Ultrafine cube-shape Ce2Sn2O7 nanoparticles crystallized in pure pyrochlore phase with a size of about 10 nm have been successfully synthesized by a facile hydrothermal method.Conditional experiments have been conduct...Ultrafine cube-shape Ce2Sn2O7 nanoparticles crystallized in pure pyrochlore phase with a size of about 10 nm have been successfully synthesized by a facile hydrothermal method.Conditional experiments have been conducted to optimize the processing parameters including temperature,pH,reaction duration,precipitator types to obtain phase-pure Ce2Sn2O7.The crystal structure,morphology and sizes and specific surface area have been characterized by X-ray diffractometer(XRD),Raman spectrum,transmission electron microscope(TEM),high resolution transmission electron microscope(HRTEM),and Brunauer-Emmett-Teller(BET).The as-synthesized Ce2Sn2O7 ultrafine nanocubes have been evaluated as electrode materials for pseudo-capacitors and lithium ion batteries.When testing as supercapacitors,a high specific capacitance of 222 F/g at 0.1 A/g and a good cycling stability with a capacitance retention of higher than 86%after 5000 cycle have been achieved.When targeted for anode material for lithium ion batteries,the nanocubes deliver a high specific reversible capacity of more than 900 mA·h/g at 0.05C rate.The rate capability and cycling performance is also very promising as compared with the traditional graphite anode.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
Development of high-voltage electrolytes with non-flammability is significantly important for future energy storage devices.Aqueous electrolytes are inherently non-flammable,easy to handle,and their electrochemical st...Development of high-voltage electrolytes with non-flammability is significantly important for future energy storage devices.Aqueous electrolytes are inherently non-flammable,easy to handle,and their electrochemical stability windows(ESWs)can be considerably expanded by increasing electrolyte concentrations.However,further breakthroughs of their ESWs encounter bottlenecks because of the limited salt solubility,leading to that most of the high-energy anode materials can hardly function reversibly in aqueous electrolytes.Here,by introducing a non-flammable ionic liquid as co-solvent in a lithium salt/water system,we develop a"water in salt/ionic liquid"(WiSIL)electrolyte with extremely low water content.In such WiSIL electrolyte,commercial niobium pentoxide(Nb2O5)material can operate at a low potential(-1.6 V versus Ag/AgCl)and contribute its full capacity.Consequently,the resultant Nb2O5-based aqueous lithium-ion capacitor is able to operate at a high voltage of 2.8 V along with long cycling stability over 3000 cycles,and displays comparable energy and power performance(51.9 Wh kg^-1 at 0.37 kW kg^-1 and 16.4 Wh kg^-1 at 4.9 kW kg^-1)to those using non-aqueous electrolytes but with improved safety performance and manufacturing efficiency.展开更多
Conversion-type anode materials hold great potential for Li+storage applications owing to their high specific capacity,while large volume expansion and poor electrical conductivity limit their rate and cycling perform...Conversion-type anode materials hold great potential for Li+storage applications owing to their high specific capacity,while large volume expansion and poor electrical conductivity limit their rate and cycling performances.Herein,a bimetal ZnMn-based metal-organic framework(ZnMn-MOF)is engineered for in situ conversion of MnO-encapsulated porous carbon(MnO/PC)composite.The templating and activation effects of coordinated Zn endow the converted PC matrix with a highly porous structure.This enhances the compatibility of PC matrix with MnO particles,resulting in the full encapsulation of MnO particles in the PC matrix.More significantly,the PC matrix provides enough void space to buffer the volume change,which fully wraps the MnO without crack or fracture during repeated cycling.As a result,MnO/PC shows high charge storage capability,extraordinary rate performance,and long-term cycling stability at the same time.Thus MnO/PC exhibits high delithiation capacities of 768mA h g^(-1)at 0.1Ag^(-1)and 487mA h g^(-1)at a high rate of 0.7Ag^(-1),combined with an unattenuated cycling performance after 500 cycles at 0.3Ag^(-1).More significantly,MnO/PC demonstrates a well-matched performance with the capacitive activated carbon electrode in a Li-ion capacitor(LIC)full cell.LIC demonstrates a high specific energy of 153.6W h kg^(-1)at 210W kg^(-1),combined with a specific energy of 71.8W h kg^(-1)at a high specific power of 63.0kW kg^(-1).展开更多
TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highr...TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highrate capability is limited by their poor electronic and ionic conductivity.In particular,studies on TNO for LICs are lacking and that for flexible LICs have not yet been reported.Herein,a unique TNO porous electrode with cross-linked nanorods tailored by post-annealing and its application in flexible LICs are reported.This binder-free TNO anode exhibits superior rate performance(~66.3%capacity retention as the rate increases from 1 to 40 C),which is ascribed to the greatly shortened ion-diffusion length in TNO nanorods,facile electrolyte penetration and fast electron transport along the continuous single-crystalline nanorod network.Furthermore,the TNO anode shows an excellent cycling stability up to 2000 cycles and good flexibility(no capacity loss after continuous bending for 500 times).Model flexible LIC assembled with the TNO anode and activated carbon cathode exhibits increased gravimetric and volumetric energy/power densities(~100.6 W h kg^-1/4108.8 W kg^-1;10.7 mW h cm^-3/419.3 mW cm^-3),more superior to previously reported hybrid supercapacitors.The device also efficiently powers an LED light upon 180°bending.展开更多
Li-ion hybrid supercapacitors (Li-HECs) facilitate effective combination of the advantages of supercapacitors and Li-ion batteries (LIBs). However, challenges remain in designing and preparing suitable anode and c...Li-ion hybrid supercapacitors (Li-HECs) facilitate effective combination of the advantages of supercapacitors and Li-ion batteries (LIBs). However, challenges remain in designing and preparing suitable anode and cathode materials, which often require tedious and expensive procedures. Herein, we demonstrated that hollow N-doped carbon capsules (HNC) with and without a Fe304 nanoparticle core can respectively function as the anode and the cathode in very-high-performance Li-HECs. The Fe3Oa@NC anode exhibited a high reversible specific capacity exceeding 1530 mA h g^-1 at 100 mA g^-1 and excellent rate capability (45% capacity retention from 0.1 to 5 A g^-1) and cycle stability (〉97% retention after 100 cycles). Moreover, high rate performance was achieved in a full-cell using the HNC cathode. By combining the respective structural advantages of the components, the hybrid device with Fe3Oa@NC//HN C exhibited a remark- able energy density of 185 W h kg^-1 at a power density of 39 W kg^-1. The hybrid device furnished a battery-inaccessible power density of 28 kW kg^-1 with rapid charging/discharging within 9 s at an energy density of 95 W h kg^-1.展开更多
基金Project(JCYJ20170817110251498)supported by the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen,ChinaProject(2016TQ03C919)supported by the Guangdong Special Support for the Science and Technology Leading Young Scientist,ChinaProjects(21603094,21703096)supported by the National Natural Science Foundation of China
文摘Ultrafine cube-shape Ce2Sn2O7 nanoparticles crystallized in pure pyrochlore phase with a size of about 10 nm have been successfully synthesized by a facile hydrothermal method.Conditional experiments have been conducted to optimize the processing parameters including temperature,pH,reaction duration,precipitator types to obtain phase-pure Ce2Sn2O7.The crystal structure,morphology and sizes and specific surface area have been characterized by X-ray diffractometer(XRD),Raman spectrum,transmission electron microscope(TEM),high resolution transmission electron microscope(HRTEM),and Brunauer-Emmett-Teller(BET).The as-synthesized Ce2Sn2O7 ultrafine nanocubes have been evaluated as electrode materials for pseudo-capacitors and lithium ion batteries.When testing as supercapacitors,a high specific capacitance of 222 F/g at 0.1 A/g and a good cycling stability with a capacitance retention of higher than 86%after 5000 cycle have been achieved.When targeted for anode material for lithium ion batteries,the nanocubes deliver a high specific reversible capacity of more than 900 mA·h/g at 0.05C rate.The rate capability and cycling performance is also very promising as compared with the traditional graphite anode.
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supported by the National Natural Science Foundations of China(21573265 and 21673263)the Zhaoqing Municipal Science and Technology Bureau(2019K038)+2 种基金the Key Cultivation Projects of the Institute in 13th Five-Yearthe Instruments Function Development&Technology Innovation Project of Chinese Academy of Sciences(2020g105)the Western Young Scholars Foundations of Chinese Academy of Sciences。
文摘Development of high-voltage electrolytes with non-flammability is significantly important for future energy storage devices.Aqueous electrolytes are inherently non-flammable,easy to handle,and their electrochemical stability windows(ESWs)can be considerably expanded by increasing electrolyte concentrations.However,further breakthroughs of their ESWs encounter bottlenecks because of the limited salt solubility,leading to that most of the high-energy anode materials can hardly function reversibly in aqueous electrolytes.Here,by introducing a non-flammable ionic liquid as co-solvent in a lithium salt/water system,we develop a"water in salt/ionic liquid"(WiSIL)electrolyte with extremely low water content.In such WiSIL electrolyte,commercial niobium pentoxide(Nb2O5)material can operate at a low potential(-1.6 V versus Ag/AgCl)and contribute its full capacity.Consequently,the resultant Nb2O5-based aqueous lithium-ion capacitor is able to operate at a high voltage of 2.8 V along with long cycling stability over 3000 cycles,and displays comparable energy and power performance(51.9 Wh kg^-1 at 0.37 kW kg^-1 and 16.4 Wh kg^-1 at 4.9 kW kg^-1)to those using non-aqueous electrolytes but with improved safety performance and manufacturing efficiency.
基金supported by the National Natural Science Foundation of China(21905148)China Postdoctoral Science Foundation(2019T120567 and 2017M612184)+2 种基金the 1000-Talents Planthe World-Class Discipline Programthe Taishan Scholars Advantageous and Distinctive Discipline Program of Shandong province for supporting the research team of energy storage materials.
文摘Conversion-type anode materials hold great potential for Li+storage applications owing to their high specific capacity,while large volume expansion and poor electrical conductivity limit their rate and cycling performances.Herein,a bimetal ZnMn-based metal-organic framework(ZnMn-MOF)is engineered for in situ conversion of MnO-encapsulated porous carbon(MnO/PC)composite.The templating and activation effects of coordinated Zn endow the converted PC matrix with a highly porous structure.This enhances the compatibility of PC matrix with MnO particles,resulting in the full encapsulation of MnO particles in the PC matrix.More significantly,the PC matrix provides enough void space to buffer the volume change,which fully wraps the MnO without crack or fracture during repeated cycling.As a result,MnO/PC shows high charge storage capability,extraordinary rate performance,and long-term cycling stability at the same time.Thus MnO/PC exhibits high delithiation capacities of 768mA h g^(-1)at 0.1Ag^(-1)and 487mA h g^(-1)at a high rate of 0.7Ag^(-1),combined with an unattenuated cycling performance after 500 cycles at 0.3Ag^(-1).More significantly,MnO/PC demonstrates a well-matched performance with the capacitive activated carbon electrode in a Li-ion capacitor(LIC)full cell.LIC demonstrates a high specific energy of 153.6W h kg^(-1)at 210W kg^(-1),combined with a specific energy of 71.8W h kg^(-1)at a high specific power of 63.0kW kg^(-1).
基金supported by the National Natural Science Foundation of China (51672205, 21673169 and 51972257)the National Key R&D Program of China (2016YFA0202602)the Natural Science Foundation of Hubei Province (2018CFB581)
文摘TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highrate capability is limited by their poor electronic and ionic conductivity.In particular,studies on TNO for LICs are lacking and that for flexible LICs have not yet been reported.Herein,a unique TNO porous electrode with cross-linked nanorods tailored by post-annealing and its application in flexible LICs are reported.This binder-free TNO anode exhibits superior rate performance(~66.3%capacity retention as the rate increases from 1 to 40 C),which is ascribed to the greatly shortened ion-diffusion length in TNO nanorods,facile electrolyte penetration and fast electron transport along the continuous single-crystalline nanorod network.Furthermore,the TNO anode shows an excellent cycling stability up to 2000 cycles and good flexibility(no capacity loss after continuous bending for 500 times).Model flexible LIC assembled with the TNO anode and activated carbon cathode exhibits increased gravimetric and volumetric energy/power densities(~100.6 W h kg^-1/4108.8 W kg^-1;10.7 mW h cm^-3/419.3 mW cm^-3),more superior to previously reported hybrid supercapacitors.The device also efficiently powers an LED light upon 180°bending.
基金supported by the National Natural Science Foundation of China (51601127, 21603162 and 51671145)China Post-doctoral Science Fund (2015M581304)+1 种基金Tianjin Municipal Education Commission, Tianjin Municipal Science and Technology Commission (16ZXCLGX00120)the Fundamental Research Funds of Tianjin University of Technology
文摘Li-ion hybrid supercapacitors (Li-HECs) facilitate effective combination of the advantages of supercapacitors and Li-ion batteries (LIBs). However, challenges remain in designing and preparing suitable anode and cathode materials, which often require tedious and expensive procedures. Herein, we demonstrated that hollow N-doped carbon capsules (HNC) with and without a Fe304 nanoparticle core can respectively function as the anode and the cathode in very-high-performance Li-HECs. The Fe3Oa@NC anode exhibited a high reversible specific capacity exceeding 1530 mA h g^-1 at 100 mA g^-1 and excellent rate capability (45% capacity retention from 0.1 to 5 A g^-1) and cycle stability (〉97% retention after 100 cycles). Moreover, high rate performance was achieved in a full-cell using the HNC cathode. By combining the respective structural advantages of the components, the hybrid device with Fe3Oa@NC//HN C exhibited a remark- able energy density of 185 W h kg^-1 at a power density of 39 W kg^-1. The hybrid device furnished a battery-inaccessible power density of 28 kW kg^-1 with rapid charging/discharging within 9 s at an energy density of 95 W h kg^-1.