties.Here,we fabricated hierarchical MOF-derived carbonaceous nickel selenides with bi-phase composition for enhanced sodium storage capability.As MOF formation time increases,the pyrolyzed and selenized products gradually transform from a single-phase Ni3Se4 into bi-phase NiSex then single-phase NiSe2,with concomitant morphological evolution from solid spheres into hierarchical urchin-like yolk-shell structures.As SIBs anodes,bi-phase NiSex@C/CNT-10h(10 h of hydrothermal synthesis time)exhibits a high specific capacity of 387.1 mAh/g at 0.1 A/g,long cycling stability of 306.3 mAh/g at a moderately high current density of 1 A/g after 2,000 cycles.Computational simulation further proves the lattice mismatch at the phase boundary facilitates more interstitial space for sodium storage.Our understanding of the phase boundary engineering of transformed MOFs and their morphological evolution is conducive to fabricate novel composites/hybrids for applications in batteries,catalysis,sensors,and environmental remediation.
基金This research was supported by the National Natural Science Foundation of China(Nos.51773165 and 11772249)the Fundamental Research Funds for the Central Universities(xjj2015119)the Young Talent Support Plan of Xi’an Jiaotong University。
文摘Highly stretchable and transparent ionic conducting materials have enabled new concepts of electronic devices denoted as iontronics,with a distinguishable working mechanism and performances from the conventional electronics.However,the existing ionic conducting materials can hardly bear the humidity and temperature change of our daily life,which has greatly hindered the development and real-world application of iontronics.Herein,we design an ion gel possessing unique traits of hydrophobicity,humidity insensitivity,wide working temperature range(exceeding 100℃,and the range covered our daily life temperature),high conductivity(10^(-3)~10^(-5) S/cm),extensive stretchability,and high transparency,which is among the bestperforming ionic conductors ever developed for flexible iontronics.Several ion gel-based iontronics have been demonstrated,including large-deformation sensors,electroluminescent devices,and ionic cables,which can serve for a long time under harsh conditions.The designed material opens new potential for the real-world application progress of iontronics.