The adsorption capacity and absorption rate for electrolyte onto activated carbon are important parameters used to characterize activated carbon electric double-layer capacitor electrodes. In this paper the pore struc...The adsorption capacity and absorption rate for electrolyte onto activated carbon are important parameters used to characterize activated carbon electric double-layer capacitor electrodes. In this paper the pore structure of typical commercial activated carbons, and various Mn-doped activated carbons prepared on a laboratory scale, are described. The pore structure was character-ized by N2 adsorption/desorption isotherms. Isotherms for K+ adsorption onto these activated carbons from the aqueous phase were also obtained. The experimental, equilibrium K+ adsorption data were fitted to the Langmuir, Freundlich or Temkin equations. Adsorption of K+ onto the activated carbons was measured and plotted as a function of time. The adsorption kinetic data were modeled by either pseudo-first or pseudo-second order equations. The Elvoich equation, a liquid film diffusion and an intra-particle diffusion model were used to fit the kinetic data. The results indicate that the adsorption of K+ onto activated carbon is influenced by many factors including pore size distribution, specific surface area and the surface chemistry of the activated carbons. The Temkin equation best describes the equilibrium adsorption data. The pseudo-second order model exactly describes the whole adsorption process, which is controlled by both liquid film and intra-particle diffusion.展开更多
Electrical double-layer capacitors are widely concerned for their high power density,long cycling life and high cycling efficiency.However,their wide application is limited by their low energy density.In this study,we...Electrical double-layer capacitors are widely concerned for their high power density,long cycling life and high cycling efficiency.However,their wide application is limited by their low energy density.In this study,we propose a simple yet environmental friendly method to synthesize cobalt and nitrogen atoms co-doped porous carbon(CoAT-NC) material.Cobalt atoms connected with primarily pyridinic nitrogen atoms can be uniformly dispersed in the amorphous carbon matrix,which is benefit for improving electrical conductivity and density of states of the carbon material.Therefore,an enhanced perfo rmance is expected when CoAT-NC is served as electrode in a supercapacitor device.CoAT-NC displays a good gravimetric capacitance of 160 F/g at 0.5 A/g combing with outstanding capacitance retention of 90% at an extremely high current density of 100 A/g in acid electrolyte.Furthermore,a good energy density of 30 Wh/kg can be obtained in the organic electrolyte.展开更多
In this study, carbon aerogels were derived via the pyrolysis of resorcinol-formaldehyde (RF) aerogels, which were cost-effectively manufactured from RF wet gels by an ambient drying technique instead of conventional ...In this study, carbon aerogels were derived via the pyrolysis of resorcinol-formaldehyde (RF) aerogels, which were cost-effectively manufactured from RF wet gels by an ambient drying technique instead of conventional supercritical drying. By varying the R/C ratio (molar ratio of resorcinol to catalyst), mesoporous carbon aerogels with high specific surface area were prepared successfully and further investigated as electrode materials for electric double-layer capacitors (EDLCs). The textural properties of carbon aerogels obtained were characterized by nitrogen adsorption/desorption analysis and SEM. The electrochemical performances of carbon aerogels were investigated by impedance spectroscopy, galvanostatic charge/discharge and cyclic voltammetry methods. The results show that BET surface area and specific capacitance increase with R/C ratio, the maximum values of 727 m2·g-1 and 132 F·g-1 are achieved at R/C ratio will of 300. Increasing R/C ratio increase the average pore size of carbon aerogel electrode, which has improved the rate capability. Furthermore, EDLC with carbon aerogel electrodes has an excellent stability at large discharge current and long cycle life.展开更多
A spiro-type quaternary ammonium salt, spiro-(1,1′)-bipyrrolidinium tetrafluoroborate(SBP-BF4) was successfully prepared by an economical and efficient three-step process comprising the cyclization reaction of 1,4-di...A spiro-type quaternary ammonium salt, spiro-(1,1′)-bipyrrolidinium tetrafluoroborate(SBP-BF4) was successfully prepared by an economical and efficient three-step process comprising the cyclization reaction of 1,4-dibromobutane and pyrrolidine, and subsequent ion exchange pathway with KOH followed by neutralization reaction via HBF4 in the system of ethanol solution. 1H NMR, 13 C NMR, FI-IR and XPS analyses showed the structure of SBP-BF4. The as-obtained SBP-BF4 was dissolved in AN and used as the electrolyte for supercapacitor. Electrochemical measurements demonstrate that, compared with commercial electrolyte TEMA-BF4/AN, SBP-BF4/AN exhibits high ionic conductivity, lower resistance and improved cycling performance, which is due to its smaller ion size and stable symmetry structure.展开更多
Multi-walled carbon nanombes with homogeneous diameters （40 - 60 nm）, produced by chemical vapor deposition of hydrocarbon gas, are purified by nitric acids. Infrared and Raman studies indicate that oxygen containin...Multi-walled carbon nanombes with homogeneous diameters （40 - 60 nm）, produced by chemical vapor deposition of hydrocarbon gas, are purified by nitric acids. Infrared and Raman studies indicate that oxygen containing surface groups, which are predominately carboxylic, phenolic and lactonic groups, are introduced into purified carbon nanotubes. Then three kinds of block-form porous tablets of carbon nanotubes are fabricated as electrodes in electrochemical double-layer capacitors. Using mounded mixture comprising carbon nanotubes and binder powders provides these tablets. Comparison of the effect of different processing on the structural performance of the capacitors is specifically investigated. Using chemically treated electrodes, electrochemical double-layer capacitors with a specific capacitance of about 33 F/g are obtained with 38 wt % H2SO4 as the electrolyte.展开更多
To investigate the influence of expansion pretreatment for materials on carbon structure, activated carbons （ACs） were prepared from corncob with/without expansion pretreatment by KOH activation, the structure prope...To investigate the influence of expansion pretreatment for materials on carbon structure, activated carbons （ACs） were prepared from corncob with/without expansion pretreatment by KOH activation, the structure properties of which were determined based on N2 adsorption isotherm at 77 K. The results show that the expansion pretreatment for corncobs is beneficial to the preparation of ACs with high surface area. The specific surface area of the AC derived from corncob with expansion pretreatment （AC-1） is 32.5% larger than that without expansion pretreatment （AC-2）. Furthermore, to probe the potential application of corncob-based ACs in electric double-layer capacitor （EDLC）, the prepared ACs were used as electrode materials to assemble EDLC, and its electrochemical performance was investi- gated. The results indicate that the specific capacitance of AC-I is 276 F/g at 50 mA/g, which increases by 27% com- pared with that of AC-2 （217 F/g）. As electrode materials, AC-1 presents a better electrochemical performance than AC-2, including a higher voltage maintenance ratio and a lower leakage current.展开更多
Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizabl...Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizable electrodes of electric double-layer capacitors(EDLCs) in an aqueous electrolytic solution. The porous structures and electrochemical double-layer capacitance of the activated carbons were investigated by virtue of nitrogen gas adsorption and constant current cycling(CCC) methods. The relationship among the surface area, pore volume of the activated carbons and specific double-layer capacitance was discussed. It was found that the specific capacitance of ACs increased linearly with the increase of surface area. The presence of mesopores in the activated carbons with very high surface area(>2000 m\+2/g) was not very effective for them to be used as EDLCs. The influence of chemical characteristics of the activated carbons on the double layer formation could be considered to be negligible.展开更多
In recent years, application of carbon-based nano material to electrode material has been paid attention, however, due to its higher cost, it would be difficult to put it into practical use. Then, we have proposed to ...In recent years, application of carbon-based nano material to electrode material has been paid attention, however, due to its higher cost, it would be difficult to put it into practical use. Then, we have proposed to make nano carbon fiber with lower production cost. The purpose of our research was, to apply our nano carbon fiber to electrical double-layer capacitor electrode. We used cotton candy method to make nano fiber, and applied microwave heating for carbonization. By applying nano carbon fiber to electrical double-layer capacitor electrode, we got results that thicker electrode containing nano carbon fiber leads to lower resistance value, compared with electrode without containing nano carbon fiber. From this result, it was indicated that by containing nano carbon fiber, the electric bypass was formed in the electrode.展开更多
Electrolytic conductivity, viscosity and electrochemical behavior were investigated for organic electrolytes based on PC（Propylene carbonate）, MAN（Methoxy acetonitrile） and GBL（γ-Butyrolactone） solvents. It was...Electrolytic conductivity, viscosity and electrochemical behavior were investigated for organic electrolytes based on PC（Propylene carbonate）, MAN（Methoxy acetonitrile） and GBL（γ-Butyrolactone） solvents. It was found that 1 mol/L Et4NBF4-MAN had the highest conductivity, lowest viscosity and acceptable potential window. The specific capacitance and energy density obtained from the capacitor using 1 mol/L Et4NBF4-MAN as electrolyte were the highest among all the tested electrolytes.（1 mol/L） Et4NBF4-GBL also seemed promising to be used in electric double-layer capacitor （EDLCs）.展开更多
Lignocellulose is an ideal precursor for supercapacitor electrodes due to its diverse structures and abundant availability.For supercapacitors,particularly electric double-layer capacitors(EDLCs),pore structure is cri...Lignocellulose is an ideal precursor for supercapacitor electrodes due to its diverse structures and abundant availability.For supercapacitors,particularly electric double-layer capacitors(EDLCs),pore structure is critical.This review summarizes advances in lignocellulose-derived hierarchical porous carbon(LHPC)for supercapacitors,focusing on pore structure and future research directions.We discuss how pore structure influences supercapacitor performance,the activation methods for creating pores in LHPC,and review studies on optimizing pore structure for high-performance supercapacitors.Hierarchical porous carbon should feature a sufficient micropore surface area along with suitable mesoporous and macroporous surfaces to enhance rate performance while maintaining capacitance.This review is expected to actively advance the selection of lignocellulosic precursors and the development of optimized pore structure models,with the ultimate goal of enabling efficient production of lignocellulose-derived hierarchical porous carbon electrodes with superior properties.展开更多
The electrochemical stability window(ESW)is crucial for determining the energy density of electric double-layer capacitors(EDLCs).However,current ESW testing protocols of EDLCs are strongly affected by artificial fact...The electrochemical stability window(ESW)is crucial for determining the energy density of electric double-layer capacitors(EDLCs).However,current ESW testing protocols of EDLCs are strongly affected by artificial factors,thereby leading to unreliable result.To solve this problem,we first identify the key shortcomings of the traditional protocols by analyzing their test principles.Subsequently,taking an aqueous carbon-based EDLC as an example,we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods.With the aid of this descriptor,we propose a new ESW testing protocol,which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations.The protocol can be extended from the single electrode to the full device.This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.展开更多
For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectu...For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.展开更多
Activated carbon(AC)in organic electrolytebased electric double-layer capacitors(EDLCs)usually suffers from low specific capacitance.Most studies on AC focus on improving its surface area and optimizing pore structure...Activated carbon(AC)in organic electrolytebased electric double-layer capacitors(EDLCs)usually suffers from low specific capacitance.Most studies on AC focus on improving its surface area and optimizing pore structures to enhance its electrochemical performance in EDLCs.Unfortunately,the interfacial microenvironment,which is composed of nanoporous carbon and the organic electrolyte confined in it,is always ignored.Herein,a simple and powerful strategy to create AC with an ionophobic surface is proposed to address the poor efficiency of the electric doublelayer process.The polar C±F bonds formed in the AC material are characterized through near-edge X-ray absorption fine structure and X-ray photoelectron spectroscopy.The ionophobic characteristic of YP-F60 s in an organic electrolyte is extensively studied via contact angle measurements and smallangle X-ray scattering spectroscopy.An EDLC constructed with YP-F60 s as the electrode and 1 mol L^(-1) tetraethylammonium tetrafluoroborate/propylene carbonate as the electrolyte demonstrates high specific capacitance,low internal resistance,and excellent cycling stability.Our results successfully demonstrate the importance of the interfacial microenvironment of AC and its confined electrolyte to the electrochemical performance of EDLCs.Our work also offers new perspectives on the use of the CF;plasma technique to fabricate low-cost superior carbon for EDLCs.展开更多
The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tu...The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tube(CT)grids(3D-CTGs)using a 3D porous anodic aluminum oxide template-assisted method as electrodes of electrical double-layer capacitors(EDLCs),showing excellent frequency response performance.The unique design warrants fast ion migration channels,excellent electronic conductivity,and good structural stability.This study achieved one of the highest carbon-based ultrahigh-power EDLCs with the 3D-CTG electrodes,resulting in ultrahigh power of 437 and 1708 W·cm−3 with aqueous and organic electrolytes,respectively.Capacitors constructed with these electrodes would have important application prospects in the ultrahigh-power output.The rational design and fabrication of the 3D-CTGs electrodes have demonstrated their capability to build capacitors with ultrahighpower performance and open up new possibilities for applications requiring high-power output.展开更多
The space-charge distributions of electric double-layer capacitors （EDLCs）, which are energy storage devices, were examined with the pulsed electroacoustic （PEA） method. It was found that the experimental results ...The space-charge distributions of electric double-layer capacitors （EDLCs）, which are energy storage devices, were examined with the pulsed electroacoustic （PEA） method. It was found that the experimental results could be influenced by the reflection and penetration of sound waves when the space-charge dis- tributions of EDLCs were measured with the PEA method. This is because EDLCs have a five-layer structure consisting of three materials （aluminum, cellulose, and activated carbon）. We calculated the reflection wave components that influenced the charge density through the acoustic impedance and the relative permittivity of the materials. In this way, we found that the changes in the space-charge distributions of EDLCs and their charge characteristics corresponded closely. We determined that measuring the space- charge distributions with the PEA method was effective for evaluating the charge accumulation of EDLCs. In this study, a polarized electrode was prepared for use in EDLCs. The ratio of the surface area to the average pore diameter of the polarized electrode was measured with the nitrogen adsorption method at 77 K. The relationship between the ratio of the surface area to the average pore size and the space-charge distributions of EDLCs is also discussed in this paper.展开更多
Two-dimensional double-layer honeycomb(DLHC)materials are known for their diverse physical properties,but superconductivity has been a notably absent characteristic in this structure.We address this gap by investigati...Two-dimensional double-layer honeycomb(DLHC)materials are known for their diverse physical properties,but superconductivity has been a notably absent characteristic in this structure.We address this gap by investigating M_(2)N_(2)(M=Nb,Ta)with DLHC structure using first-principles calculations.Our results show that M_(2)N_(2)are stable and metallic,exhibiting superconducting behavior.Specifically,Nb_(2)N_(2)and Ta_(2)N_(2)display superconducting transition temperatures of 6.8 K and 8.8 K,respectively.Their electron-phonon coupling is predominantly driven by the coupling between metal d-orbitals and low-frequency metal-dominated vibration modes.Interestingly,two compounds also exhibit non-trivial band topology.Thus,M_(2)N_(2)are promising platforms for studying the interplay between topology and superconductivity and fill the gap in superconductivity research for DLHC materials.展开更多
Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate ...Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.展开更多
Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Modern power electronics,from electric vehicles to renewable energy systems,demand capacitors that can reliably store high energy at elevated temperatures.Polymer dielectrics are widely used in capacitors due to their...Modern power electronics,from electric vehicles to renewable energy systems,demand capacitors that can reliably store high energy at elevated temperatures.Polymer dielectrics are widely used in capacitors due to their high breakdown strength and ease of processing,but they traditionally suffer from poor energy density at high temperatures[1-4].展开更多
Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy ...Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.展开更多
基金the financial support from the Research Fund for the Doctoral Program of Higher Education of China (No.2006 0290006)
文摘The adsorption capacity and absorption rate for electrolyte onto activated carbon are important parameters used to characterize activated carbon electric double-layer capacitor electrodes. In this paper the pore structure of typical commercial activated carbons, and various Mn-doped activated carbons prepared on a laboratory scale, are described. The pore structure was character-ized by N2 adsorption/desorption isotherms. Isotherms for K+ adsorption onto these activated carbons from the aqueous phase were also obtained. The experimental, equilibrium K+ adsorption data were fitted to the Langmuir, Freundlich or Temkin equations. Adsorption of K+ onto the activated carbons was measured and plotted as a function of time. The adsorption kinetic data were modeled by either pseudo-first or pseudo-second order equations. The Elvoich equation, a liquid film diffusion and an intra-particle diffusion model were used to fit the kinetic data. The results indicate that the adsorption of K+ onto activated carbon is influenced by many factors including pore size distribution, specific surface area and the surface chemistry of the activated carbons. The Temkin equation best describes the equilibrium adsorption data. The pseudo-second order model exactly describes the whole adsorption process, which is controlled by both liquid film and intra-particle diffusion.
基金financial support from the National Natural Science Foundation of China (Nos.51761145046,51672262, 21503064)100 Talents Program of the Chinese Academy of Sciences+1 种基金National Program for Support of Top notch Young ProfessionalFundamental Research Funds for the Central Universities (No.WK2060140003) and iChEM。
文摘Electrical double-layer capacitors are widely concerned for their high power density,long cycling life and high cycling efficiency.However,their wide application is limited by their low energy density.In this study,we propose a simple yet environmental friendly method to synthesize cobalt and nitrogen atoms co-doped porous carbon(CoAT-NC) material.Cobalt atoms connected with primarily pyridinic nitrogen atoms can be uniformly dispersed in the amorphous carbon matrix,which is benefit for improving electrical conductivity and density of states of the carbon material.Therefore,an enhanced perfo rmance is expected when CoAT-NC is served as electrode in a supercapacitor device.CoAT-NC displays a good gravimetric capacitance of 160 F/g at 0.5 A/g combing with outstanding capacitance retention of 90% at an extremely high current density of 100 A/g in acid electrolyte.Furthermore,a good energy density of 30 Wh/kg can be obtained in the organic electrolyte.
文摘In this study, carbon aerogels were derived via the pyrolysis of resorcinol-formaldehyde (RF) aerogels, which were cost-effectively manufactured from RF wet gels by an ambient drying technique instead of conventional supercritical drying. By varying the R/C ratio (molar ratio of resorcinol to catalyst), mesoporous carbon aerogels with high specific surface area were prepared successfully and further investigated as electrode materials for electric double-layer capacitors (EDLCs). The textural properties of carbon aerogels obtained were characterized by nitrogen adsorption/desorption analysis and SEM. The electrochemical performances of carbon aerogels were investigated by impedance spectroscopy, galvanostatic charge/discharge and cyclic voltammetry methods. The results show that BET surface area and specific capacitance increase with R/C ratio, the maximum values of 727 m2·g-1 and 132 F·g-1 are achieved at R/C ratio will of 300. Increasing R/C ratio increase the average pore size of carbon aerogel electrode, which has improved the rate capability. Furthermore, EDLC with carbon aerogel electrodes has an excellent stability at large discharge current and long cycle life.
基金Project(51371198)supported by the National Natural Science Foundation of China
文摘A spiro-type quaternary ammonium salt, spiro-(1,1′)-bipyrrolidinium tetrafluoroborate(SBP-BF4) was successfully prepared by an economical and efficient three-step process comprising the cyclization reaction of 1,4-dibromobutane and pyrrolidine, and subsequent ion exchange pathway with KOH followed by neutralization reaction via HBF4 in the system of ethanol solution. 1H NMR, 13 C NMR, FI-IR and XPS analyses showed the structure of SBP-BF4. The as-obtained SBP-BF4 was dissolved in AN and used as the electrolyte for supercapacitor. Electrochemical measurements demonstrate that, compared with commercial electrolyte TEMA-BF4/AN, SBP-BF4/AN exhibits high ionic conductivity, lower resistance and improved cycling performance, which is due to its smaller ion size and stable symmetry structure.
基金Project supported by National High-Technology Research and De-velopment Program(Grant No .863 -2002AA302302)
文摘Multi-walled carbon nanombes with homogeneous diameters （40 - 60 nm）, produced by chemical vapor deposition of hydrocarbon gas, are purified by nitric acids. Infrared and Raman studies indicate that oxygen containing surface groups, which are predominately carboxylic, phenolic and lactonic groups, are introduced into purified carbon nanotubes. Then three kinds of block-form porous tablets of carbon nanotubes are fabricated as electrodes in electrochemical double-layer capacitors. Using mounded mixture comprising carbon nanotubes and binder powders provides these tablets. Comparison of the effect of different processing on the structural performance of the capacitors is specifically investigated. Using chemically treated electrodes, electrochemical double-layer capacitors with a specific capacitance of about 33 F/g are obtained with 38 wt % H2SO4 as the electrolyte.
基金National Natural Science Foundation of China (No. 50902102 and No. 51172160)
文摘To investigate the influence of expansion pretreatment for materials on carbon structure, activated carbons （ACs） were prepared from corncob with/without expansion pretreatment by KOH activation, the structure properties of which were determined based on N2 adsorption isotherm at 77 K. The results show that the expansion pretreatment for corncobs is beneficial to the preparation of ACs with high surface area. The specific surface area of the AC derived from corncob with expansion pretreatment （AC-1） is 32.5% larger than that without expansion pretreatment （AC-2）. Furthermore, to probe the potential application of corncob-based ACs in electric double-layer capacitor （EDLC）, the prepared ACs were used as electrode materials to assemble EDLC, and its electrochemical performance was investi- gated. The results indicate that the specific capacitance of AC-I is 276 F/g at 50 mA/g, which increases by 27% com- pared with that of AC-2 （217 F/g）. As electrode materials, AC-1 presents a better electrochemical performance than AC-2, including a higher voltage maintenance ratio and a lower leakage current.
基金Supported by the Young Teacher Scientific Research Foundation of BU CT(No.QN0 2 4 9) and National Natural ScienceFoundation(No.5 0 2 72 0 70 )
文摘Activated carbons(ACs) with a wide range of surface areas were made from petroleum coke by means of KOH activation. The electrochemical characterization was carried out for several activated carbons used as polarizable electrodes of electric double-layer capacitors(EDLCs) in an aqueous electrolytic solution. The porous structures and electrochemical double-layer capacitance of the activated carbons were investigated by virtue of nitrogen gas adsorption and constant current cycling(CCC) methods. The relationship among the surface area, pore volume of the activated carbons and specific double-layer capacitance was discussed. It was found that the specific capacitance of ACs increased linearly with the increase of surface area. The presence of mesopores in the activated carbons with very high surface area(>2000 m\+2/g) was not very effective for them to be used as EDLCs. The influence of chemical characteristics of the activated carbons on the double layer formation could be considered to be negligible.
文摘In recent years, application of carbon-based nano material to electrode material has been paid attention, however, due to its higher cost, it would be difficult to put it into practical use. Then, we have proposed to make nano carbon fiber with lower production cost. The purpose of our research was, to apply our nano carbon fiber to electrical double-layer capacitor electrode. We used cotton candy method to make nano fiber, and applied microwave heating for carbonization. By applying nano carbon fiber to electrical double-layer capacitor electrode, we got results that thicker electrode containing nano carbon fiber leads to lower resistance value, compared with electrode without containing nano carbon fiber. From this result, it was indicated that by containing nano carbon fiber, the electric bypass was formed in the electrode.
文摘Electrolytic conductivity, viscosity and electrochemical behavior were investigated for organic electrolytes based on PC（Propylene carbonate）, MAN（Methoxy acetonitrile） and GBL（γ-Butyrolactone） solvents. It was found that 1 mol/L Et4NBF4-MAN had the highest conductivity, lowest viscosity and acceptable potential window. The specific capacitance and energy density obtained from the capacitor using 1 mol/L Et4NBF4-MAN as electrolyte were the highest among all the tested electrolytes.（1 mol/L） Et4NBF4-GBL also seemed promising to be used in electric double-layer capacitor （EDLCs）.
基金financial support for this research from the National Key Research Development Program of China(No.2021YFB3800300)Shanghai Pujiang Programme(No.23PJD045)the Shanghai Science and Technology Committee(No.24CL2900600).
文摘Lignocellulose is an ideal precursor for supercapacitor electrodes due to its diverse structures and abundant availability.For supercapacitors,particularly electric double-layer capacitors(EDLCs),pore structure is critical.This review summarizes advances in lignocellulose-derived hierarchical porous carbon(LHPC)for supercapacitors,focusing on pore structure and future research directions.We discuss how pore structure influences supercapacitor performance,the activation methods for creating pores in LHPC,and review studies on optimizing pore structure for high-performance supercapacitors.Hierarchical porous carbon should feature a sufficient micropore surface area along with suitable mesoporous and macroporous surfaces to enhance rate performance while maintaining capacitance.This review is expected to actively advance the selection of lignocellulosic precursors and the development of optimized pore structure models,with the ultimate goal of enabling efficient production of lignocellulose-derived hierarchical porous carbon electrodes with superior properties.
基金supported by the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(22279166)the Guangdong Basic and Applied Basic Research Foundation(2022B1515120019)。
文摘The electrochemical stability window(ESW)is crucial for determining the energy density of electric double-layer capacitors(EDLCs).However,current ESW testing protocols of EDLCs are strongly affected by artificial factors,thereby leading to unreliable result.To solve this problem,we first identify the key shortcomings of the traditional protocols by analyzing their test principles.Subsequently,taking an aqueous carbon-based EDLC as an example,we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods.With the aid of this descriptor,we propose a new ESW testing protocol,which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations.The protocol can be extended from the single electrode to the full device.This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.
基金The authors acknowledge the support from National Natural Science Foundation of China(51972168,51672124,21603096)Program for Innovative Talents and Entrepreneur in Jiangsu,State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC),and Technical Center of Nano Fabrication and Characterization of Nanjing University.
文摘For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.
基金supported by the National Natural Science Foundation of China(21203008 and 21975025)Beijing Natural Science Foundation(2172051)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Donghua University。
文摘Activated carbon(AC)in organic electrolytebased electric double-layer capacitors(EDLCs)usually suffers from low specific capacitance.Most studies on AC focus on improving its surface area and optimizing pore structures to enhance its electrochemical performance in EDLCs.Unfortunately,the interfacial microenvironment,which is composed of nanoporous carbon and the organic electrolyte confined in it,is always ignored.Herein,a simple and powerful strategy to create AC with an ionophobic surface is proposed to address the poor efficiency of the electric doublelayer process.The polar C±F bonds formed in the AC material are characterized through near-edge X-ray absorption fine structure and X-ray photoelectron spectroscopy.The ionophobic characteristic of YP-F60 s in an organic electrolyte is extensively studied via contact angle measurements and smallangle X-ray scattering spectroscopy.An EDLC constructed with YP-F60 s as the electrode and 1 mol L^(-1) tetraethylammonium tetrafluoroborate/propylene carbonate as the electrolyte demonstrates high specific capacitance,low internal resistance,and excellent cycling stability.Our results successfully demonstrate the importance of the interfacial microenvironment of AC and its confined electrolyte to the electrochemical performance of EDLCs.Our work also offers new perspectives on the use of the CF;plasma technique to fabricate low-cost superior carbon for EDLCs.
基金supported by the National Natural Science Foundation of China(Nos.91963202,52072372,and 52232007).
文摘The rational design of electrodes is the key to achieving ultrahigh-power performance in electrochemical energy storage devices.Recently,we have constructed well-organized and integrated three-dimensional(3D)carbon tube(CT)grids(3D-CTGs)using a 3D porous anodic aluminum oxide template-assisted method as electrodes of electrical double-layer capacitors(EDLCs),showing excellent frequency response performance.The unique design warrants fast ion migration channels,excellent electronic conductivity,and good structural stability.This study achieved one of the highest carbon-based ultrahigh-power EDLCs with the 3D-CTG electrodes,resulting in ultrahigh power of 437 and 1708 W·cm−3 with aqueous and organic electrolytes,respectively.Capacitors constructed with these electrodes would have important application prospects in the ultrahigh-power output.The rational design and fabrication of the 3D-CTGs electrodes have demonstrated their capability to build capacitors with ultrahighpower performance and open up new possibilities for applications requiring high-power output.
基金supported by a Scientific Research Grant from the Japan Society for the Promotion of Science and the Special Coordination Fund for Promoting Science and Technology from the Japanese Ministry of Education, Culture, Sports, Science and Technology and a grant for Scientific Research on Priority Areas from the University of Miyazaki
文摘The space-charge distributions of electric double-layer capacitors （EDLCs）, which are energy storage devices, were examined with the pulsed electroacoustic （PEA） method. It was found that the experimental results could be influenced by the reflection and penetration of sound waves when the space-charge dis- tributions of EDLCs were measured with the PEA method. This is because EDLCs have a five-layer structure consisting of three materials （aluminum, cellulose, and activated carbon）. We calculated the reflection wave components that influenced the charge density through the acoustic impedance and the relative permittivity of the materials. In this way, we found that the changes in the space-charge distributions of EDLCs and their charge characteristics corresponded closely. We determined that measuring the space- charge distributions with the PEA method was effective for evaluating the charge accumulation of EDLCs. In this study, a polarized electrode was prepared for use in EDLCs. The ratio of the surface area to the average pore diameter of the polarized electrode was measured with the nitrogen adsorption method at 77 K. The relationship between the ratio of the surface area to the average pore size and the space-charge distributions of EDLCs is also discussed in this paper.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074213 and 11574108)the National Key R&D Program of China(Grant No.2022YFA1403103)+2 种基金the Major Basic Program of Natural Science Foundation of Shandong Province(Grant No.ZR2021ZD01)the Natural Science Foundation of Shandong Province(Grant No.ZR2023MA082)the Project of Introduction and Cultivation for Young Innovative Talents in Colleges and Universities of Shandong Province。
文摘Two-dimensional double-layer honeycomb(DLHC)materials are known for their diverse physical properties,but superconductivity has been a notably absent characteristic in this structure.We address this gap by investigating M_(2)N_(2)(M=Nb,Ta)with DLHC structure using first-principles calculations.Our results show that M_(2)N_(2)are stable and metallic,exhibiting superconducting behavior.Specifically,Nb_(2)N_(2)and Ta_(2)N_(2)display superconducting transition temperatures of 6.8 K and 8.8 K,respectively.Their electron-phonon coupling is predominantly driven by the coupling between metal d-orbitals and low-frequency metal-dominated vibration modes.Interestingly,two compounds also exhibit non-trivial band topology.Thus,M_(2)N_(2)are promising platforms for studying the interplay between topology and superconductivity and fill the gap in superconductivity research for DLHC materials.
基金supported by the Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the National Natural Science Foundation of China(Key Program)(52131306,52122209,52403001)+1 种基金the Project on National Key R&D Program of China(2021YFB2400400)the Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University。
文摘Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
文摘Modern power electronics,from electric vehicles to renewable energy systems,demand capacitors that can reliably store high energy at elevated temperatures.Polymer dielectrics are widely used in capacitors due to their high breakdown strength and ease of processing,but they traditionally suffer from poor energy density at high temperatures[1-4].
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(No.20242BAB25223,20232BCJ23025,20232BCJ25040,20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594).
文摘Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.
