Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-l...Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.展开更多
Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appea...Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness,high conductivity and intrinsic flexibility.However,the electrolyte/electrode interfacial contact and anti-freezing properties of current hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors.Here,we report a class of hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance.The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode.Meanwhile,the cooperative solvation of ZnCl2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures.More significantly,the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance,delivering high-energy density of 39 Wh kg^(-1)at-60°C with capacity retention of 98.7%over 10,000 cycles.With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte,the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at-60°C.This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.展开更多
Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Comp...Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Compared to Li^(+) storage,Na^(+) storage makes higher demands on the structural optimization of perovskite bismuth ferrite(BiFeO_(3)).We propose a novel strategy of defect engineering on BiFeO_(3) through Na and V codoping for high-efficiency Na^(+) storage,to reveal the roles of oxygen vacancies and V ions played in the enhanced electrochemical energy storage performances of Na-ion capacitors.The formation of the oxygen vacancies in the Na and V codoped BiFeO_(3)(denoted as NV-BFO),is promoted by Na doping and suppressed by V doping,which can be demonstrated by XPS and EPR spectra.By the first-principles calculations,the oxygen vacancies and V ions in NV-BFO are confirmed to substantially lower the Na^(+)migration energy barriers through the space and electric field effects,to effectively promote the Na^(+) transport in the crystals.Electrochemical kinetic analysis of the NV-BFO//NV-BFO capacitors indicates the dominant capacitive-controlled capacity,which depends on fast Na^(+) deintercalation-intercalation process in the NV-BFO electrode.The NV-BFO//NV-BFO capacitors open up a new avenue for developing highperformance Na-ion capacitors.展开更多
There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of t...There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of traditional rechargeable batteries with the superior power density and long life of supercapacitors(SCs).Nevertheless,the development of LICs is still hampered by limited kinetic processes and capacity mismatch between the cathode and anode.Metal-organic frameworks(MOFs)and their derivatives have received significant attention because of their extensive specific surface area,different pore structures and topologies,and customizable functional sites,making them compelling candidate materials for achieving high-performance LICs.MOF-derived carbons,known for their exceptional electronic conductivity and large surface area,provide improved charge storage and rapid ion transport.MOF-derived transition metal oxides contribute to high specific capacities and improved electrochemical stability.Additionally,MOF-derived metal compounds/carbons provide combined effects that increase both the capacitive and Faradaic reactions,leading to a superior overall performance.The review begins with an overview of the fundamental principles of LICs,followed by an exploration of synthesis strategies and ligand selection for MOF-based composite materials.It then analyzes the advantages of original MOFs and their derived materials,such as carbon materials and metal compounds,in enhancing LIC performance.Finally,the review discusses the major challenges faced by MOFs and their derivatives in LIC applications and offers future research directions and recommendations.展开更多
Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have othe...Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have other advantages such as abundant resources,high safety and environmental friendliness.However,they still face problems such as insufficient specific capacitance,a short cycling life,and narrow operating voltage and temperature ranges,which are hindering their practical use.We provide a comprehensive overview of the fundamental theory of carbon-based ZICs and summarize recent research progress from three perspectives:the carbon cathode,electrolyte and zinc anode.The influence of the structure and surface chemical properties of the carbon materials on the capacitive performance of ZICs is considered together with theoretical guidance for advancing their development and practical use.展开更多
The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived fro...The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).展开更多
Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.Howev...Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.展开更多
The orthorhombic CuNb_(2)O_(6)(O-CNO)is established as a competitive anode for lithium-ion capacitors(LICs)owing to its attractive compositional/structural merits.However,the high-temperature synthesis(>900℃)and c...The orthorhombic CuNb_(2)O_(6)(O-CNO)is established as a competitive anode for lithium-ion capacitors(LICs)owing to its attractive compositional/structural merits.However,the high-temperature synthesis(>900℃)and controversial charge-storage mechanism always limit its applications.Herein,we develop a low-temperature strategy to fabricate a nano-blocks-constructed hierarchical accordional O-CNO framework by employing multilayered Nb_(2)CT_(x)as the niobium source.The intrinsic stress-induced formation/transformation mechanism of the monoclinic CuNb_(2)O_(6)to O-CNO is tentatively put forward.Furthermore,the integrated phase conversion and solid solution lithium-storage mechanism is reasonably unveiled with comprehensive in(ex)situ characterizations.Thanks to its unique structural merits and lithium-storage process,the resulted O-CNO anode is endowed with a large capacity of 150.3 mAh g^(-1)at 2.0 A g^(-1),along with long-duration cycling behaviors.Furthermore,the constructed O-CNO-based LICs exhibit a high energy(138.9 Wh kg^(-1))and power(4.0 kW kg^(-1))densities with a modest cycling stability(15.8%capacity degradation after 3000 consecutive cycles).More meaningfully,the in-depth insights into the formation and charge-storage process here can promote the extensive development of binary metal Nb-based oxides for advanced LICs.展开更多
Zinc ion hybrid capacitors(ZIHCs), which integrate the features of the high power of supercapacitors and the high energy of zinc ion batteries, are promising competitors in future electrochemical energy storage applic...Zinc ion hybrid capacitors(ZIHCs), which integrate the features of the high power of supercapacitors and the high energy of zinc ion batteries, are promising competitors in future electrochemical energy storage applications. Carbon-based materials are deemed the competitive candidates for cathodes of ZIHC due to their cost-effectiveness, high electronic conductivity, chemical inertness, controllable surface states, and tunable pore architectures. In recent years, great research efforts have been devoted to further improving the energy density and cycling stability of ZIHCs. Reasonable modification and optimization of carbon-based materials offer a remedy for these challenges. In this review, the structural design, and electrochemical properties of carbon-based cathode materials with different dimensions, as well as the selection of compatible, robust current collectors and separators for ZIHCs are discussed. The challenges and prospects of ZIHCs are showcased to guide the innovative development of carbon-based cathode materials and the development of novel ZIHCs.展开更多
Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged inter...Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.展开更多
Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nit...Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nitrogen-doped hard carbon nanofibers(NHCNFs)were prepared by a lowtemperature carbonization treatment assisted with electrospinning technology.Density functional theory analysis elucidates the incorporation of nitrogen heteroatoms with various chemical states into carbon matrix would significantly alter the total electronic configurations,leading to the robust adsorption and efficient diffusion of Na atoms on electrode interface.The obtained material carbonized at 600°C(NHCNF-600)presented a reversible specific capacity of 191.0 mAh g^(−1)and no capacity decay after 200 cycles at 1 A g^(−1).It was found that the sodium-intercalated degree had a correlation with the electrochemical impedance.A sodium-intercalated potential of 0.2 V was adopted to lower the electrochemical impedance.The constructed sodium-ion capacitor with activated carbon cathode and presodiated NHCNF-600 anode can present an energy power density of 82.1 Wh kg^(−1)and a power density of 7.0 kW kg^(−1).展开更多
Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness ...Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness and low output voltage greatly hinder the realization of high-energy-density LICs.Herein,a strategy of balancing capacity towards fastest dynamics is proposed to enable high-voltage LICs.Through electrochemical prelithiation of Nb_(2)C to be 1.1 V with 165 mAh g^(-1),Nb_(2)C//LiFePO_(4) LICs show a broadened potential window from 3.0 to 4.2 V and an according high energy density of 420 Wh kg^(-1).Moreover,the underlying mechanism between prelithiation and high voltage is disclosed by electrochemical dynamic analysis.Prelithiation declines the Nb_(2)C anode potential that facilitates electron transmission in the interlayer of two-dimensional Nb_(2)C MXene.This effect induces small drive force for Li^(+)ions deposition and hence weakens the repulsive force from adsorbed ions on the electrode surface.Benefiting from even more Li^(+)ions deposition,a higher voltage is eventually delivered.In addition,prelithiation significantly increases Coulomb efficiency of the 1st cycle from 74%to 90%,which is crucial to commercial application of LICs.展开更多
Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons...Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).展开更多
Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and s...Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and stability,organic integration from electrode design to device assembly is required.To address these challenges,a free-standing reduced graphene oxide(rGO)/carbon film with a unique sandwich structure has been designed via the assistance of vacuum-assistant filtration for lithium-ion capacitors(LICs).The graphene acts as not only a binder to construct a three-dimensional conductive network but also an active material to provide additional capacitive lithium storage sites,thus enabling fast ion/electron transport and improving the capacity.The designed rGO/hard carbon(rGO/HC)and rGO/activated carbon(rGO/AC)free-standing films exhibit enhanced specific capacities(513.7 mA h g^(-1)for rGO/HC and 102.8 mA h g^(-1)for rGO/AC)and excellent stability.Moreover,the integrated flexible quasi-solid-state rGO/AC//rGO/HC LIC devices possess a maximum energy density of 138.3 Wh kg^(-1),a high power density of 11 kW kg^(-1),and improved cycling performance(84.4%capacitance maintained after 10,000 cycles),superior to the AC//HC LIC(43.5%retention).Such a strategy enlightens the development of portable flexible LICs.展开更多
The Li-ion capacitors(LICs)develop rapidly due to their double-high features of high-energy density and high-power density.However,the relative low capacity of cathode and sluggish kinetics of anode seriously impede t...The Li-ion capacitors(LICs)develop rapidly due to their double-high features of high-energy density and high-power density.However,the relative low capacity of cathode and sluggish kinetics of anode seriously impede the development of LICs.Herein,the precisely pore-engineered and heteroatomtailored defective hierarchical porous carbons(DHPCs)as large-capacity cathode and high-rate anode to construct high-performance dual-carbon LICs have been developed.The DHPCs are prepared based on triple-activation mechanisms by direct pyrolysis of sustainable lignin with urea to generate the interconnected hierarchical porous structure and plentiful heteroatominduced defects.Benefiting from these advanced merits,DHPCs show the well-matched high capacity and fast kinetics of both cathode and anode,exhibiting large capacities,superior rate capability and long-term lifespan.Both experimental and computational results demonstrate the strong synergistic effect of pore and dopants for Li storage.Consequently,the assembled dual-carbon LIC exhibits high voltage of 4.5 V,high-energy density of 208 Wh kg^(−1),ultrahigh power density of 53.4 kW kg^(−1)and almost zerodecrement cycling lifetime.Impressively,the full device with high mass loading of 9.4 mg cm^(−2)on cathode still outputs high-energy density of 187 Wh kg^(−1),demonstrative of their potential as electrode materials for high-performance electrochemical devices.展开更多
With the advantages of high energy/power density,long cycling life and low cost,dual-carbon potassium ion hybrid capacitors(PIHCs)have great potential in the field of energy storage.Here,a novel bilayer-shelled N,O-do...With the advantages of high energy/power density,long cycling life and low cost,dual-carbon potassium ion hybrid capacitors(PIHCs)have great potential in the field of energy storage.Here,a novel bilayer-shelled N,O-doped hollow porous carbon microspheres(NOHPC)anode has been prepared by a self-template method,which is consisted of a dense thin shell and a hollow porous spherical core.Excitingly,the NOHPC anode possesses a high K-storage capacity of 325.9 mA h g^(−1)at 0.1 A g^(−1)and a capacity of 201.1 mAh g^(−1)at 5 A g^(−1)after 6000 cycles.In combination with ex situ characterizations and density functional theory calculations,the high reversible capacity has been demonstrated to be attributed to the co-doping of N/O heteroatoms and porous structure improved K+adsorption and intercalation capabilities,and the stable long-cycling performance originating from the bilayer-shelled hollow porous carbon sphere structure.Meanwhile,the hollow porous activated carbon microspheres(HPAC)cathode with a high specific surface area(1472.65 m^(2)g^(−1))deriving from etching NOHPC with KOH,contributing to a high electrochemical adsorption capacity of 71.2 mAh g^(−1)at 1 A g^(−1).Notably,the NOHPC//HPAC PIHC delivers a high energy density of 90.1 Wh kg^(−1)at a power density of 939.6 W kg^(−1)after 6000 consecutive charge-discharge cycles.展开更多
Electrochemical capacitors(ECs)with unique merits of fast charge/discharge rate and long cyclability are one of the representative electrochemical energy storage systems,possessing wide applications in power electroni...Electrochemical capacitors(ECs)with unique merits of fast charge/discharge rate and long cyclability are one of the representative electrochemical energy storage systems,possessing wide applications in power electronics and automotive transportation,etc.[1,2].Furthermore.展开更多
Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in superca...Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.展开更多
Similar to lithium-ion batteries(LIBs),during the first charge/discharge process of lithium-ion capacitors(LICs),lithium-intercalated anodes(e.g.,silicon,graphite,and hard carbon)also exhibit irreversible lithium inte...Similar to lithium-ion batteries(LIBs),during the first charge/discharge process of lithium-ion capacitors(LICs),lithium-intercalated anodes(e.g.,silicon,graphite,and hard carbon)also exhibit irreversible lithium intercalation behaviors,such as the formation of a solid electrolyte interface(SEI),which will consume Li^(+)in the electrolyte and significantly reduce the electrochemical performance of the system.Therefore,pre-lithiation is an indispensable procedure for LICs.At present,commercial LICs mostly use lithium metal as the lithium source to compensate for the irreversible capacity loss,which has the demerits of operational complexity and danger.However,the pre-lithiation strategy based on cathode sacrificial lithium salts(CSLSs)has been proposed,which has the advantages of low cost,simple operation,environmental protection,and safety.Therefore,there is an urgent need for a timely and comprehensive summary of the application of CSLSs to LICs.In this review,the important roles of pre-lithiation in LICs are detailed,and different pre-lithiation methods are reviewed and compared systematically and comprehensively.After that,we systematically discuss the pre-lithiation strategies based on CSLSs and mainly introduce the lithium extraction mechanism of CSLSs and the influence of intrinsic characteristics and doping amount of CSLSs on LICs performance.In addition,a summary and outlook are conducted,aiming to provide the essential basic knowledge and guidance for developing a new pre-lithiation technology.展开更多
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金financial support from Project funded by National Natural Science Foundation of China(52172038,22179017)funding from Dalian University of Technology Open Fund for Large Scale Instrument Equipment
文摘Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.
基金This work was supported by the Natural Science Foundation of Jiangsu Province(BK20220213)the Fundamental Research Funds of Jiangsu Key Laboratory of Biomass Energy and Material(JSBEM-S-202210 and JSBEM-S-202102).
文摘Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness,high conductivity and intrinsic flexibility.However,the electrolyte/electrode interfacial contact and anti-freezing properties of current hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors.Here,we report a class of hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance.The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode.Meanwhile,the cooperative solvation of ZnCl2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures.More significantly,the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance,delivering high-energy density of 39 Wh kg^(-1)at-60°C with capacity retention of 98.7%over 10,000 cycles.With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte,the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at-60°C.This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.
基金financial supports from National Natural Science Foundation of China(22005174 and 52271133)。
文摘Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na^(+) ions.Compared to Li^(+) storage,Na^(+) storage makes higher demands on the structural optimization of perovskite bismuth ferrite(BiFeO_(3)).We propose a novel strategy of defect engineering on BiFeO_(3) through Na and V codoping for high-efficiency Na^(+) storage,to reveal the roles of oxygen vacancies and V ions played in the enhanced electrochemical energy storage performances of Na-ion capacitors.The formation of the oxygen vacancies in the Na and V codoped BiFeO_(3)(denoted as NV-BFO),is promoted by Na doping and suppressed by V doping,which can be demonstrated by XPS and EPR spectra.By the first-principles calculations,the oxygen vacancies and V ions in NV-BFO are confirmed to substantially lower the Na^(+)migration energy barriers through the space and electric field effects,to effectively promote the Na^(+) transport in the crystals.Electrochemical kinetic analysis of the NV-BFO//NV-BFO capacitors indicates the dominant capacitive-controlled capacity,which depends on fast Na^(+) deintercalation-intercalation process in the NV-BFO electrode.The NV-BFO//NV-BFO capacitors open up a new avenue for developing highperformance Na-ion capacitors.
文摘There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of traditional rechargeable batteries with the superior power density and long life of supercapacitors(SCs).Nevertheless,the development of LICs is still hampered by limited kinetic processes and capacity mismatch between the cathode and anode.Metal-organic frameworks(MOFs)and their derivatives have received significant attention because of their extensive specific surface area,different pore structures and topologies,and customizable functional sites,making them compelling candidate materials for achieving high-performance LICs.MOF-derived carbons,known for their exceptional electronic conductivity and large surface area,provide improved charge storage and rapid ion transport.MOF-derived transition metal oxides contribute to high specific capacities and improved electrochemical stability.Additionally,MOF-derived metal compounds/carbons provide combined effects that increase both the capacitive and Faradaic reactions,leading to a superior overall performance.The review begins with an overview of the fundamental principles of LICs,followed by an exploration of synthesis strategies and ligand selection for MOF-based composite materials.It then analyzes the advantages of original MOFs and their derived materials,such as carbon materials and metal compounds,in enhancing LIC performance.Finally,the review discusses the major challenges faced by MOFs and their derivatives in LIC applications and offers future research directions and recommendations.
文摘Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have other advantages such as abundant resources,high safety and environmental friendliness.However,they still face problems such as insufficient specific capacitance,a short cycling life,and narrow operating voltage and temperature ranges,which are hindering their practical use.We provide a comprehensive overview of the fundamental theory of carbon-based ZICs and summarize recent research progress from three perspectives:the carbon cathode,electrolyte and zinc anode.The influence of the structure and surface chemical properties of the carbon materials on the capacitive performance of ZICs is considered together with theoretical guidance for advancing their development and practical use.
基金the National Natural Science Foundation of China(No.52004179)the Natural Nat-ural Science Foundation of Guangxi Province,China(No.2020GXNSFAA159015)Shanxi Water and Wood New Carbon Materials Technology Co.,Ltd.,China,and Shanxi Wote Haimer New Materials Technology Co.,Ltd,China.
文摘The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).
基金supported by the National Natural Science Foundation of China(No.52002320,and 51972267)the China Postdoctoral Science Foundation(No.2022M712574)+3 种基金the Science Foundation of Shaanxi Province(2022GD-TSLD-18,No.2023-JCZD-03)Natural Science Foundation of Shaanxi Province(No.2022GY-372,2021GY-153)Industrial Projects Foundation of Ankang Science and Technology Bureau(No.AK2020-GY02-2)the Platform Construction Projects and Technology Service Teams of Ankang University(No.2021AYPT12 and 2022TD07)。
文摘Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.
基金financially supported by the National Natural Science Foundation of China(No.52072151,52171211,52102253,52271218,and U22A20145)Taishan Scholars(No.ts201712050)+1 种基金Jinan Independent Innovative Team(2020GXRC015)Major Program of Shandong Province Natural Science Foundation(ZR2021ZD05)
文摘The orthorhombic CuNb_(2)O_(6)(O-CNO)is established as a competitive anode for lithium-ion capacitors(LICs)owing to its attractive compositional/structural merits.However,the high-temperature synthesis(>900℃)and controversial charge-storage mechanism always limit its applications.Herein,we develop a low-temperature strategy to fabricate a nano-blocks-constructed hierarchical accordional O-CNO framework by employing multilayered Nb_(2)CT_(x)as the niobium source.The intrinsic stress-induced formation/transformation mechanism of the monoclinic CuNb_(2)O_(6)to O-CNO is tentatively put forward.Furthermore,the integrated phase conversion and solid solution lithium-storage mechanism is reasonably unveiled with comprehensive in(ex)situ characterizations.Thanks to its unique structural merits and lithium-storage process,the resulted O-CNO anode is endowed with a large capacity of 150.3 mAh g^(-1)at 2.0 A g^(-1),along with long-duration cycling behaviors.Furthermore,the constructed O-CNO-based LICs exhibit a high energy(138.9 Wh kg^(-1))and power(4.0 kW kg^(-1))densities with a modest cycling stability(15.8%capacity degradation after 3000 consecutive cycles).More meaningfully,the in-depth insights into the formation and charge-storage process here can promote the extensive development of binary metal Nb-based oxides for advanced LICs.
基金the financial support from the National Natural Science Foundation of China (22108044)the 111 Project (B20088)+3 种基金the Fundamental Research Funds for the Central Universities (2572022DJ02)the Research and Development Program in Key Fields of Guangdong Province (2020B1111380002)the Basic Research and Applicable Basic Research in Guangzhou City (202201010290)the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery (2021GDKLPRB07)。
文摘Zinc ion hybrid capacitors(ZIHCs), which integrate the features of the high power of supercapacitors and the high energy of zinc ion batteries, are promising competitors in future electrochemical energy storage applications. Carbon-based materials are deemed the competitive candidates for cathodes of ZIHC due to their cost-effectiveness, high electronic conductivity, chemical inertness, controllable surface states, and tunable pore architectures. In recent years, great research efforts have been devoted to further improving the energy density and cycling stability of ZIHCs. Reasonable modification and optimization of carbon-based materials offer a remedy for these challenges. In this review, the structural design, and electrochemical properties of carbon-based cathode materials with different dimensions, as well as the selection of compatible, robust current collectors and separators for ZIHCs are discussed. The challenges and prospects of ZIHCs are showcased to guide the innovative development of carbon-based cathode materials and the development of novel ZIHCs.
基金financially supported by the National Natural Science Foundation of China(Nos.21873026,21573061,21773059)。
文摘Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.
基金supported by the National Natural Science Foundation of China(No.51907193,51822706,and 51777200)the Key Research Program of Frontier Sciences,CAS(No.ZDBS-LY-JSC047)the Youth Innovation Promotion Association,CAS(No.2020145)
文摘Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nitrogen-doped hard carbon nanofibers(NHCNFs)were prepared by a lowtemperature carbonization treatment assisted with electrospinning technology.Density functional theory analysis elucidates the incorporation of nitrogen heteroatoms with various chemical states into carbon matrix would significantly alter the total electronic configurations,leading to the robust adsorption and efficient diffusion of Na atoms on electrode interface.The obtained material carbonized at 600°C(NHCNF-600)presented a reversible specific capacity of 191.0 mAh g^(−1)and no capacity decay after 200 cycles at 1 A g^(−1).It was found that the sodium-intercalated degree had a correlation with the electrochemical impedance.A sodium-intercalated potential of 0.2 V was adopted to lower the electrochemical impedance.The constructed sodium-ion capacitor with activated carbon cathode and presodiated NHCNF-600 anode can present an energy power density of 82.1 Wh kg^(−1)and a power density of 7.0 kW kg^(−1).
基金financial supported from the National Natural Science Foundation of China (Nos. 51977185 and 51972277)the financial supported from Southwest Jiaotong University Science and Technology Rising Star Program (No. 2682021CG021)
文摘Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness and low output voltage greatly hinder the realization of high-energy-density LICs.Herein,a strategy of balancing capacity towards fastest dynamics is proposed to enable high-voltage LICs.Through electrochemical prelithiation of Nb_(2)C to be 1.1 V with 165 mAh g^(-1),Nb_(2)C//LiFePO_(4) LICs show a broadened potential window from 3.0 to 4.2 V and an according high energy density of 420 Wh kg^(-1).Moreover,the underlying mechanism between prelithiation and high voltage is disclosed by electrochemical dynamic analysis.Prelithiation declines the Nb_(2)C anode potential that facilitates electron transmission in the interlayer of two-dimensional Nb_(2)C MXene.This effect induces small drive force for Li^(+)ions deposition and hence weakens the repulsive force from adsorbed ions on the electrode surface.Benefiting from even more Li^(+)ions deposition,a higher voltage is eventually delivered.In addition,prelithiation significantly increases Coulomb efficiency of the 1st cycle from 74%to 90%,which is crucial to commercial application of LICs.
基金the financial support from the National Natural Science Foundation of China(22108044,22208061)the Research and Development Program in Key Fields of Guangdong Province(2020B1111380002)+1 种基金the Basic Research and Applicable Basic Research in Guangzhou City(202201010290)the financial support from the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery(2021GDKLPRB07)。
文摘Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).
基金financially supported by the National Natural Science Foundation of China(52077207 and 51907193)the Key Research Program of Frontier Sciences,CAS(ZDBS-LY-JSC047)the Youth Innovation Promotion Association CAS(2020145)。
文摘Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and stability,organic integration from electrode design to device assembly is required.To address these challenges,a free-standing reduced graphene oxide(rGO)/carbon film with a unique sandwich structure has been designed via the assistance of vacuum-assistant filtration for lithium-ion capacitors(LICs).The graphene acts as not only a binder to construct a three-dimensional conductive network but also an active material to provide additional capacitive lithium storage sites,thus enabling fast ion/electron transport and improving the capacity.The designed rGO/hard carbon(rGO/HC)and rGO/activated carbon(rGO/AC)free-standing films exhibit enhanced specific capacities(513.7 mA h g^(-1)for rGO/HC and 102.8 mA h g^(-1)for rGO/AC)and excellent stability.Moreover,the integrated flexible quasi-solid-state rGO/AC//rGO/HC LIC devices possess a maximum energy density of 138.3 Wh kg^(-1),a high power density of 11 kW kg^(-1),and improved cycling performance(84.4%capacitance maintained after 10,000 cycles),superior to the AC//HC LIC(43.5%retention).Such a strategy enlightens the development of portable flexible LICs.
基金financialy supported by National Natural Science Foundation of China(Grants 22005298,22125903,51872283,22075279,22279137)Dalian Innovation Support Plan for High Level Talents(2019RT09)+3 种基金Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL201912,DNL201915,DNL202016,DNL202019),DICP(DICP I2020032)The Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLUDNL Fund 2021002,YLU-DNL Fund 2021009)Suzhou University Scientific Research Platform(2021XJPT07)China Postdoctoral Science Foundation(2019 M661141)
文摘The Li-ion capacitors(LICs)develop rapidly due to their double-high features of high-energy density and high-power density.However,the relative low capacity of cathode and sluggish kinetics of anode seriously impede the development of LICs.Herein,the precisely pore-engineered and heteroatomtailored defective hierarchical porous carbons(DHPCs)as large-capacity cathode and high-rate anode to construct high-performance dual-carbon LICs have been developed.The DHPCs are prepared based on triple-activation mechanisms by direct pyrolysis of sustainable lignin with urea to generate the interconnected hierarchical porous structure and plentiful heteroatominduced defects.Benefiting from these advanced merits,DHPCs show the well-matched high capacity and fast kinetics of both cathode and anode,exhibiting large capacities,superior rate capability and long-term lifespan.Both experimental and computational results demonstrate the strong synergistic effect of pore and dopants for Li storage.Consequently,the assembled dual-carbon LIC exhibits high voltage of 4.5 V,high-energy density of 208 Wh kg^(−1),ultrahigh power density of 53.4 kW kg^(−1)and almost zerodecrement cycling lifetime.Impressively,the full device with high mass loading of 9.4 mg cm^(−2)on cathode still outputs high-energy density of 187 Wh kg^(−1),demonstrative of their potential as electrode materials for high-performance electrochemical devices.
基金supported by the National Natural Science Foundation of China(Nos.21701163,21671181,21831006,and 22075268)the Fundamental Research Funds for the Central Universities(No.WK5290000003)Innovation Key Fund Project of University of Science and Technology of China(YD2060002023).
文摘With the advantages of high energy/power density,long cycling life and low cost,dual-carbon potassium ion hybrid capacitors(PIHCs)have great potential in the field of energy storage.Here,a novel bilayer-shelled N,O-doped hollow porous carbon microspheres(NOHPC)anode has been prepared by a self-template method,which is consisted of a dense thin shell and a hollow porous spherical core.Excitingly,the NOHPC anode possesses a high K-storage capacity of 325.9 mA h g^(−1)at 0.1 A g^(−1)and a capacity of 201.1 mAh g^(−1)at 5 A g^(−1)after 6000 cycles.In combination with ex situ characterizations and density functional theory calculations,the high reversible capacity has been demonstrated to be attributed to the co-doping of N/O heteroatoms and porous structure improved K+adsorption and intercalation capabilities,and the stable long-cycling performance originating from the bilayer-shelled hollow porous carbon sphere structure.Meanwhile,the hollow porous activated carbon microspheres(HPAC)cathode with a high specific surface area(1472.65 m^(2)g^(−1))deriving from etching NOHPC with KOH,contributing to a high electrochemical adsorption capacity of 71.2 mAh g^(−1)at 1 A g^(−1).Notably,the NOHPC//HPAC PIHC delivers a high energy density of 90.1 Wh kg^(−1)at a power density of 939.6 W kg^(−1)after 6000 consecutive charge-discharge cycles.
基金financially supported by the National Natural Science Foundation of China(22125903,51872283,22005298)。
文摘Electrochemical capacitors(ECs)with unique merits of fast charge/discharge rate and long cyclability are one of the representative electrochemical energy storage systems,possessing wide applications in power electronics and automotive transportation,etc.[1,2].Furthermore.
基金We are grateful to National Natural Science Foundation of China(Grant No.22375056,52272163)the Key R&D Program of Hebei(Grant No.216Z1201G)+1 种基金Natural Science Foundation of Hebei Province(Grant No.E2022208066,B2021208014)Key R&D Program of Hebei Technological Innovation Center of Chiral Medicine(Grant No.ZXJJ20220105).
文摘Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.
基金supported by the National Natural Science Foundation of China[grant number 22005318,22075303]the Western Young Scholars Foundations of Chinese Academy of Sciences,the Science Fund of Shandong Laboratory of Yantai Advanced Materials and Green Manufacturing(AMGM2022A02)the Provincial Youth Science and Technology Fund Program of Gansu Province[Project No.21JR7RA092].
文摘Similar to lithium-ion batteries(LIBs),during the first charge/discharge process of lithium-ion capacitors(LICs),lithium-intercalated anodes(e.g.,silicon,graphite,and hard carbon)also exhibit irreversible lithium intercalation behaviors,such as the formation of a solid electrolyte interface(SEI),which will consume Li^(+)in the electrolyte and significantly reduce the electrochemical performance of the system.Therefore,pre-lithiation is an indispensable procedure for LICs.At present,commercial LICs mostly use lithium metal as the lithium source to compensate for the irreversible capacity loss,which has the demerits of operational complexity and danger.However,the pre-lithiation strategy based on cathode sacrificial lithium salts(CSLSs)has been proposed,which has the advantages of low cost,simple operation,environmental protection,and safety.Therefore,there is an urgent need for a timely and comprehensive summary of the application of CSLSs to LICs.In this review,the important roles of pre-lithiation in LICs are detailed,and different pre-lithiation methods are reviewed and compared systematically and comprehensively.After that,we systematically discuss the pre-lithiation strategies based on CSLSs and mainly introduce the lithium extraction mechanism of CSLSs and the influence of intrinsic characteristics and doping amount of CSLSs on LICs performance.In addition,a summary and outlook are conducted,aiming to provide the essential basic knowledge and guidance for developing a new pre-lithiation technology.