Extensively explored for their distinctive pseudocapacitance characteristics,MXenes,a distinguished group of 2D materials,have led to remarkable achievements,particularly in the realm of energy storage devices.This wo...Extensively explored for their distinctive pseudocapacitance characteristics,MXenes,a distinguished group of 2D materials,have led to remarkable achievements,particularly in the realm of energy storage devices.This work presents an innovative Pseudocapacitive Sensor.The key lies in switching the energy storage kinetics from pseudocapacitor to electrical double layer capacitor by employing the change of local pH(-log[H^(+)])in MXene-based flexible supercapacitors during bending.Pseudocapacitive sensing is observed in acidic electrolyte but absent in neutral electrolyte.Applied shearing during bending causes liquid-crystalline MXene sheets to increase in their degree of anisotropic alignment.With blocking of H+mobility due to the higher diffusion barrier,local pH increases.The electrochemical energy storage kinetics transits from Faradaic chemical protonation(intercalation)to non-Faradaic physical adsorption.We utilize the phenomenon of capacitance change due to shifting energy storage kinetics for strain sensing purposes.The developed highly sensitive Pseudocapacitive Sensors feature a remarkable gauge factor(GF)of approximately 1200,far surpassing conventional strain sensors(GF:~1 for dielectric-cap sensor).The introduction of the Pseudocapacitive Sensor represents a paradigm shift,expanding the application of pseudocapacitance from being solely confined to energy devices to the realm of multifunctional electronics.This technological leap enriches our understanding of the pseudocapacitance mechanism of MXenes,and will drive innovation in cutting-edge technology areas,including advanced robotics,implantable biomedical devices,and health monitoring systems.展开更多
The progression of anodes has markedly promoted the advancement of lithium-ion batteries(LIBs).Typical LIBs using carbon anodes cannot meet the continuously increasing demands for qualified safety and longevity.Spinel...The progression of anodes has markedly promoted the advancement of lithium-ion batteries(LIBs).Typical LIBs using carbon anodes cannot meet the continuously increasing demands for qualified safety and longevity.Spinel lithium titanate(LTO)is a strong contender to replace graphite anodes due to its optimal zero-strain merit and outstanding structural stability.Nevertheless,low reversible capacity and poor rate performance hinder the widespread application of LTO.Amazingly,the promising pseudocapacitive effect enables LTO to surmount the limit of theoretical capacity via boosted surface Li storage,contributing to observably upgraded energy and power densities in a wide temperature range.By leveraging the synergistic effect of multiple modification strategies to create additional active sites,the pseudocapacitive response of LTO can be markedly enhanced.This paper reviews the progress of pseudocapacitive LTO for the first time.We highlight the zero-strain characteristic and pseudocapacitance mechanism of LTO and review the design strategies of pseudocapacitive LTO.Significative issues for further developing pseudocapacitive LTO are proposed.It is worth noting that the pseudocapacitive contribution can greatly improve the low-temperature electrochemical performances of LTO.We anticipate that more efforts will be aroused to study the advanced pseudocapacitive LTO to accelerate the development of next-generation LIBs and energy storage devices.展开更多
Developing an efficient approach of transforming biomass waste to functional carbon-based electrode materials applied in supercapacitor offers an important and high value-added practical application due to the abundan...Developing an efficient approach of transforming biomass waste to functional carbon-based electrode materials applied in supercapacitor offers an important and high value-added practical application due to the abundance and considerable low price of biomass wastes.Herein,a hierarchical carbon functionalized with electrochemical-active oxygen-containing groups was fabricated by microwave treatment from the biomass waste of camellia oleifera.The obtained mesoporous carbon(MAC)owns nanosheet morphology,rich mesoporosity,large surface area(1726 m2/g)and very high oxygenic functionalities(16.2 wt%)with pseudocapacitive activity.Prepared electrode of supercapacitor and tested in 2.0 M H2 SO4,the MAC exhibits an obvious pseudocapacitive activity and achieved a superior supercapacitive performance to that of directly activated carbon(DAC-800)including high specific capacitance(367 F/g vs.298 F/g)and better rate performance(66%vs.44%).The symmetrical supercapacitor based on MAC shows a high capacity of275 F/g,large energy density of 9.55 Wh/kg(at power density of 478 W/kg)and excellent cycling stability with 99%capacitance retention after 10000 continuous charge-discharge,endowing the obtained MAC a promising functional material for electrochemical energy storage.展开更多
Lithium ion capacitors(LICs)have been widely used as energy storage devices due to their high energy density and high power density.For LICs,pre-lithiation of negative electrode is necessary.In this work,we employ a b...Lithium ion capacitors(LICs)have been widely used as energy storage devices due to their high energy density and high power density.For LICs,pre-lithiation of negative electrode is necessary.In this work,we employ a bifunctional Li6CoO4(LCO)as cathodic pre-lithiation reagent to improve the electrochemical performance of LICs.The synthesized LCO exhibited high first charge specific capacity of 721 mAh g-1and extremely low initial coulombic efficiency of 3.19%,providing sufficient Li+ for the pre-lithiation of negative electrode in the first charge.Simultaneously,Li6–xCoOy is generated from LCO during the first charge process,which exhibits pseudocapacitive property and contributes to capacity in form of surface capacitance during subsequent cycles,increasing the capacity of capacitive positive electrode.With the appropriate amounts of addition to the positive side in LICs,this bifunctional prelithiation reagent LCO shows significantly improved the electrochemical performance with the energy density of 78.5 Wh kg-1after 300 cycles between 2.0 and 4.2 V at 250 mA g-1.展开更多
To improve rate and cycling performance of manganese oxide anode material,a precipitation method was combined with thermal annealing to prepare the Mn O/Mn3O4/Se Ox(x=0,2)hybrid anode by controlling the reaction tempe...To improve rate and cycling performance of manganese oxide anode material,a precipitation method was combined with thermal annealing to prepare the Mn O/Mn3O4/Se Ox(x=0,2)hybrid anode by controlling the reaction temperature of Mn2O3 and Se powders.At 3 A/g,the synthesized Mn O/Mn3O4/Se Ox anode delivers a discharge capacity of 1007 m A·h/g after 560 cycles.A cyclic voltammetry quantitative analysis reveals that 89.5%pseudocapacitive contribution is gained at a scanning rate of 2.0 m V/s,and the test results show that there is a significant synergistic effect between Mn O and Mn3O4 phases.展开更多
Sodium-organic batteries utilizing natural abundance of sodium element and renewable active materials gain great attentions for grid-scale applications.However,the development is still limited by lack of suitable orga...Sodium-organic batteries utilizing natural abundance of sodium element and renewable active materials gain great attentions for grid-scale applications.However,the development is still limited by lack of suitable organic cathode materials with high electronic conductivity that can be operated stably in liquid electrolyte.Herein,we present 5,15-bis(ethynyl)-10,20-diphenylporphyrin(DEPP)and[5,15-bis(ethynyl)-10,20-diphenylporphinato]copper(II)(CuDEPP)as new cathodes for extremely stable sodium-organic batteries.The copper(II)ion partially contributes the charge storage and significantly stabilizes the structure of porphyrin complex for electrochemical energy storage.In situ electrochemical stabilization of organic cathode with a lower charging current density was identified which enables both improved high energy density and power density.An excellent longterm cycling stability up to 600 cycles and an extremely high power density of 28 kW kg−1 were achieved for porphyrin-based cathode.This observation would open new pathway for developing highly stable sodium-organic cathode for electrochemical energy storage.展开更多
Lithium-ion capacitors(LICs)have attracted wide attention due to their potential of achieving merits of high-power output as well as high energy density.How-ever,the key issue of kinetics mismatch between anode and ca...Lithium-ion capacitors(LICs)have attracted wide attention due to their potential of achieving merits of high-power output as well as high energy density.How-ever,the key issue of kinetics mismatch between anode and cathode hinders the electrochemical performance of LICs.Therefore,a vanadium nitride composite with nanoparti-cles embedded in carbon matrix(VN-C)was prepared as an efficiently pseudocapacitive anode material with high electronic conductivity and fast Li-ion diffusion rate.The VN-C composites were synthesized through one-step ammonia heating treatment at different temperatures among which the sample annealed at 600℃exhibits high specific capacity(513 mAh·g^(-1)at 0.1 A·g^(-1)),outstanding rate performance(~300 mAh·g^(-1)at 10 A·g^(-1)),and excellent cyclic steadiness(negligible capacity decay over 2000 cycles)in half-cell devices.A high-performance lithium-ion capacitor device was also fabricated by using VN-C-600 as the anode and activated carbon as the cath-ode,delivering a maximum energy density of 112.6 Wh·kg^(-1)and an extreme power density of 10 kW·kg^(-1).展开更多
Pseudocapacitive materials generally offer both high capacitance and high rate capability, which has stimulated great efforts in developing the materials system and related energy storage devices. In recent years, how...Pseudocapacitive materials generally offer both high capacitance and high rate capability, which has stimulated great efforts in developing the materials system and related energy storage devices. In recent years, however, with the extensive use of nanomaterials in batteries, fast redox kinetics comparable to pseudocapacitive have been achieved in many kinds of battery materials due to the much shortened ion diffusion lengths and highly exposed surface/interface as a result of nanosize effect. Consequently, the terms"pseudocapacitive materials" and "battery materials" are becoming more and more confusing. In this review, different opinions on the definition of pseudocapacitive materials and the evolution of the definitions as well as the resulting confusion will be firstly reviewed. Then, to accurately distinguish pseudocapacitive and battery materials, method with the consideration of both the electrochemical signatures(CVs and GCD) and quantitative kinetics analysis as a supplement is proposed. Finally, we end this review by discussing the possible device configurations of asymmetric supercapacitors and hybrid supercapacitors. The present review will help understanding the differences between pseudocapacitive materials and battery materials, and thus avoiding the definition confusion.展开更多
An innovative K+vacant ternary perovskite fluoride(K_(0.89)Ni_(0.02)Co_(0.03)Mn_(0.95)F_(3.0),KNCMF-3#)anode was designed for advanced Li-ion supercapattery(i.e.,Li-ion capacitors/batteries,LIC/Bs).Owing to the conver...An innovative K+vacant ternary perovskite fluoride(K_(0.89)Ni_(0.02)Co_(0.03)Mn_(0.95)F_(3.0),KNCMF-3#)anode was designed for advanced Li-ion supercapattery(i.e.,Li-ion capacitors/batteries,LIC/Bs).Owing to the conversion/insertion dual mechanisms and fast pseudocapacitive con-trol dynamics,the KNCMF-3#electrode exhibits superior electrochemical performance,especially the excellent cycle performance(467%(229 mAh·g^(-1))/1000 cycles/2 A·g^(-1)).Moreover,the hybrid KNCMF-3#/reduced gra-phene oxide(rGO)electrode can further increase the electrochemical performance(217-97 mAh·g^(-1)/0.1-3.2 A·g^(-1),150%(197 mAh·g^(-1))/1000 cycles/2 A·g^(-1)).Also,a novel capacitor/battery cathode,activated carbon(AC)+LiFePO_(4)+graphene(AC+LFP+G),exhibits impres-sive performance(128-82 mAh·g^(-1)/0.1-3.2 A·g^(-1),84%/1000 cycles/2 A·g^(-1)).By the synergistic optimization of anode and cathode,the Li-ion supercapattery KNCMF-3#@rGO//AC+LFP+G demonstrates remarkable per-formance,for example,111.9-23.8 Wh·kg^(-1)/0.4-8.0 kW·kg^(-1)/82%/2000 cycles/5 A·g^(-1)/0-4 V,which is superior to KNCMF-3#//AC LICs,KNCMF-3#@rGO//AC LICs,KNCMF-3#//AC+LFP+G LIC/Bs.In all,the novel Li-ion supercapattery idea adds a promising per-spective to develop advanced energy storage devices.展开更多
We report a simple method for fabricating all-solid-state micro-supercapacitors, utilizing laser writing technology. Porous graphene films with three-dimensional networks induced by laser from commercial polymer was a...We report a simple method for fabricating all-solid-state micro-supercapacitors, utilizing laser writing technology. Porous graphene films with three-dimensional networks induced by laser from commercial polymer was acted as scaffold for loading MnO2, a typical pseudocapacitive materials. Using gel electrolyte, all-solid-state pseudocapacitive micro-supercapacitors were fabricated. Compare to traditional printing and lithography techniques produced micro-supercapacitors, the as-fabricated devices demonstrate high volumetric capacitances, good stability and low leakage current, indicating a scalable and facile approach for future energy storage devices in portable microelectronics.展开更多
Recent developments in the synthesis of graphene-based structures focus on continuous improvement of porous nanostructures,doping of thin films,and mechanisms for the construction of threedimensional architectures.Her...Recent developments in the synthesis of graphene-based structures focus on continuous improvement of porous nanostructures,doping of thin films,and mechanisms for the construction of threedimensional architectures.Herein,we synthesize creeper-like Ni3Si2/NiOOH/graphene nanostructures via low-pressure all-solid meltingreconstruction chemical vapor deposition.In a carbon-rich atmosphere,high-energy atoms bombard the Ni and Si surface,and reduce the free energy in the thermodynamic equilibrium of solid Ni–Si particles,considerably catalyzing the growth of Ni–Si nanocrystals.By controlling the carbon source content,a Ni3Si2 single crystal with high crystallinity and good homogeneity is stably synthesized.Electrochemical measurements indicate that the nanostructures exhibit an ultrahigh specific capacity of 835.3 C g^−1(1193.28 F g^−1)at 1 A g^−1;when integrated as an all-solidstate supercapacitor,it provides a remarkable energy density as high as 25.9 Wh kg^−1 at 750 W kg^−1,which can be attributed to the freestanding Ni3Si2/graphene skeleton providing a large specific area and NiOOH inhibits insulation on the electrode surface in an alkaline solution,thereby accelerating the electron exchange rate.The growth of the high-performance composite nanostructure is simple and controllable,enabling the large-scale production and application of microenergy storage devices.展开更多
Rechargeable aqueous zinc-ion hybrid capacitors and zincion batteries are promising safe energy storage systems.In this study,amorphous RuO2·H2O for the first time was employed to achieve fast and ultralong-life ...Rechargeable aqueous zinc-ion hybrid capacitors and zincion batteries are promising safe energy storage systems.In this study,amorphous RuO2·H2O for the first time was employed to achieve fast and ultralong-life Zn2+storage based on a pseudocapacitive storage mechanism.In the RuO2·H2O||Zn zinc-ion hybrid capacitors with Zn(CF3SO3)2 aqueous electrolyte,the RuO2·H2O cathode can reversibly store Zn2+in a voltage window of 0.4-1.6 V(vs.Zn/Zn2+),delivering a high discharge capacity of 122 mAh g?1.In particular,the zinc-ion hybrid capacitors can be rapidly charged/discharged within 36 s with a very high power density of 16.74 kW kg?1 and a high energy density of 82 Wh kg?1.Besides,the zinc-ion hybrid capacitors demonstrate an ultralong cycle life(over 10,000 charge/discharge cycles).The kinetic analysis elucidates that the ultrafast Zn2+storage in the RuO2·H2O cathode originates from redox pseudocapacitive reactions.This work could greatly facilitate the development of high-power and safe electrochemical energy storage.展开更多
Flexible pressure sensors are unprecedentedly studied on monitoring human physical activities and robotics.Simultaneously,improving the response sensitivity and sensing range of flexible pressure sensors is a great ch...Flexible pressure sensors are unprecedentedly studied on monitoring human physical activities and robotics.Simultaneously,improving the response sensitivity and sensing range of flexible pressure sensors is a great challenge,which hinders the devices’practical application.Targeting this obstacle,we developed a Ti_(3)C_(2)T_(x)-derived iontronic pressure sensor(TIPS)by taking the advantages of the high intercalation pseudocapacitance under high pressure and rationally designed structural configuration.TIPS achieved an ultrahigh sen-sitivity(S_(min)>200 kPa^(−1),S_(max)>45,000 kPa^(−1))in a broad sensing range of over 1.4 MPa and low limit of detection of 20 Pa as well as stable long-term working durability for 10,000 cycles.The practical application of TIPS in physical activity monitoring and flexible robot manifested its versatile potential.This study provides a demonstration for exploring pseudocapacitive materials for building flexible iontronic sensors with ultrahigh sensitivity and sensing range to advance the development of high-performance wearable electronics.展开更多
Sodium-ion battery materials and devices are promising candidates for largescale applications,owing to the abundance and low cost of sodium sources.Emerging sodium-ion pseudocapacitive materials provide one approach f...Sodium-ion battery materials and devices are promising candidates for largescale applications,owing to the abundance and low cost of sodium sources.Emerging sodium-ion pseudocapacitive materials provide one approach for achieving high capacity at high rates,but are currently not well understood.Herein,a comprehensive overview of the fundamentals and electrochemical behaviors of vanadium-based pseudocapacitive materials for sodium-ion storage is presented.The insight of sodium-ion storage mechanisms for various vanadium-based materials,including vanadium oxides,vanadates,vanadium sulfides,nitrides,and carbides are systematically discussed and summarized.In particular,areas for further development to improve fundamental understanding of electrochemical and structural properties of materials are identified.Finally,we provide a perspective on the application of pseudocapacitive materials in high-power and high-energy sodium-ion storage devices(e.g.,sodium-ion capacitors).展开更多
The development of potential transition-metal carbide/nitride heterojunctions is hindered by overall understanding and precise modulation for heterointerface effects.Herein,we demonstrate that Mo_(2)C/Mo_(2)N heteroju...The development of potential transition-metal carbide/nitride heterojunctions is hindered by overall understanding and precise modulation for heterointerface effects.Herein,we demonstrate that Mo_(2)C/Mo_(2)N heterojunction with the precisely regulated high-quality interface can achieve marvelous rate performance and energy output via enlarging the interface-effect range and maximizing "accelerated charge" amount The heterointerface mechanism improving properties is synergistically revealed from kinetics and thermodynamics perspectives.Kinetics analysis confirms that the self-built electric field affords a robust force to drive rapid interface electrons/ions migration.The small adsorption energy,high density of states and quite low diffusion barrier thermodynamically enhance the electrochemical reaction dynamics on heterointerface.Consequently,the almost optimal performance of ultrahigh capacitance retention(85.6% even at 10 A g^(-1)) and pronounced energy output(96.4 Wh kg^(-1))in hybridsupercapacitors than other Mo_(2)C/Mo_(2)N-based materials is presented.This work gives new insight into the energy storage mechanism of heterojunction and guides the design of advanced electrodes.展开更多
Carbon is a promising capacitive electrode material for Zn-ion hybrid supercapacitors(ZHSCs),as it is low-cost,environmentally friendly,controllable and adjustable.By now,achieving both high energy and high power with...Carbon is a promising capacitive electrode material for Zn-ion hybrid supercapacitors(ZHSCs),as it is low-cost,environmentally friendly,controllable and adjustable.By now,achieving both high energy and high power with carbon electrodes is still challenging,limited by their intrinsic properties.In this work,we have designed and presented an amorphous hollow carbon bowl material with surface chemical modifications of oxygen groups to figure out these concerns.The preparation of bowl-like structures and the storage behavior between Zn^(2+)and oxygen functional groups have also been discussed.With the contributions from its unique hollow structure and surface functional groups,it can significantly enhance the electrode pseudocapacitance and the entire electrochemical performance.展开更多
As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broa...As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broader distribution of sodium[1–7].Sodium has similar electrochemical properties to lithium,and thus the concepts for the preparation of electrode materials for SIBs can be borrowed from LIBs[8,9].展开更多
Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical...Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical reaction mechanism of Zn_(2)Ti_(3)O_(8)has rarely been studied.In this work,a porous Zn_(2)Ti_(3)O_(8)anode with considerably high capacity(421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles)was reported,which is even higher than ever reported titanium-based anodes materials including Li_(4)Ti_(5)O_(12),TiO_(2)and Li_(2)ZnTi_(3)O_(8).Here,for the first time,the accurate theoretical capacity of Zn_(2)Ti_(3)O_(8)was confirmed to be 266.4 mAh/g.It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn_(2)Ti_(3)O_(8),making it possibly higher than the theoretical value.Most importantly,the porous structure of Zn_(2)Ti_(3)O_(8)not only promotes the intercalation reaction,but also induces high pseudocapacitance capacity(225.4 mAh/g),which boosts the reversible capacity.Therefore,it is the outstanding pseudocapacitance capacity of porous Zn_(2)Ti_(3)O_(8)that accounts for high actual capacity exceeding the theoretical one.This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.展开更多
The emerging Li//H_(2)battery is a promising candidate for energy storage systems to meet the demand for the worldwide transition to clean and sustainable energy.To leverage the H_(2)electrode’s advantages and decrea...The emerging Li//H_(2)battery is a promising candidate for energy storage systems to meet the demand for the worldwide transition to clean and sustainable energy.To leverage the H_(2)electrode’s advantages and decrease costs,a high areal capacity anode-free Li anode is ideal.Here we propose using a pseudocapacitive Cu(PC-Cu)substrate to accommodate the high areal capacity anode-free Li//H_(2)battery(AFLHB).The PC-Cu substrate exhibits intense electrochemical adsorption and intrinsic strong chemisorption to Li,which leads to aggregation of the Li salts so as to induce enrichment of interfacial lithiophilicity.This aids uniform Li nucleation,anion concentration,and robust SEI formation.The AFLHB displays stable cycling at a high areal capacity of 5 mAh cm^(-2)with an average coulombic efficiency of 98.80%for over 350 h.Notably,the PC-Cu substrate enables superdense Li deposition with only 7%thickness exceeding the theoretical value.Moreover,the modified substrate enables a reversible Li stripping/plating at an ultralarge areal capacity of 20 mAh cm^(-2).This work presents an interfacial lithiophilicity enrichment strategy to stabilize the cycling performance of high areal capacity AFLHB and advances this novel battery system one step closer to practical application.展开更多
Silicon(Si)has emerged as a promising anode material for lithium-ion batteries(LIBs)due to its extremely high theoretical capacity of 4200 mAh·g^(-1).However,its practical application is limited by several critic...Silicon(Si)has emerged as a promising anode material for lithium-ion batteries(LIBs)due to its extremely high theoretical capacity of 4200 mAh·g^(-1).However,its practical application is limited by several critical challenges,including severe volume expansion and poor electrical conductivity.Herein,we employ a two-dimensional(2D)oxygen modification engineering approach to fabricate 2D oxygen-functionalized CaSi_(2)(CaSi_(2)O_(x))layers.During the preparation of 2D CaSi_(2) layers,O atoms are gradually incorporated onto their surface.The resulting 2D CaSi_(2)O_(x) layers have a thickness of 3-5 nm,closely matching the theoretical thickness of 6-10 layers.When used as lithium anodes,the 2D CaSi_(2)O_(x) layers exhibit exceptional electrochemical performance,maintaining stability over 3000 cycles at an ultrahigh current density of 30 A·g^(-1).By tailoring the surface properties,their pseudocapacitive charge storage mechanism is significantly enhanced,effectively overcoming the intrinsic limitations of traditional Si anodes.This study highlights the promise of 2D surface engineering in the development of advanced materials for next-generation LIBs.展开更多
基金supported by NRF-2021M3H4A1A03047333 and NRF-2022R1F1A1075084 of the National Research Foundation(NRF)of Korea funded by the Ministry of Science and ICT,Koreasupported by Semiconductor-Secondary Battery Interfacing Platform Technology Development Project of NNFC.
文摘Extensively explored for their distinctive pseudocapacitance characteristics,MXenes,a distinguished group of 2D materials,have led to remarkable achievements,particularly in the realm of energy storage devices.This work presents an innovative Pseudocapacitive Sensor.The key lies in switching the energy storage kinetics from pseudocapacitor to electrical double layer capacitor by employing the change of local pH(-log[H^(+)])in MXene-based flexible supercapacitors during bending.Pseudocapacitive sensing is observed in acidic electrolyte but absent in neutral electrolyte.Applied shearing during bending causes liquid-crystalline MXene sheets to increase in their degree of anisotropic alignment.With blocking of H+mobility due to the higher diffusion barrier,local pH increases.The electrochemical energy storage kinetics transits from Faradaic chemical protonation(intercalation)to non-Faradaic physical adsorption.We utilize the phenomenon of capacitance change due to shifting energy storage kinetics for strain sensing purposes.The developed highly sensitive Pseudocapacitive Sensors feature a remarkable gauge factor(GF)of approximately 1200,far surpassing conventional strain sensors(GF:~1 for dielectric-cap sensor).The introduction of the Pseudocapacitive Sensor represents a paradigm shift,expanding the application of pseudocapacitance from being solely confined to energy devices to the realm of multifunctional electronics.This technological leap enriches our understanding of the pseudocapacitance mechanism of MXenes,and will drive innovation in cutting-edge technology areas,including advanced robotics,implantable biomedical devices,and health monitoring systems.
基金financially supported by the National Natural Science Foundation of China(51108455,52106264)Civil Aviation Safety Capacity Building Fund(ADSA2022026)+2 种基金Liaoning Revitalization Talents Program(XLYC2018013)Liaoning Province AppliedFoundation Research Program Project(2023JH2/101300215)Unveiled the List of Local Service Projects from Education Department of Liaoning Province(JYTMS20230227)。
文摘The progression of anodes has markedly promoted the advancement of lithium-ion batteries(LIBs).Typical LIBs using carbon anodes cannot meet the continuously increasing demands for qualified safety and longevity.Spinel lithium titanate(LTO)is a strong contender to replace graphite anodes due to its optimal zero-strain merit and outstanding structural stability.Nevertheless,low reversible capacity and poor rate performance hinder the widespread application of LTO.Amazingly,the promising pseudocapacitive effect enables LTO to surmount the limit of theoretical capacity via boosted surface Li storage,contributing to observably upgraded energy and power densities in a wide temperature range.By leveraging the synergistic effect of multiple modification strategies to create additional active sites,the pseudocapacitive response of LTO can be markedly enhanced.This paper reviews the progress of pseudocapacitive LTO for the first time.We highlight the zero-strain characteristic and pseudocapacitance mechanism of LTO and review the design strategies of pseudocapacitive LTO.Significative issues for further developing pseudocapacitive LTO are proposed.It is worth noting that the pseudocapacitive contribution can greatly improve the low-temperature electrochemical performances of LTO.We anticipate that more efforts will be aroused to study the advanced pseudocapacitive LTO to accelerate the development of next-generation LIBs and energy storage devices.
基金financially supported by the National Key Technology R&D Program of China(2017YFB0310704)the National Natural Science Foundation of China(21773112 and 21173119)the Fundamental Research Funds for the Central Universities
文摘Developing an efficient approach of transforming biomass waste to functional carbon-based electrode materials applied in supercapacitor offers an important and high value-added practical application due to the abundance and considerable low price of biomass wastes.Herein,a hierarchical carbon functionalized with electrochemical-active oxygen-containing groups was fabricated by microwave treatment from the biomass waste of camellia oleifera.The obtained mesoporous carbon(MAC)owns nanosheet morphology,rich mesoporosity,large surface area(1726 m2/g)and very high oxygenic functionalities(16.2 wt%)with pseudocapacitive activity.Prepared electrode of supercapacitor and tested in 2.0 M H2 SO4,the MAC exhibits an obvious pseudocapacitive activity and achieved a superior supercapacitive performance to that of directly activated carbon(DAC-800)including high specific capacitance(367 F/g vs.298 F/g)and better rate performance(66%vs.44%).The symmetrical supercapacitor based on MAC shows a high capacity of275 F/g,large energy density of 9.55 Wh/kg(at power density of 478 W/kg)and excellent cycling stability with 99%capacitance retention after 10000 continuous charge-discharge,endowing the obtained MAC a promising functional material for electrochemical energy storage.
基金supported by the National Natural Science Foundation of China (51974370)the Program of Huxiang Young Talents (2019RS2002)the Innovation and Entrepreneurship Project of Hunan Province, China (Grant No.2018GK5026)。
文摘Lithium ion capacitors(LICs)have been widely used as energy storage devices due to their high energy density and high power density.For LICs,pre-lithiation of negative electrode is necessary.In this work,we employ a bifunctional Li6CoO4(LCO)as cathodic pre-lithiation reagent to improve the electrochemical performance of LICs.The synthesized LCO exhibited high first charge specific capacity of 721 mAh g-1and extremely low initial coulombic efficiency of 3.19%,providing sufficient Li+ for the pre-lithiation of negative electrode in the first charge.Simultaneously,Li6–xCoOy is generated from LCO during the first charge process,which exhibits pseudocapacitive property and contributes to capacity in form of surface capacitance during subsequent cycles,increasing the capacity of capacitive positive electrode.With the appropriate amounts of addition to the positive side in LICs,this bifunctional prelithiation reagent LCO shows significantly improved the electrochemical performance with the energy density of 78.5 Wh kg-1after 300 cycles between 2.0 and 4.2 V at 250 mA g-1.
基金Project(2018JJ2513)supported by the Natural Science Foundation of Hunan Province,ChinaProject(18A378)supported by the Education Bureau Research Foundation of Hunan Province,ChinaProject(2019GK4012)supported by the Emerging Strategic Industrial Science and Technology Project of Hunan Province,China。
文摘To improve rate and cycling performance of manganese oxide anode material,a precipitation method was combined with thermal annealing to prepare the Mn O/Mn3O4/Se Ox(x=0,2)hybrid anode by controlling the reaction temperature of Mn2O3 and Se powders.At 3 A/g,the synthesized Mn O/Mn3O4/Se Ox anode delivers a discharge capacity of 1007 m A·h/g after 560 cycles.A cyclic voltammetry quantitative analysis reveals that 89.5%pseudocapacitive contribution is gained at a scanning rate of 2.0 m V/s,and the test results show that there is a significant synergistic effect between Mn O and Mn3O4 phases.
基金financially supported by National Natural Science Foundation of China(21805236)Scientific Research Fund of Hunan Provincial Education Department(18B062)+1 种基金Fundamental Research Fund of Xiangtan University(18QDZ14)Guangdong Basic and Applied Basic Research Foundation(2019A1515110819)。
文摘Sodium-organic batteries utilizing natural abundance of sodium element and renewable active materials gain great attentions for grid-scale applications.However,the development is still limited by lack of suitable organic cathode materials with high electronic conductivity that can be operated stably in liquid electrolyte.Herein,we present 5,15-bis(ethynyl)-10,20-diphenylporphyrin(DEPP)and[5,15-bis(ethynyl)-10,20-diphenylporphinato]copper(II)(CuDEPP)as new cathodes for extremely stable sodium-organic batteries.The copper(II)ion partially contributes the charge storage and significantly stabilizes the structure of porphyrin complex for electrochemical energy storage.In situ electrochemical stabilization of organic cathode with a lower charging current density was identified which enables both improved high energy density and power density.An excellent longterm cycling stability up to 600 cycles and an extremely high power density of 28 kW kg−1 were achieved for porphyrin-based cathode.This observation would open new pathway for developing highly stable sodium-organic cathode for electrochemical energy storage.
基金financially supported by the National Natural Science Foundation of China (Nos. 52072173 and U1802256)Jiangsu Specially-Appointed Professors Program+2 种基金Jiangsu Province Outstanding Youth Fund (No. BK20200016)the Leading-Edge Technology of Jiangsu Province (No. BK20202008)the Fundamental Research Funds for the Central Universities (No. NE2016005)
文摘Lithium-ion capacitors(LICs)have attracted wide attention due to their potential of achieving merits of high-power output as well as high energy density.How-ever,the key issue of kinetics mismatch between anode and cathode hinders the electrochemical performance of LICs.Therefore,a vanadium nitride composite with nanoparti-cles embedded in carbon matrix(VN-C)was prepared as an efficiently pseudocapacitive anode material with high electronic conductivity and fast Li-ion diffusion rate.The VN-C composites were synthesized through one-step ammonia heating treatment at different temperatures among which the sample annealed at 600℃exhibits high specific capacity(513 mAh·g^(-1)at 0.1 A·g^(-1)),outstanding rate performance(~300 mAh·g^(-1)at 10 A·g^(-1)),and excellent cyclic steadiness(negligible capacity decay over 2000 cycles)in half-cell devices.A high-performance lithium-ion capacitor device was also fabricated by using VN-C-600 as the anode and activated carbon as the cath-ode,delivering a maximum energy density of 112.6 Wh·kg^(-1)and an extreme power density of 10 kW·kg^(-1).
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.51672205,51872104 and 21673169)the National Key R&D Program of China(Grant No.2016YFA0202602)+1 种基金the Research Start-Up Fund from Wuhan University of Technologythe Fundamental Research Funds for the Central Universities(WUT:2016IVA083,2017IB005,185220011)
文摘Pseudocapacitive materials generally offer both high capacitance and high rate capability, which has stimulated great efforts in developing the materials system and related energy storage devices. In recent years, however, with the extensive use of nanomaterials in batteries, fast redox kinetics comparable to pseudocapacitive have been achieved in many kinds of battery materials due to the much shortened ion diffusion lengths and highly exposed surface/interface as a result of nanosize effect. Consequently, the terms"pseudocapacitive materials" and "battery materials" are becoming more and more confusing. In this review, different opinions on the definition of pseudocapacitive materials and the evolution of the definitions as well as the resulting confusion will be firstly reviewed. Then, to accurately distinguish pseudocapacitive and battery materials, method with the consideration of both the electrochemical signatures(CVs and GCD) and quantitative kinetics analysis as a supplement is proposed. Finally, we end this review by discussing the possible device configurations of asymmetric supercapacitors and hybrid supercapacitors. The present review will help understanding the differences between pseudocapacitive materials and battery materials, and thus avoiding the definition confusion.
基金financially supported by the National Natural Science Foundation of China (No. 22078279)
文摘An innovative K+vacant ternary perovskite fluoride(K_(0.89)Ni_(0.02)Co_(0.03)Mn_(0.95)F_(3.0),KNCMF-3#)anode was designed for advanced Li-ion supercapattery(i.e.,Li-ion capacitors/batteries,LIC/Bs).Owing to the conversion/insertion dual mechanisms and fast pseudocapacitive con-trol dynamics,the KNCMF-3#electrode exhibits superior electrochemical performance,especially the excellent cycle performance(467%(229 mAh·g^(-1))/1000 cycles/2 A·g^(-1)).Moreover,the hybrid KNCMF-3#/reduced gra-phene oxide(rGO)electrode can further increase the electrochemical performance(217-97 mAh·g^(-1)/0.1-3.2 A·g^(-1),150%(197 mAh·g^(-1))/1000 cycles/2 A·g^(-1)).Also,a novel capacitor/battery cathode,activated carbon(AC)+LiFePO_(4)+graphene(AC+LFP+G),exhibits impres-sive performance(128-82 mAh·g^(-1)/0.1-3.2 A·g^(-1),84%/1000 cycles/2 A·g^(-1)).By the synergistic optimization of anode and cathode,the Li-ion supercapattery KNCMF-3#@rGO//AC+LFP+G demonstrates remarkable per-formance,for example,111.9-23.8 Wh·kg^(-1)/0.4-8.0 kW·kg^(-1)/82%/2000 cycles/5 A·g^(-1)/0-4 V,which is superior to KNCMF-3#//AC LICs,KNCMF-3#@rGO//AC LICs,KNCMF-3#//AC+LFP+G LIC/Bs.In all,the novel Li-ion supercapattery idea adds a promising per-spective to develop advanced energy storage devices.
基金financially supported by the National Natural Science Foundation of China(Nos.51706016,51506014)the China Postdoctoral Science Foundation(No.2017T100677)
文摘We report a simple method for fabricating all-solid-state micro-supercapacitors, utilizing laser writing technology. Porous graphene films with three-dimensional networks induced by laser from commercial polymer was acted as scaffold for loading MnO2, a typical pseudocapacitive materials. Using gel electrolyte, all-solid-state pseudocapacitive micro-supercapacitors were fabricated. Compare to traditional printing and lithography techniques produced micro-supercapacitors, the as-fabricated devices demonstrate high volumetric capacitances, good stability and low leakage current, indicating a scalable and facile approach for future energy storage devices in portable microelectronics.
基金the Natural Science Basic Research Plan in Shaanxi Province of China(Program Nos.2019ZDLGY16-02,2019ZDLGY16-03,and 2019ZDLGY16-08)Youth Science and Technology Nova Program of Shaanxi Province(2020KJXX-068)the Wuhu and Xidian University special fund for industry-university-research cooperation(Program No.HX01201909039).
文摘Recent developments in the synthesis of graphene-based structures focus on continuous improvement of porous nanostructures,doping of thin films,and mechanisms for the construction of threedimensional architectures.Herein,we synthesize creeper-like Ni3Si2/NiOOH/graphene nanostructures via low-pressure all-solid meltingreconstruction chemical vapor deposition.In a carbon-rich atmosphere,high-energy atoms bombard the Ni and Si surface,and reduce the free energy in the thermodynamic equilibrium of solid Ni–Si particles,considerably catalyzing the growth of Ni–Si nanocrystals.By controlling the carbon source content,a Ni3Si2 single crystal with high crystallinity and good homogeneity is stably synthesized.Electrochemical measurements indicate that the nanostructures exhibit an ultrahigh specific capacity of 835.3 C g^−1(1193.28 F g^−1)at 1 A g^−1;when integrated as an all-solidstate supercapacitor,it provides a remarkable energy density as high as 25.9 Wh kg^−1 at 750 W kg^−1,which can be attributed to the freestanding Ni3Si2/graphene skeleton providing a large specific area and NiOOH inhibits insulation on the electrode surface in an alkaline solution,thereby accelerating the electron exchange rate.The growth of the high-performance composite nanostructure is simple and controllable,enabling the large-scale production and application of microenergy storage devices.
基金the financial support by the Australian Research Council through the ARC Discovery projects(DP160104340 and DP170100436)Rail Manufacturing Cooperative Research Centre(RMCRC 1.1.1 and RMCRC 1.1.2 projects)+1 种基金financially supported by the International Science&Technology Cooperation Program of China(No.2016YFE0102200)Shenzhen Technical Plan Project(No.JCYJ20160301154114273).
文摘Rechargeable aqueous zinc-ion hybrid capacitors and zincion batteries are promising safe energy storage systems.In this study,amorphous RuO2·H2O for the first time was employed to achieve fast and ultralong-life Zn2+storage based on a pseudocapacitive storage mechanism.In the RuO2·H2O||Zn zinc-ion hybrid capacitors with Zn(CF3SO3)2 aqueous electrolyte,the RuO2·H2O cathode can reversibly store Zn2+in a voltage window of 0.4-1.6 V(vs.Zn/Zn2+),delivering a high discharge capacity of 122 mAh g?1.In particular,the zinc-ion hybrid capacitors can be rapidly charged/discharged within 36 s with a very high power density of 16.74 kW kg?1 and a high energy density of 82 Wh kg?1.Besides,the zinc-ion hybrid capacitors demonstrate an ultralong cycle life(over 10,000 charge/discharge cycles).The kinetic analysis elucidates that the ultrafast Zn2+storage in the RuO2·H2O cathode originates from redox pseudocapacitive reactions.This work could greatly facilitate the development of high-power and safe electrochemical energy storage.
基金These authors would like to acknowledge the financial support of the project from the National Natural Science Foundation of China(No.61904141)the funding of Natural Science Foundation of Shaanxi Province(No.2020JQ-295)+4 种基金China Postdoctoral Science Foundation(2020M673340)the Fundamental Research Funds for the Central Universities(JB210407)the Key Research and Development Program of Shaanxi(Program No.2020GY-252No.2021GY-277)National Key Laboratory of Science and Technology on Vacuum Technology and Physics(HTKJ2019KL510007).
文摘Flexible pressure sensors are unprecedentedly studied on monitoring human physical activities and robotics.Simultaneously,improving the response sensitivity and sensing range of flexible pressure sensors is a great challenge,which hinders the devices’practical application.Targeting this obstacle,we developed a Ti_(3)C_(2)T_(x)-derived iontronic pressure sensor(TIPS)by taking the advantages of the high intercalation pseudocapacitance under high pressure and rationally designed structural configuration.TIPS achieved an ultrahigh sen-sitivity(S_(min)>200 kPa^(−1),S_(max)>45,000 kPa^(−1))in a broad sensing range of over 1.4 MPa and low limit of detection of 20 Pa as well as stable long-term working durability for 10,000 cycles.The practical application of TIPS in physical activity monitoring and flexible robot manifested its versatile potential.This study provides a demonstration for exploring pseudocapacitive materials for building flexible iontronic sensors with ultrahigh sensitivity and sensing range to advance the development of high-performance wearable electronics.
基金support of the Office of Naval Research(ONR grant numbers N000141712244 and N000141912113)support from the National Key R&D Program of China(Grant Number:2016YFA0202602)+1 种基金Natural Science Foundation of Fujian Province of China“Double-First Class”Foundation of Materials and Intel igent Manufacturing Discipline of Xiamen University
文摘Sodium-ion battery materials and devices are promising candidates for largescale applications,owing to the abundance and low cost of sodium sources.Emerging sodium-ion pseudocapacitive materials provide one approach for achieving high capacity at high rates,but are currently not well understood.Herein,a comprehensive overview of the fundamentals and electrochemical behaviors of vanadium-based pseudocapacitive materials for sodium-ion storage is presented.The insight of sodium-ion storage mechanisms for various vanadium-based materials,including vanadium oxides,vanadates,vanadium sulfides,nitrides,and carbides are systematically discussed and summarized.In particular,areas for further development to improve fundamental understanding of electrochemical and structural properties of materials are identified.Finally,we provide a perspective on the application of pseudocapacitive materials in high-power and high-energy sodium-ion storage devices(e.g.,sodium-ion capacitors).
基金supported by the Beijing Natural Science Founding (2202050)the Beijing Institute of Technology scientific cooperation project (BITBLR2020010)+1 种基金the National Nature Science Foundation of China (21111120074)the National Nature Science Foundation of China (20806008)。
文摘The development of potential transition-metal carbide/nitride heterojunctions is hindered by overall understanding and precise modulation for heterointerface effects.Herein,we demonstrate that Mo_(2)C/Mo_(2)N heterojunction with the precisely regulated high-quality interface can achieve marvelous rate performance and energy output via enlarging the interface-effect range and maximizing "accelerated charge" amount The heterointerface mechanism improving properties is synergistically revealed from kinetics and thermodynamics perspectives.Kinetics analysis confirms that the self-built electric field affords a robust force to drive rapid interface electrons/ions migration.The small adsorption energy,high density of states and quite low diffusion barrier thermodynamically enhance the electrochemical reaction dynamics on heterointerface.Consequently,the almost optimal performance of ultrahigh capacitance retention(85.6% even at 10 A g^(-1)) and pronounced energy output(96.4 Wh kg^(-1))in hybridsupercapacitors than other Mo_(2)C/Mo_(2)N-based materials is presented.This work gives new insight into the energy storage mechanism of heterojunction and guides the design of advanced electrodes.
基金financially supported by the National Natural Science Foundation of China(Nos.22075109,22279056)the Jiangsu Provincial Department of Science and Technology(No.BK20220010).
文摘Carbon is a promising capacitive electrode material for Zn-ion hybrid supercapacitors(ZHSCs),as it is low-cost,environmentally friendly,controllable and adjustable.By now,achieving both high energy and high power with carbon electrodes is still challenging,limited by their intrinsic properties.In this work,we have designed and presented an amorphous hollow carbon bowl material with surface chemical modifications of oxygen groups to figure out these concerns.The preparation of bowl-like structures and the storage behavior between Zn^(2+)and oxygen functional groups have also been discussed.With the contributions from its unique hollow structure and surface functional groups,it can significantly enhance the electrode pseudocapacitance and the entire electrochemical performance.
基金supported by the National Key R&D Program of China(Grant No.2017YFA0207202)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_1058)。
文摘As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broader distribution of sodium[1–7].Sodium has similar electrochemical properties to lithium,and thus the concepts for the preparation of electrode materials for SIBs can be borrowed from LIBs[8,9].
基金the support of Project Supported by Keypoint Research and Invention in Shaanxi Province of China(No.2020GY-270)Service local special plan project of Education Department of Shaanxi Province(No.19JC009)。
文摘Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical reaction mechanism of Zn_(2)Ti_(3)O_(8)has rarely been studied.In this work,a porous Zn_(2)Ti_(3)O_(8)anode with considerably high capacity(421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles)was reported,which is even higher than ever reported titanium-based anodes materials including Li_(4)Ti_(5)O_(12),TiO_(2)and Li_(2)ZnTi_(3)O_(8).Here,for the first time,the accurate theoretical capacity of Zn_(2)Ti_(3)O_(8)was confirmed to be 266.4 mAh/g.It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn_(2)Ti_(3)O_(8),making it possibly higher than the theoretical value.Most importantly,the porous structure of Zn_(2)Ti_(3)O_(8)not only promotes the intercalation reaction,but also induces high pseudocapacitance capacity(225.4 mAh/g),which boosts the reversible capacity.Therefore,it is the outstanding pseudocapacitance capacity of porous Zn_(2)Ti_(3)O_(8)that accounts for high actual capacity exceeding the theoretical one.This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.
基金the funding support from the National Natural Science Foundation of China(grant nos.92372122 and 52471242)the Fundamental Research Funds for the Central Universities(grant nos.KY2060000269,WK2060000040,KY2060000150,and GG2060127001)+3 种基金the Joint Laboratory for University of Science and Technology of China(USTC),Yanchang Petroleum(grant no.2022ZKD-03)the Shandong Province Natural Science Foundation(grant no.ZR2024ZD01)support from the China Postdoctoral Science Foundation(grant no.2023M730562)the Jiangsu Funding Program for Excellent Postdoctoral Talent(grant no.2023ZB187).
文摘The emerging Li//H_(2)battery is a promising candidate for energy storage systems to meet the demand for the worldwide transition to clean and sustainable energy.To leverage the H_(2)electrode’s advantages and decrease costs,a high areal capacity anode-free Li anode is ideal.Here we propose using a pseudocapacitive Cu(PC-Cu)substrate to accommodate the high areal capacity anode-free Li//H_(2)battery(AFLHB).The PC-Cu substrate exhibits intense electrochemical adsorption and intrinsic strong chemisorption to Li,which leads to aggregation of the Li salts so as to induce enrichment of interfacial lithiophilicity.This aids uniform Li nucleation,anion concentration,and robust SEI formation.The AFLHB displays stable cycling at a high areal capacity of 5 mAh cm^(-2)with an average coulombic efficiency of 98.80%for over 350 h.Notably,the PC-Cu substrate enables superdense Li deposition with only 7%thickness exceeding the theoretical value.Moreover,the modified substrate enables a reversible Li stripping/plating at an ultralarge areal capacity of 20 mAh cm^(-2).This work presents an interfacial lithiophilicity enrichment strategy to stabilize the cycling performance of high areal capacity AFLHB and advances this novel battery system one step closer to practical application.
基金supported partially by project of the National Natural Science Foundation of China(Nos.62474064 and 52102203)the Fundamental Research Funds for the Central Universities(No.2024MS082)the NCEPU“Double First-Class”Program.
文摘Silicon(Si)has emerged as a promising anode material for lithium-ion batteries(LIBs)due to its extremely high theoretical capacity of 4200 mAh·g^(-1).However,its practical application is limited by several critical challenges,including severe volume expansion and poor electrical conductivity.Herein,we employ a two-dimensional(2D)oxygen modification engineering approach to fabricate 2D oxygen-functionalized CaSi_(2)(CaSi_(2)O_(x))layers.During the preparation of 2D CaSi_(2) layers,O atoms are gradually incorporated onto their surface.The resulting 2D CaSi_(2)O_(x) layers have a thickness of 3-5 nm,closely matching the theoretical thickness of 6-10 layers.When used as lithium anodes,the 2D CaSi_(2)O_(x) layers exhibit exceptional electrochemical performance,maintaining stability over 3000 cycles at an ultrahigh current density of 30 A·g^(-1).By tailoring the surface properties,their pseudocapacitive charge storage mechanism is significantly enhanced,effectively overcoming the intrinsic limitations of traditional Si anodes.This study highlights the promise of 2D surface engineering in the development of advanced materials for next-generation LIBs.