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
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
In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strat...In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strategy utilizing high-electronegativity N(χ=3.04)to modulate local electronic domains and stabilize amorphous Mo–Se coordination(N/Mo-Se).Through self-polymerization and tunable selenization,N-doped carbon(NC)nanospheres encapsulating N-stabilized amorphous Mo-Se clusters(N/Mo-Se@NC)are successfully constructed.Theoretical and experimental analyses reveal that N-optimization effectively reconstructs the electronic distribution of Mo–Se coordination via strong covalent Mo–N bonds.This significantly enhances the covalency of Mo-Se clusters and induces localized electronic domains,thereby substantially suppressing polyselenide dissolution/shuttle during cycling.Concurrently,the amorphous N/Mo-Se clusters provide isotropic ion diffusion pathways,and together with the threedimensional(3D)conductive networks of the NC,they jointly optimize charge transfer kinetics.The N/Mo-Se@NC anode exhibits a high reversible capacity of 328.7 mAh g^(-1)after 5000 cycles,even at 10.0 A g^(-1),with a remarkable capacity retention of 110%.The assembled N/Mo-Se@NC//AC SIHCs achieve high energy/power densities(236.1 Wh kg^(-1)/9990 W kg^(-1)),demonstrating superior comprehensive performance compared to most previously reported anodes.This study,through high-electronegativity atom modulation and amorphization engineering,opens new avenues for designing highly stable and high-rate Na^(+) storage materials.展开更多
Carbon materials hold the great promise for application in energy storage devices owing to their low cost, high thermal/chemical stability, and high electrical conductivity. However, it remains challenging to synthesi...Carbon materials hold the great promise for application in energy storage devices owing to their low cost, high thermal/chemical stability, and high electrical conductivity. However, it remains challenging to synthesize high-performance carbon electrodes in a simple, scalable and sustainable way. Here, we report a facile method for scalable synthesis of porous carbon anode by using cheap and easily accessible zeolitic imidazolate framework-8 as a template and polyvinylpyrrolidone as an additional carbon source. The obtained porous carbon shows the macroscopic sheet-like morphology, which has the highly disordered structure, expanded interlayer spacing, abundant pore structure, and nitrogen doping properties. This porous carbon anode is demonstrated to have the excellent K^(+) charge storage properties in specific capacity, rate capability, and cycling stability. A potassium-ion capacitor assembled by using this porous carbon as the anode, delivers a maximum energy density of 85.12 Wh/kg and power density of 11860 W/kg as well as long cycle life exceeding 3000 cycles. This represents a critical advance in the design of low cost and scalable carbon material for applications in energy storage devices.展开更多
We investigate the dynamic responses of the series parallel-plate mesoscopic capacitors to a time-dependent external voltage. The results indicate that the quantum coherence between two capacitors strongly depends on ...We investigate the dynamic responses of the series parallel-plate mesoscopic capacitors to a time-dependent external voltage. The results indicate that the quantum coherence between two capacitors strongly depends on the frequency of the external voltage and the distance between the two capacitors （c-c distance）. The behaviors of the series capacitance incompletely follow the Kirchhoff＇s laws; only in the low frequency case or the limit of the c-c distance, the capacitance approaches to the classical series capacitance. In addition, the real part of the frequency-dependent capacitance shows a maximum and a minimum, which appear around the peak of the imaginary part. These phenomena may be associated with the plasmon excitation in the mesoscopic capacitors.展开更多
Metal-insulator-metal aluminium electrolytic capacitors(MIM-AECs)combine high capacity-density and high breakdown field strength of solid AECs with high-frequency responsibility,wide workingtemperature window and wate...Metal-insulator-metal aluminium electrolytic capacitors(MIM-AECs)combine high capacity-density and high breakdown field strength of solid AECs with high-frequency responsibility,wide workingtemperature window and waterproof properties of MIM nanocapacitors.However,interfacial atomic diffusion poses a major obstacle,preventing the high-voltage MIM-AECs exploitation and thereby hampering their potential and advantages in high-power and high-energy-density applications.Here,an innovative high-voltage MIM-AECs were fabricated.The AlPO_(4)buffer layer is formed on AlO(OH)/AAO/Al surface by using H_(3)PO_(4)treatment,then a stable van der Waals(vdW)SnO_(2)/AlPO_(4)/AAO/Al multilayer was constructed via atomic layer deposition(ALD)technology.Due to higher diffusion barrier and lower carrier migration of SnO_(2)/AlPO_(4)/AAO interfaces,Sn atom diffusion is inhibited and carrier acceleration by electric field is weakened,guaranteeing high breakdown field strength of dielectric AAO and avoiding local breakdown risks.Through partial etching to hydrated AlO(OH)by H_(3)PO_(4)treatment,the tunnel was further opened up to facilitate subsequent ALD-SnO_(2)entry,thus obtaining a high SnO_(2)coverage.The SnO_(2)/AlPO_(4)/AAO/Al capacitors show a comprehensive performance in high-voltage(260 V),hightemperature(335℃),high-humidity(100%RH)and high-frequency response(100 k Hz),outperforming commercial solid-state AECs,and high-energy density(8.6μWh/cm^(2)),markedly exceeding previously reported MIM capacitors.The work lays the foundation for next-generation capacitors with highvoltage,high-frequency,high-temperature and high-humidity resistance.展开更多
In the context of rapid economic development,the pursuit of sustainable energy solutions has become a major challenge.Lithium-ion capacitors(LICs),which integrate the high energy density of lithium-ion batteries with ...In the context of rapid economic development,the pursuit of sustainable energy solutions has become a major challenge.Lithium-ion capacitors(LICs),which integrate the high energy density of lithium-ion batteries with the high power density of supercapacitors,have emerged as promising candidates.However,challenges such as poor capacity matching and limited energy density still hinder their practical application.Carbon nanofibers(CNFs),with their high specific surface area,excellent electrical conductivity,mechanical flexibility,and strong compatibility with active materials,are regarded as ideal electrode frameworks for LICs.This review summarizes key strategies to improve the electrochemical performance of CNF-based LICs,including structural engineering,heteroatom doping,and hybridization with transition metal oxides.The underlying mechanisms of each approach are discussed in detail,with a focus on their roles in improving capacitance,energy density,and cycling stability.This review aims to provide insights into material design and guide future research toward high-performance LICs for next-generation energy storage applications.展开更多
Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operati...Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.展开更多
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.
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.
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(Grant Nos.20242BAB25223,20232BCJ23025,20232BCJ25040,and 20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594)。
文摘In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strategy utilizing high-electronegativity N(χ=3.04)to modulate local electronic domains and stabilize amorphous Mo–Se coordination(N/Mo-Se).Through self-polymerization and tunable selenization,N-doped carbon(NC)nanospheres encapsulating N-stabilized amorphous Mo-Se clusters(N/Mo-Se@NC)are successfully constructed.Theoretical and experimental analyses reveal that N-optimization effectively reconstructs the electronic distribution of Mo–Se coordination via strong covalent Mo–N bonds.This significantly enhances the covalency of Mo-Se clusters and induces localized electronic domains,thereby substantially suppressing polyselenide dissolution/shuttle during cycling.Concurrently,the amorphous N/Mo-Se clusters provide isotropic ion diffusion pathways,and together with the threedimensional(3D)conductive networks of the NC,they jointly optimize charge transfer kinetics.The N/Mo-Se@NC anode exhibits a high reversible capacity of 328.7 mAh g^(-1)after 5000 cycles,even at 10.0 A g^(-1),with a remarkable capacity retention of 110%.The assembled N/Mo-Se@NC//AC SIHCs achieve high energy/power densities(236.1 Wh kg^(-1)/9990 W kg^(-1)),demonstrating superior comprehensive performance compared to most previously reported anodes.This study,through high-electronegativity atom modulation and amorphization engineering,opens new avenues for designing highly stable and high-rate Na^(+) storage materials.
文摘为了评价PIC猪的胴体性状和肉质性状,试验屠宰了健康的PIC猪9头,测定了其胴体性状、肉质性状和肌肉成分等相关指标,并分析了各性状间的相关性。结果表明,宰前活重为123.78 kg的PIC猪,屠宰率为75.58%,瘦肉率为60.8%,平均背膘厚25.62 mm,眼肌面积45.95 cm 2,滴水损失2.14%,嫩度43.56N,肌内脂肪含量2.23%,总氨基酸含量20.3%,饱和脂肪酸含量41.54%,总不饱和脂肪酸含量58.44%。性状间相关性分析表明,PIC猪的宰前活重与屠宰率呈显著正相关(P<0.05),肌内脂肪与MUFA呈极显著正相关(P<0.01),与PUFA呈极显著负相关(P<0.01),与水分呈显著负相关(P<0.05)。肌内脂肪与水分间的相关系数为-0.718,二者间线性模型Y=-0.9985x+75.299,决定系数R^(2)为0.5153。
基金supported by National Natural Science Foundation of China (No. 51902188)Key Research&Development Program of Shandong Province (No. 2019JZZY010355)+1 种基金Natural Science Foundation of Jiangsu Province (No. BK20190207)the CAS Key Laboratory of Carbon Materials (No. KLCMKFJJ2006)。
文摘Carbon materials hold the great promise for application in energy storage devices owing to their low cost, high thermal/chemical stability, and high electrical conductivity. However, it remains challenging to synthesize high-performance carbon electrodes in a simple, scalable and sustainable way. Here, we report a facile method for scalable synthesis of porous carbon anode by using cheap and easily accessible zeolitic imidazolate framework-8 as a template and polyvinylpyrrolidone as an additional carbon source. The obtained porous carbon shows the macroscopic sheet-like morphology, which has the highly disordered structure, expanded interlayer spacing, abundant pore structure, and nitrogen doping properties. This porous carbon anode is demonstrated to have the excellent K^(+) charge storage properties in specific capacity, rate capability, and cycling stability. A potassium-ion capacitor assembled by using this porous carbon as the anode, delivers a maximum energy density of 85.12 Wh/kg and power density of 11860 W/kg as well as long cycle life exceeding 3000 cycles. This represents a critical advance in the design of low cost and scalable carbon material for applications in energy storage devices.
基金supported by the National Natural Science Foundation of China(Grant No.11304276)the Natural Science Foundation of Guangdong Province,China(Grant No.2014A030307035)+1 种基金the Cultivation of Innovative Talents in Colleges and Universities of Guangdong Province,China(Grant No.LYM10098)the Doctor Subject Foundation of Lingnan Normal University of China(Grant No.ZL1004)
文摘We investigate the dynamic responses of the series parallel-plate mesoscopic capacitors to a time-dependent external voltage. The results indicate that the quantum coherence between two capacitors strongly depends on the frequency of the external voltage and the distance between the two capacitors （c-c distance）. The behaviors of the series capacitance incompletely follow the Kirchhoff＇s laws; only in the low frequency case or the limit of the c-c distance, the capacitance approaches to the classical series capacitance. In addition, the real part of the frequency-dependent capacitance shows a maximum and a minimum, which appear around the peak of the imaginary part. These phenomena may be associated with the plasmon excitation in the mesoscopic capacitors.
基金supported by the National Natural Science Foundation of China(52477221,52202296)the Natural Science Foundation of Shaanxi Province(2023KXJ-246,2022JQ-048)。
文摘Metal-insulator-metal aluminium electrolytic capacitors(MIM-AECs)combine high capacity-density and high breakdown field strength of solid AECs with high-frequency responsibility,wide workingtemperature window and waterproof properties of MIM nanocapacitors.However,interfacial atomic diffusion poses a major obstacle,preventing the high-voltage MIM-AECs exploitation and thereby hampering their potential and advantages in high-power and high-energy-density applications.Here,an innovative high-voltage MIM-AECs were fabricated.The AlPO_(4)buffer layer is formed on AlO(OH)/AAO/Al surface by using H_(3)PO_(4)treatment,then a stable van der Waals(vdW)SnO_(2)/AlPO_(4)/AAO/Al multilayer was constructed via atomic layer deposition(ALD)technology.Due to higher diffusion barrier and lower carrier migration of SnO_(2)/AlPO_(4)/AAO interfaces,Sn atom diffusion is inhibited and carrier acceleration by electric field is weakened,guaranteeing high breakdown field strength of dielectric AAO and avoiding local breakdown risks.Through partial etching to hydrated AlO(OH)by H_(3)PO_(4)treatment,the tunnel was further opened up to facilitate subsequent ALD-SnO_(2)entry,thus obtaining a high SnO_(2)coverage.The SnO_(2)/AlPO_(4)/AAO/Al capacitors show a comprehensive performance in high-voltage(260 V),hightemperature(335℃),high-humidity(100%RH)and high-frequency response(100 k Hz),outperforming commercial solid-state AECs,and high-energy density(8.6μWh/cm^(2)),markedly exceeding previously reported MIM capacitors.The work lays the foundation for next-generation capacitors with highvoltage,high-frequency,high-temperature and high-humidity resistance.
文摘In the context of rapid economic development,the pursuit of sustainable energy solutions has become a major challenge.Lithium-ion capacitors(LICs),which integrate the high energy density of lithium-ion batteries with the high power density of supercapacitors,have emerged as promising candidates.However,challenges such as poor capacity matching and limited energy density still hinder their practical application.Carbon nanofibers(CNFs),with their high specific surface area,excellent electrical conductivity,mechanical flexibility,and strong compatibility with active materials,are regarded as ideal electrode frameworks for LICs.This review summarizes key strategies to improve the electrochemical performance of CNF-based LICs,including structural engineering,heteroatom doping,and hybridization with transition metal oxides.The underlying mechanisms of each approach are discussed in detail,with a focus on their roles in improving capacitance,energy density,and cycling stability.This review aims to provide insights into material design and guide future research toward high-performance LICs for next-generation energy storage applications.
文摘Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.
