A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of th...A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.展开更多
Apatite-lanthanum silicate has attracted considerable interest in recent years due to its high oxide ion conductivity.In this paper,V-doped samples La10-xVx(SiO4) 6O3+x(0≤x≤1.5) were prepared by sol-gel method and t...Apatite-lanthanum silicate has attracted considerable interest in recent years due to its high oxide ion conductivity.In this paper,V-doped samples La10-xVx(SiO4) 6O3+x(0≤x≤1.5) were prepared by sol-gel method and the influences of V-dopant content on calcining temperature and conductivity were reported.The samples were characterized by thermal analysis(TG-DSC) ,X-ray diffraction(XRD) and scanning electron micrograph(SEM) . The apatite was obtained at 800°C,a relatively low temperature in comparison to 1500°C with the conventional solid-state method.The ceramic pellets sintered at 1200°C for 5 h showed a higher relative density than La9.33Si6O26 pellets sintered at 1400°C for 20 h.The conductivities of samples were measured by electrochemical impedance spectroscopy.The conductivity was improved with the increase of V-dopant content on La site.展开更多
With increasing demand on energy density of lithium-ion battery,wide electrochemical window and safety performance are the crucial request for next generation electrolyte.Gel-electrolyte as a pioneer for electrolyte s...With increasing demand on energy density of lithium-ion battery,wide electrochemical window and safety performance are the crucial request for next generation electrolyte.Gel-electrolyte as a pioneer for electrolyte solidization development aims to solve the safety and electrochemical window problems.However,low ionic conductivity and poor physical performance prohibit its further application.Herein,a fast-ionic conductor(Li_(2.64)(Sc_(0.9)Ti_(0.1))_(2)(PO_(4))_(3))(LSTP)was added into poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)base gel-electrolyte to enhance mechanical properties and ionic conductivity.Evidences reveal that LSTP was able to weaken interforce between polymer chains,which increased the ionic conductibility and decreased interface resistance during the cycling significantly.The obtained LiFePO_(4)/hybrid gel-electrolyte/Li-metal coin cell exhibited excellent rate capacity(145 mA·h/g at 1C,95 mA·h/g at 3C,28℃)which presented a potential that can be comparable with commercialized liquid electrolyte system.展开更多
Lithium-ion capacitors(LICs)could combine the virtues of high power capability of conventional supercapacitors and high energy density of lithium-ion batteries.However,the lack of high-performance electrode materials ...Lithium-ion capacitors(LICs)could combine the virtues of high power capability of conventional supercapacitors and high energy density of lithium-ion batteries.However,the lack of high-performance electrode materials and the kinetic imbalance between the positive and negative electrodes are the major challenge.In this study,Fe3O4 nanoparticles encapsulated in nitrogen-rich carbon(Fe3O4@NC)were prepared through a self-assembly of the colloidal Fe OOH with polyaniline(PANI)followed by pyrolysis.Due to the well-designed nanostructure,conductive nitrogen-rich carbon shells,abundant micropores and high specific surface area,Fe3O4@NC-700 delivers a high capacity,high rate capability and long cycling stability.Kinetic analyses of the redox reactions reveal the pseudocapacitive mechanism and the feasibility as negative material in LIC devices.A novel LIC was constructed with Fe3O4@NC-700 as the negative electrode and expanded graphene(EGN)as the positive electrode.The wellmatched two electrodes effectively alleviate the kinetic imbalance between the positive and negative electrodes.As a result,Fe3O4@NC-700//EGN LIC exhibits a wide operating voltage window,and thus achieves an ultrahigh energy density of 137.5 W h kg^-1.These results provide fundamental insights into the design of pseudocapacitive electrode and show future research directions towards the next generation energy storage devices.展开更多
Stretchable ionic conductors with high transparency and excellent resilience are highly desired for flexible electronics,but traditional ionic conductive hydrogels are easy to dry and freeze.Herein,a newly hybrid cros...Stretchable ionic conductors with high transparency and excellent resilience are highly desired for flexible electronics,but traditional ionic conductive hydrogels are easy to dry and freeze.Herein,a newly hybrid crosslinking strategy is presented for preparing a stretchable and transparent hydrogel by using sodium alginate(SA)and acrylamide based on the unique physically and covalently hybrid crosslinking mechanism,which is transformed into organohydrogel by simple solvent replacement.Due to the combination of hybrid crosslinking double network and hydrogen bond interactions introduced by the glycerin-water binary solvent,the SA-poly(acrylamide)-organohydrogel(SPOH)demonstrates excellent anti-freezing(-20℃)property,stability(>2 days),transparency,stretchability(~1600%)and high ionic conductivity(17.1 mS cm^(-1)).Thus,a triboelectric nanogenerator made from SPOH(O-TENG)shows an instantaneous peak power density of 262 mW m^(-2)at a load resistance of 10 MΩand efficiently harvests biomechanical energy to drive an electronic watch and light-emitting diode.Moreover,The O-TENG exhibits favorable long-term stability(2 weeks)and temperature tolerance(-20℃).In addition,the raw materials can be prepared into SPOH fibers by a simple tubular mold method,exhibiting high transparency,which can be used for laser transmission.The various abilities of the SPOH promise the application of energy harvesting and laser transmission for wearable electronics and biomedical field.展开更多
The intrinsic drawbacks of electrolytes and the growth of lithium dendrites limit the development of commercial lithium batteries.To address the aforementioned challenges,a novel biomimetic brain-like nanostructure(BB...The intrinsic drawbacks of electrolytes and the growth of lithium dendrites limit the development of commercial lithium batteries.To address the aforementioned challenges,a novel biomimetic brain-like nanostructure(BBLN)solid polymer electrolyte was created by manipulating the shape of the incorporated nanoparticles.Our designed BBLN solid polymer electrolyte was created by incorporating spherical core-shell(UIO-66@67)fillers into polymer electrolyte,which is significantly different from traditional polymer-based composite electrolytes.UIO-66@67 spherical nanoparticles are highly favorable to eliminating polymer electrolyte stress and deformation during solidification,indicating a great potential for fabricating highly uniform BBLN solid polymer electrolytes with a substantial number of continuous convolutions.Furthermore,spherical nanoparticles can significantly reduce the crystalline structure of polymer electrolytes,improving polymer chain segmental movement and providing continuous pathways for rapid ion transfer.As a result,BBLN solid polymer electrolyte shows excellent ionic conductivity(9.2×10^(−4)S cm^(−1)),a high lithium transference number(0.74),and outstanding cycle stability against lithium electrodes over 6500 h at room temperature.The concept of biomimetic brain-like nanostructures in this work demonstrates a novel strategy to enhance ion transport in polymerbased electrolytes for solid-state batteries.展开更多
Two-dimensional transition-metal carbides(MXenes)have superhydrophilic surfaces and superior metal conductivity,making them competitive in the field of electrochemical energy storage.However,MXenes with layered struct...Two-dimensional transition-metal carbides(MXenes)have superhydrophilic surfaces and superior metal conductivity,making them competitive in the field of electrochemical energy storage.However,MXenes with layered structures are easily stackable,which reduces the ion accessibility and transport paths,thus limiting their electrochemical performance.To fully exploit the advantages of MXenes in electrochemical energy storage,this study reports the etching of large-sized MXene into nanosheets with nanoscale ion channels via a chemical oxidation method.While the resulting ion-channel MXene electrodes retain the excellent mechanical strength and electrical conductivity of large-sized MXene nanosheets,they can effectively shorten the ion transport distance and improve the overall electrochemical activity.The fabricated self-healing MXene-based zinc-ion microcapacitor exhibits a high areal specific capacitance(532.8 mF cm^(-2))at the current density of 2mA cm^(-2),a low self-discharge rate(4.4 mV h^(-1)),and high energy density of 145.1μWh cm^(-2)at the power density of 2800μW cm^(-2).The proposed nanoscale ion channel structure provides an alternative strategy for constructing high-performance electrochemical energy storage electrodes,and has great application prospects in the fields of electrochemical energy storage and flexible electronics.展开更多
Despite the advances of aqueous zinc(Zn)batteries as sustainable energy storage systems,their practical application remains challenging due to the issues of spontaneous corrosion and dendritic deposits at the Zn metal...Despite the advances of aqueous zinc(Zn)batteries as sustainable energy storage systems,their practical application remains challenging due to the issues of spontaneous corrosion and dendritic deposits at the Zn metal anode.In this work,conformal growth of zinc hydroxide sulfate(ZHS)with dominating(001)facet was realized on(002)plane-dominated Zn metal foil fabricated through a facile thermal annealing process.The ZHS possessed high Zn^(2+)conductivity(16.9 mS cm^(-1))and low electronic conductivity(1.28×10^(4)Ωcm),and acted as a heterogeneous and robust solid electrolyte interface(SEI)layer on metallic Zn electrode,which regulated the electrochemical Zn plating behavior and suppressed side reactions simultaneously.Moreover,low self-diffusion barrier along the(002)plane promoted the 2D diffusion and horizontal electrochemical plating of metallic Zn for(002)-textured Zn electrode.Consequently,the as-achieved Zn electrode exhibited remarkable cycling stability over 7000 cycles at 2 mA cm^(-2)and 0.5 mAh cm^(-2)with a low overpotential of 25 mV in symmetric cells.Pairing with a MnO_(2)cathode,the as-achieved Zn electrode achieved stable cell cycling with 92.7%capacity retention after 1000 cycles at 10 C with a remarkable average Coulombic efficiency of 99.9%.展开更多
基金supported by the National Natural Science Foundation of China(No.21501015)the Hunan Provincial Natural Science Foundation,China(No.2022JJ30604)Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation,China(No.2022CL01)。
文摘A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.
基金Supported by the Joint Funds of NSFC-Guangdong of China(U0834004)the Natural Science Foundation of Guangdong Province(06025657)
文摘Apatite-lanthanum silicate has attracted considerable interest in recent years due to its high oxide ion conductivity.In this paper,V-doped samples La10-xVx(SiO4) 6O3+x(0≤x≤1.5) were prepared by sol-gel method and the influences of V-dopant content on calcining temperature and conductivity were reported.The samples were characterized by thermal analysis(TG-DSC) ,X-ray diffraction(XRD) and scanning electron micrograph(SEM) . The apatite was obtained at 800°C,a relatively low temperature in comparison to 1500°C with the conventional solid-state method.The ceramic pellets sintered at 1200°C for 5 h showed a higher relative density than La9.33Si6O26 pellets sintered at 1400°C for 20 h.The conductivities of samples were measured by electrochemical impedance spectroscopy.The conductivity was improved with the increase of V-dopant content on La site.
基金Projects(51974368,51774333) supported by the National Natural Science Foundation of ChinaProject(2020JJ2048) supported by the Hunan Provincial Natural Science Foundation of China。
文摘With increasing demand on energy density of lithium-ion battery,wide electrochemical window and safety performance are the crucial request for next generation electrolyte.Gel-electrolyte as a pioneer for electrolyte solidization development aims to solve the safety and electrochemical window problems.However,low ionic conductivity and poor physical performance prohibit its further application.Herein,a fast-ionic conductor(Li_(2.64)(Sc_(0.9)Ti_(0.1))_(2)(PO_(4))_(3))(LSTP)was added into poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)base gel-electrolyte to enhance mechanical properties and ionic conductivity.Evidences reveal that LSTP was able to weaken interforce between polymer chains,which increased the ionic conductibility and decreased interface resistance during the cycling significantly.The obtained LiFePO_(4)/hybrid gel-electrolyte/Li-metal coin cell exhibited excellent rate capacity(145 mA·h/g at 1C,95 mA·h/g at 3C,28℃)which presented a potential that can be comparable with commercialized liquid electrolyte system.
基金financial support of the National Natural Science Foundation of China(21773116)the Specialized Research Fund for the Doctoral Program of Higher Education(SRFDP,20130091110010)+1 种基金the Natural Science Foundation of Jiangsu Province(BK2011438)the National Science Fund for Talent Training in Basic Science(J1103310)。
文摘Lithium-ion capacitors(LICs)could combine the virtues of high power capability of conventional supercapacitors and high energy density of lithium-ion batteries.However,the lack of high-performance electrode materials and the kinetic imbalance between the positive and negative electrodes are the major challenge.In this study,Fe3O4 nanoparticles encapsulated in nitrogen-rich carbon(Fe3O4@NC)were prepared through a self-assembly of the colloidal Fe OOH with polyaniline(PANI)followed by pyrolysis.Due to the well-designed nanostructure,conductive nitrogen-rich carbon shells,abundant micropores and high specific surface area,Fe3O4@NC-700 delivers a high capacity,high rate capability and long cycling stability.Kinetic analyses of the redox reactions reveal the pseudocapacitive mechanism and the feasibility as negative material in LIC devices.A novel LIC was constructed with Fe3O4@NC-700 as the negative electrode and expanded graphene(EGN)as the positive electrode.The wellmatched two electrodes effectively alleviate the kinetic imbalance between the positive and negative electrodes.As a result,Fe3O4@NC-700//EGN LIC exhibits a wide operating voltage window,and thus achieves an ultrahigh energy density of 137.5 W h kg^-1.These results provide fundamental insights into the design of pseudocapacitive electrode and show future research directions towards the next generation energy storage devices.
基金financially supported by the National Natural Science Foundation of China(52002059 and 51872204)the Belt&Road Young Scientist Exchanges Project of Science and Technology Commission Foundation of Shanghai(20520741000)+1 种基金the Fundamental Research Funds for the Central Universities(20D110631)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials(DonghuaUniversity,KF2019)。
文摘Stretchable ionic conductors with high transparency and excellent resilience are highly desired for flexible electronics,but traditional ionic conductive hydrogels are easy to dry and freeze.Herein,a newly hybrid crosslinking strategy is presented for preparing a stretchable and transparent hydrogel by using sodium alginate(SA)and acrylamide based on the unique physically and covalently hybrid crosslinking mechanism,which is transformed into organohydrogel by simple solvent replacement.Due to the combination of hybrid crosslinking double network and hydrogen bond interactions introduced by the glycerin-water binary solvent,the SA-poly(acrylamide)-organohydrogel(SPOH)demonstrates excellent anti-freezing(-20℃)property,stability(>2 days),transparency,stretchability(~1600%)and high ionic conductivity(17.1 mS cm^(-1)).Thus,a triboelectric nanogenerator made from SPOH(O-TENG)shows an instantaneous peak power density of 262 mW m^(-2)at a load resistance of 10 MΩand efficiently harvests biomechanical energy to drive an electronic watch and light-emitting diode.Moreover,The O-TENG exhibits favorable long-term stability(2 weeks)and temperature tolerance(-20℃).In addition,the raw materials can be prepared into SPOH fibers by a simple tubular mold method,exhibiting high transparency,which can be used for laser transmission.The various abilities of the SPOH promise the application of energy harvesting and laser transmission for wearable electronics and biomedical field.
基金supported by the National Natural Science Foundation of China(51802239 and 52127816)the National Key Research and Development Program of China(2020YFA0715000)+2 种基金the Key Research and Development Program of Hubei Province(2021BAA070)Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-005)the Fundamental Research Funds for the Central Universities(2020Ⅲ011GX,2020ⅣB057,2019ⅣB054 and 2019Ⅲ062JL)。
文摘The intrinsic drawbacks of electrolytes and the growth of lithium dendrites limit the development of commercial lithium batteries.To address the aforementioned challenges,a novel biomimetic brain-like nanostructure(BBLN)solid polymer electrolyte was created by manipulating the shape of the incorporated nanoparticles.Our designed BBLN solid polymer electrolyte was created by incorporating spherical core-shell(UIO-66@67)fillers into polymer electrolyte,which is significantly different from traditional polymer-based composite electrolytes.UIO-66@67 spherical nanoparticles are highly favorable to eliminating polymer electrolyte stress and deformation during solidification,indicating a great potential for fabricating highly uniform BBLN solid polymer electrolytes with a substantial number of continuous convolutions.Furthermore,spherical nanoparticles can significantly reduce the crystalline structure of polymer electrolytes,improving polymer chain segmental movement and providing continuous pathways for rapid ion transfer.As a result,BBLN solid polymer electrolyte shows excellent ionic conductivity(9.2×10^(−4)S cm^(−1)),a high lithium transference number(0.74),and outstanding cycle stability against lithium electrodes over 6500 h at room temperature.The concept of biomimetic brain-like nanostructures in this work demonstrates a novel strategy to enhance ion transport in polymerbased electrolytes for solid-state batteries.
基金supported by the National Natural Science Foundation of China(51871104,12204010,and 52272177)the Fundamental Research Funds for the Central Universities(2019kfy RCPY074)the Natural Science Foundation of Anhui Province(2008085QA27,2008085QA41)。
文摘Two-dimensional transition-metal carbides(MXenes)have superhydrophilic surfaces and superior metal conductivity,making them competitive in the field of electrochemical energy storage.However,MXenes with layered structures are easily stackable,which reduces the ion accessibility and transport paths,thus limiting their electrochemical performance.To fully exploit the advantages of MXenes in electrochemical energy storage,this study reports the etching of large-sized MXene into nanosheets with nanoscale ion channels via a chemical oxidation method.While the resulting ion-channel MXene electrodes retain the excellent mechanical strength and electrical conductivity of large-sized MXene nanosheets,they can effectively shorten the ion transport distance and improve the overall electrochemical activity.The fabricated self-healing MXene-based zinc-ion microcapacitor exhibits a high areal specific capacitance(532.8 mF cm^(-2))at the current density of 2mA cm^(-2),a low self-discharge rate(4.4 mV h^(-1)),and high energy density of 145.1μWh cm^(-2)at the power density of 2800μW cm^(-2).The proposed nanoscale ion channel structure provides an alternative strategy for constructing high-performance electrochemical energy storage electrodes,and has great application prospects in the fields of electrochemical energy storage and flexible electronics.
基金financial support by the Innovation Fund of Wuhan National Laboratory for Optoelectronics of Huazhong University of Science and Technologythe China Postdoctoral Science Foundation (2018M640694 and 2020T130223)+1 种基金support of the Singapore National Research Foundation (NRF-NRFF2017-04)Agency for Science, Technology and Research (Central Research Fund Award)
文摘Despite the advances of aqueous zinc(Zn)batteries as sustainable energy storage systems,their practical application remains challenging due to the issues of spontaneous corrosion and dendritic deposits at the Zn metal anode.In this work,conformal growth of zinc hydroxide sulfate(ZHS)with dominating(001)facet was realized on(002)plane-dominated Zn metal foil fabricated through a facile thermal annealing process.The ZHS possessed high Zn^(2+)conductivity(16.9 mS cm^(-1))and low electronic conductivity(1.28×10^(4)Ωcm),and acted as a heterogeneous and robust solid electrolyte interface(SEI)layer on metallic Zn electrode,which regulated the electrochemical Zn plating behavior and suppressed side reactions simultaneously.Moreover,low self-diffusion barrier along the(002)plane promoted the 2D diffusion and horizontal electrochemical plating of metallic Zn for(002)-textured Zn electrode.Consequently,the as-achieved Zn electrode exhibited remarkable cycling stability over 7000 cycles at 2 mA cm^(-2)and 0.5 mAh cm^(-2)with a low overpotential of 25 mV in symmetric cells.Pairing with a MnO_(2)cathode,the as-achieved Zn electrode achieved stable cell cycling with 92.7%capacity retention after 1000 cycles at 10 C with a remarkable average Coulombic efficiency of 99.9%.
