Sulfide-Based Nickel-Plated Fabrics for Foldable Quasi-Solid-State Supercapacitors

Smart wearable market is burgeoning,and flexible energy storage is crucial to cope with its development.The commonly-used metal-based current collectors are heavy with limited flexibility.Other carbon-based current collectors are expensive and fragile.Moreover,the poor interface between active material and current collector leads to unsatisfactory stability.Herein,these two issues are attempted to be solved by using cheap and lightweight polyester-based fabrics as well as in-situ growth.A deposited thin layer of nickel on the fabrics not only enhances the conductivity,but also serves as the sacrificial precursor for the growth of active materials.Thus,intimate contact is secured via chemical bonding.The electrode with ternary(metalinorganic-organic)component shows excellent electrochemical performance.Namely,high areal capacity is realized(2.2 C cm^(-2)at 2 mA cm^(-2)),which is far superior to its rigid nickel-foam-based counterpart.Furthermore,an allsolid-state supercapacitor device was assembled.The device provides an areal capacity of 2.03 C cm^(-2)at the current density of 2 mA cm^(-2).It realizes an energy density of 0.45 mWh cm^(-2)when the power density is 1.6 mW cm^(-2).This work offers a feasible and cost-efficient way for fabricating electrode materials with excellent performance for portable supercapacitors.

Surface-engineered binder-free PEDOT shielded nickel magnesium selenide nanosheet arrays electrode for ultralong-life flexible quasi-solid-state hybrid supercapacitors

Together with the development of high-performance advanced electronics,flexible supercapacitors(SCs)with tailored nanostructures have great attraction.Electrochemically deposited nanosheet arrays of nickel magnesium selenide(NixMg3-xSe4,NMgS)with high capacitance provide high potentials as a positive electrode in flexible SCs.To further enhance their electrochemical properties and long-term cycling stability,a promising strategy of surface engineering with conducting polymer poly(3,4-ethylenedioxythiophene)(PEDOT)is proposed.The present work proposes the construction of PEDOT shielded NMgS(P@NMgS-2)on a flexible carbon cloth substrate via a hierarchical electrodeposition technique.Benefitting from the synergistic effect,the P@NMgS-2 exhibits an excellent areal capacitance value of 1440 mF cm^(-2)at 4 mA cm^(-2).A novel shape-adaptable polymer gel electrolyte-assisted flexible quasi-solid-state hybrid SC(FQHSC)device constructed with P@NMgS-2 as a positive electrode and activated carbon as a negative electrode demonstrates the maximum power and energy density values of 14.13 mW cm^(-2)and 0.18 mWh cm^(-2),respectively,followed by outstanding cycling stability(∼100%capacitance retention over 50,000 cycles).Furthermore,the FQHSC device successfully powered electronic devices with no serious degradation upon bending and twisting for wearable electronic applications.

Gradient‑Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable supercapacitors.By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella.Moreover,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of lignin.All these strategies effectively enhanced the capacitive performance of the electrodes.In addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes.Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),respectively.Moreover,their capacitances were well preserved after 1000 times of 600%stretch-release cycling.This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.

Recent advances on quasi-solid-state electrolytes for supercapacitors

Solid-state and quasi-solid-state electrolytes have been attracting the scientific community’s attention in the last decade. These electrolytes provide significant advantages, such as the absence of leakage and separators for devices and safety for users. They also allow the assembly of stretchable and bendable supercapacitors. Comparing solid-state to quasi-solid-states, the last provides the most significant energy and power densities due to the better ionic conductivity. Our goal here is to present recent advances on quasisolid-state electrolytes, including gel-polymer electrolytes. We reviewed the most recent literature on quasi-solid-state electrolytes with different solvents for supercapacitors. Organic quasi-solid-state electrolytes need greater attention once they reach an excellent working voltage window greater than 2.5 V.Meanwhile, aqueous-based solid-state electrolytes have a restricted voltage window to less than 2 V. On the other hand, they are easier to handle, provide greater ionic conductivity and capacitance. Recent water-in-salt polymer-electrolytes have shown stability as great as 2 V encouraging further development in aqueous-based quasi-solid-state electrolytes. Moreover, hydrophilic conductive polymers have great commercial appeal for bendable devices. Thus, these electrolytes can be employed in flexible and bendable devices, favoring the improvement of portable electronics and wearable devices(376 references were evaluated and summarized here).

Ti_(3)C_(2)T_(x) MXene/carbon composites for advanced supercapacitors:Synthesis,progress,and perspectives

MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivity,good hydrophilicity,and tunable terminations.Among various types of MXenes,Ti_(3)C_(2)T_(x) is the most widely studied for use in capacitive energy storage applications,especially in supercapacitors(SCs).However,the stacking and oxidation of MXene sheets inevitably lead to a significant loss of electrochemically active sites.To overcome such challenges,carbon materials are frequently incorporated into MXenes to enhance their electrochemical properties.This review introduces the common strategies used for synthesizing Ti_(3)C_(2)T_(x),followed by a comprehensive overview of recent developments in Ti_(3)C_(2)T_(x)/carbon composites as electrode materials for SCs.Ti_(3)C_(2)T_(x)/carbon composites are categorized based on the dimensions of carbons,including 0D carbon dots,1D carbon nanotubes and fibers,2D graphene,and 3D carbon materials(activated carbon,polymer-derived carbon,etc.).Finally,this review also provides a perspective on developing novel MXenes/carbon composites as electrodes for application in SCs.

All-cellulose-based quasi-solid-state supercapacitor with nitrogen and boron dual-doped carbon electrodes exhibiting high energy density and excellent cyclic stability

The key to construct high-energy supercapacitors is to maximize the capacitance of electrode and the voltage of the device. Realizing this purpose by utilizing sustainable and low-cost resources is still a big challenge. Herein, N, B co-doped carbon nanosheets are obtained through the proposed dual-template assisted approach by using methyl cellulose as the precursor. Due to the synergistic effects form the high surface area with the hierarchical porous structure, N/B dual doping, and a high degree of graphitization, the resultant carbon electrode exhibits a high capacitance of 572 F g^(-1)at 0.5 A g^(-1)and retains 281 F g^(-1)at 50 A g^(-1)in an acidic electrolyte. Furthermore, the symmetric device assembled using bacterial cellulose-based gel polymer electrolyte can deliver high energy density of 43 W h kg^(-1)and excellent cyclability with 97.8% capacity retention after 20 000 cycles in “water in salt” electrolyte. This work successfully realizes the fabrication of high-performance allcellulose-based quasi-solid-state supercapacitors, which brings a cost-effective insight into jointly designing electrodes and electrolytes for supporting highly efficient energy storage.

Cotton pads-derived carbon materials/reduced graphene oxide modified with polypyrrole for electrode of supercapacitors

This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.

Recent Research Progress of Paper-Based Supercapacitors Based on Cellulose

In recent years,paper-based functional materials have received extensive attention in the field of energy storage due to their advantages of rich and adjustable porous network structure and good flexibility.As an important energy storage device,paper-based supercapacitors have important application prospects in many fields and have also received extensive attention from researchers in recent years.At present,researchers have modified and regulated paper-based materials by different means such as structural design and material composition to enhance their electrochemical storage capacity.The development of paper-based supercapacitors provides an important direction for the development of green and sustainable energy.Therefore,it is of great significance to summarize the relevant work of paper-based supercapacitors for their rapid development and application.In this review,the recent research progress of paper-based supercapacitors based on cellulose was summarized in terms of various cellulose-based composites,preparation skills,and electrochemical performance.Finally,some opinions on the problems in the development of this field and the future development trend were proposed.It is hoped that this review can provide valuable references and ideas for the rapid development of paper-based energy storage devices.

Self-Powered Piezo-Supercapacitors Based on ZnO@Mo-Fe-MnO_(2)Nanoarrays

The development of self-charging supercapacitor power cells(SCSPCs)has profound implications for smart electronic devices used in different fields.Here,we epitaxially electrodeposited Mo-and Fe-codoped MnO_(2)films on piezoelectric ZnO nanoarrays(NAs)grown on the flexible carbon cloth(denoted ZnO@Mo-Fe-MnO_(2)NAs).A self-charging supercapacitor power cell device was assembled with the Mo-and Fe-codoped MnO_(2)nanoarray electrode and poly(vinylidenefluoride-co-trifluoroethylene)(PVDF-Trfe)piezoelectric film doped with BaTiO_(3)(BTO)and carbon nanotubes(CNTs)(denoted PVDF-Trfe/CNTs/BTO).The self-charging supercapacitor power cell device exhibited an energy density of 30μWh cm^(-2)with a high power density of 40 mW cm^(-2)and delivered an excellent self-charging performance of 363 mV(10 N)driven by both the piezoelectric ZnO nanoarrays and the poly(vinylidenefluoride-co-trifluoroethylene)piezoelectric film doped with BaTiO_(3)and carbon nanotubes.More intriguingly,the device could also be self-charged by 184 mV due to residual stress alone and showed excellent energy conversion efficiency and low self-discharge rate.This work illustrates for the first time the self-charging mechanism involving electrolyte ion migration driven by both electrodes and films.A comprehensive analysis strongly confirmed the important contribution of the piezoelectric ZnO nanoarrays in the self-charging process of the self-charging supercapacitor power cell device.This work provides novel directions and insights for the development of selfcharging supercapacitor power cells.

Ag-integrated mixed metallic Co-Fe-Ni-Mn hydroxide composite as advanced electrode for high-performance hybrid supercapacitors

Direct growth of redox-active noble metals and rational design of multifunctional electrochemical active materials play crucial roles in developing novel electrode materials for energy storage devices.In this regard,silver(Ag)has attracted great attention in the design of efficient electrodes.Inspired by the house/building process,which means electing the right land,it lays a strong foundation and building essential columns for a complex structure.Herein,we report the construction of multifaceted heterostructure cobalt-iron hydroxide(CFOH)nanowires(NWs)@nickel cobalt manganese hydroxides and/or hydrate(NCMOH)nanosheets(NSs)on the Ag-deposited nickel foam and carbon cloth(i.e.,Ag/NF and Ag/CC)substrates.Moreover,the formation and charge storage mechanism of Ag are described,and these contribute to good conductive and redox chemistry features.The switching architectural integrity of metal and redox materials on metallic frames may significantly boost charge storage and rate performance with noticeable drop in resistance.The as-fabricated Ag@CFOH@NCMOH/NF electrode delivered superior areal capacity value of 2081.9μA h cm^(-2)at 5 mA cm^(-2).Moreover,as-assembled hybrid cell based on NF(HC/NF)device exhibited remarkable areal capacity value of 1.82 mA h cm^(-2)at 5 mA cm^(-2)with excellent rate capability of 74.77%even at 70 mA cm^(-2)Furthermore,HC/NF device achieved maximum energy and power densities of 1.39 mW h cm^(-2)and 42.35 mW cm^(-2),respectively.To verify practical applicability,both devices were also tested to serve as a self-charging station for various portable electronic devices.

Mechanical reliable,NIR light-induced rapid self-healing hydrogel electrolyte towards flexible zinc-ion hybrid supercapacitors with low-temperature adaptability and long service life

Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.

Recent advances in transition metal phosphide materials:Synthesis and applications in supercapacitors

Supercapacitors(SCs)are considered promising energy storge systems because of their outstanding power density,fast charge and discharge rate and long-term cycling stability.The exploitation of cheap and efficient electrode materials is the key to improve the performance of supercapacitors.As the battery-type materials,transition metal phosphides(TMPs)possess high theoretical specific capacity,good electrical conductivity and superior structural stability,which have been extensively studied to be electrode materials for supercapacitors.In this review,we summarize the up-to-date progress on TMPs materials from diversified synthetic methods,diverse nanostructures and several prominent TMPs and their composites in application of supercapacitors.In the end,we also propose the remaining challenges toward the rational discovery and synthesis of high-performance TMP electrodes materials for energy storage.

Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors

Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.

Flexible quasi-solid-state dual-ion asymmetric supercapacitor based on Ni（OH）2 and Nb2O5 nanosheet arrays

Increasing the energy density, power density as well as widening the operation voltage are essential to electrochemical capacitors to meet the practical energy demands. Herein, a novel flexible quasi-solid-state dual-ion asymmetric supercapacitor(ASC) with Ni(OH)2 and Nb2O5 nanosheets directly grown on stainless steel mesh is developed. In the dual-ion ASC, Nb2O5 negative and Ni(OH)2 positive electrodes react with Li+ and OH- respectively in alkaline gel electrolyte to store energy, which is quite different from conventional alkali metal ion SCs and alkaline SCs. The as-assembled flexible device has an extended working voltage of 1.7 V and delivers a capacity of 5.37 mAh cm-2, a maximum energy density and power density of 0.52 mWh cm-3 and 170 mW cm-3 , respectively. The device maintains around 60% capacity retention after long cycling up to 1000 cycles. Moreover, our device can light up a LED light efficiently upon fast charging. The proposed quasi-solid-state dual-ion ASC has potential applications in future portable electronics and flexible energy storage devices.

High Areal Capacity and Long Cycle Life Flexible Mild Quasi-Solid-State Ag-Zn Battery with Dendrite-Free Anode

Silver-zinc(Ag-Zn)batteries are a promising battery system for flexible electronics owing to their high safety,high energy density,and stable output voltage.However,poor cycling performance,low areal capacity,and inferior flexibility limit the practical application of Ag-Zn batteries.Herein,we develop a flexible quasi-solid-state Ag-Zn battery system with superior performance by using mild electrolyte and binder-free electrodes.Copper foam current collector is introduced to impede the growth of Zn dendrite,and the structure of Ag cathode is engineered by electrodeposition and chloridization process to improve the areal capacity.This novel battery demonstrates a remarkable cycle retention of 90%for 200 cycles at 3 mA cm^(-2).More importantly,this binder-free battery can afford a high capacity of 3.5 mAh cm^(-2)at 3 mA cm^(-2),an outstanding power density of 2.42 mW cm^(-2),and a maximum energy density of 3.4 mWh cm^(-2).An energy management circuit is adopted to boost the output voltage of a single battery,which can power electronic ink display and Bluetooth temperature and humidity sensor.The developed battery can even operate under the extreme conditions,such as being bent and sealed in solid ice.This work offers a path for designing electrodes and electrolyte toward high-performance flexible Ag-Zn batteries.

One-Step Scalable Fabrication of Nitrogen and Chlorine Co-doped Graphene by Electrochemical Exfoliation for High-Performance Supercapacitors

The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation technique to fabricate nitrogen(N)and chlorine(Cl)co-doped graphene nanosheets(i.e.,N-Cl-G)via the application of constant voltage on graphite in a mixture of 0.1 mol/L H_(2)SO_(4)and 0.1 mol/L NH_(4)Cl without using dangerous and exhaustive operation.The introduction of Cl(with its large radius)and N,both with high electrical negativity,facilitates the modulation of the electronic structure of graphene and creation of rich structural defects in it.Consequently,in the as-constructed supercapacitors,N-Cl-G exhibits a high specific capacitance of 77 F/g at 0.2 A/g and remarkable cycling stability with 91.7%retention of initial capacitance after 20,000 cycles at 10 A/g.Furthermore,a symmetrical supercapacitor assembled with N-Cl-G as the positive and negative electrodes(denoted as N-Cl-G//N-Cl-G)exhibits an energy density of 3.38 Wh/kg at a power density of 600 W/kg and superior cycling stability with almost no capacitance loss after 5000 cycles at 5 A/g.This study provides a scalable protocol for the facile fabrication of high-performance co-doped graphene as an electrode material candidate for supercapacitors.

Dual-salt poly(tetrahydrofuran) electrolyte enables quasi-solid-state lithium metal batteries to operate at -30 ℃

The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migration.Herein,we prepare a dual-salt poly(tetrahydrofuran)-based electrolyte consisting of lithium hexafluorophosphate and lithium difluoro(oxalato)borate(LiDFOB).The Li-salt anions(DFOB−)not only accelerate the ring-opening polymerization of tetrahydrofuran,but also promote the formation of highly ion-conductive and sustainable interphases on Li metal anodes without sacrificing the Li^(+)conductivity of electrolytes,which is favorable for Li^(+)transport kinetics at low temperatures.Applications of this polymer electrolyte in Li||LiFePO_(4)cells show 82.3%capacity retention over 1000 cycles at 30℃and endow stable discharge capacity at−30℃.Remarkably,the Li||LiFePO4 cells retain 52%of their room-temperature capacity at−20℃and 0.1 C.This rational design of dual-salt polymer-based electrolytes may provide a new perspective for the stable operation of quasi-solid-state batteries at low temperatures.

In-depth analysis of VARTM-based solid-state supercapacitors utilizing CNT-dispersed cobalt-bismuth-samarium ternary hydroxide on woven carbon fiber for enhanced energy storage

Multi-metal hydroxides possess unique physical and chemical properties,making them promising candidates for supercapacitor working electrodes.Enhancing their electrochemical performance can be achieved through a combination with carbon materials.In this study,we synthesized a composite material by hydrothermally dispersed 4,6,and 10 wt%carbon nanotubes(CNT)into ternary cobaltbismuth-samarium hydroxide(CoBiSm-TOH).These nanocomposites were employed as the material for the working electrode in a supercapacitor.The findings reveal that at 1.5 A/g,the specific capacitance of CNT3@CoBiSm-TOH,using a three-electrode system,was found to be 852.91 F/g,higher than that of CoBi-BOH,CoBiSm-TOH,CNT1@CoBiSm-TOH and CNT5@CoBiSm-TOH-measuring 699.69,750.34,789.54 and 817.79 F/g,respectively.Moreover,CNT3@CoBiSm-TOH electrodes exhibited a capacitance retention of around 88%over 10,000 cycles.To demonstrate practical applicability,CNT3@CoBiSm-TOH was grown on woven carbon fiber(WCF),and a solid-state supercapacitor device was developed using the VARTM(vacuum-assisted resin transfer molding).This device displayed a specific capacitance of 272.67 F/g at 2.25 A/g.Notably,it achieved a maximum energy density of 53.01 Wh/kg at a power density of 750 W/kg and sustained excellent cycle stability over 50,000 cycles,maintaining 70%of its initial capacitance.These results underscore the importance of interfacial nanoengineering and provide crucial insights for the development of future energy storage devices.

Phase reconfiguration of heterogeneous CoFeS/CoNiS nanoparticles for superior battery-type supercapacitors

Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.

Enhancing MXene-based supercapacitors:Role of synthesis and 3D architectures

MXene has been the limelight for studies on electrode active materials,aiming at developing supercapacitors with boosted energy density to meet the emerging influx of wearable and portable electronic devices.Despite its various desirable properties including intrinsic flexibility,high specific surface area,excellent metallic conductivity and unique abundance of surface functionalities,its full potential for electrochemical performance is hindered by the notorious restacking phenomenon of MXene nanosheets.Ascribed to its two-dimensional(2D)nature and surface functional groups,inevitable Van der Waals interactions drive the agglomeration of nanosheets,ultimately reducing the exposure of electrochemically active sites to the electrolyte,as well as severely lengthening electrolyte ion transport pathways.As a result,energy and power density deteriorate,limiting the application versatility of MXene-based supercapacitors.Constructing 3D architectures using 2D nanosheets presents as a straightforward yet ingenious approach to mitigate the fatal flaws of MXene.However,the sheer number of distinct methodologies reported,thus far,calls for a systematic review that unravels the rationale behind such 3D MXene structural designs.Herein,this review aims to serve this purpose while also scrutinizing the structure–property relationship to correlate such structural modifications to their ensuing electrochemical performance enhancements.Besides,the physicochemical properties of MXene play fundamental roles in determining the effective charge storage capabilities of 3D MXene-based electrodes.This largely depends on different MXene synthesis techniques and synthesis condition variations,hence,elucidated in this review as well.Lastly,the challenges and perspectives for achieving viable commercialization of MXene-based supercapacitor electrodes are highlighted.