Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless...Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative electrode.Herein, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate capability.Benefiting from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.展开更多
The popularization of portable,implantable and wearable microelectronics has greatly stimulated the rapid development of high-power planar micro-supercapacitors(PMSCs).Particularly,the introduction of new functionalit...The popularization of portable,implantable and wearable microelectronics has greatly stimulated the rapid development of high-power planar micro-supercapacitors(PMSCs).Particularly,the introduction of new functionalities(e.g.,high voltage,flexibility,stretchability,self-healing,electrochromism and photo/thermal response)to PMSCs is essential for building multifunctional PMSCs and their smart selfpowered integrated microsystems.In this review,we summarized the latest advances in PMSCs from various functional microdevices to their smart integrated microsystems.Primarily,the functionalities of PMSCs are characterized by three major factors to emphasize their electrochemical behavior and unique scope of application.These include but are not limited to high-voltage outputs(realized through asymmetric configuration,novel electrolyte and modular integration),mechanical resilience that includes various feats of flexibility or stretchability,and response to stimuli(self-healing,electrochromic,photo-responsive,or thermal-responsive properties).Furthermore,three representative integrated microsystems including energy harvester-PMSC,PMSC-energy consumption,and all-in-one selfpowered microsystems are elaborately overviewed to understand the emerging intelligent interaction models.Finally,the key perspectives,challenges and opportunities of PMSCs for powering smart microelectronics are proposed in brief.展开更多
By means of inkjet printing technique, flexible and all-solid-state micro-supercapacitors(MSCs) were fabricated with carbon-based hybrid ink composed of graphene oxide(GO,98.0vol.%) ink and commercial pen ink(2.0vol.%...By means of inkjet printing technique, flexible and all-solid-state micro-supercapacitors(MSCs) were fabricated with carbon-based hybrid ink composed of graphene oxide(GO,98.0vol.%) ink and commercial pen ink(2.0vol.%). A small amount of commercial pen ink was added to effectively reduce the agglomeration of theGO sheets during solvent evaporation and the following reduction processes in which the presence of graphite carbon nanoparticles served as nano-spacer to separate GO sheets. The printed device fabricated using the hybrid ink,combined with the binder-free microelectrodes and interdigital microelectrode configuration, exhibits nearly 780%enhancement in areal capacitance compared with that of pure GO ink. It also shows excellent flexibility and cycling stability with nearly 100% retention of the areal capacitance after 10,000 cycles. The all-solid-state device can be optionally connected in series or in parallel to meet the voltage and capacity requirements for a given application.This work demonstrates a promising future of the carbonbased hybrid ink for directly large-scale inkjet printing MSCs for disposable energy storage devices.展开更多
Rational design and precise regulation over the morphology, structure, and pore size of functional conducting mesoporous polymers with enriched active sites and shorten electron–ion transport pathway are extremely im...Rational design and precise regulation over the morphology, structure, and pore size of functional conducting mesoporous polymers with enriched active sites and shorten electron–ion transport pathway are extremely important for developing high-performance micro-supercapacitors (MSCs), but still remain a great challenge. Herein, a general dual-colloid interface co-assembly strategy is proposed to fabricate hollow mesoporous polypyrrole nano-bowls (mPPy-nbs) for high-energy-density solid-state planar MSCs. By simply adjusting the size of block copolymer micelles, the diameter of polystyrene nanospheres and the amount of pyrrole monomer, mesopore size of the shell, void and shell thickness of mPPy-nbs can be simultaneously controlled. Importantly, this strategy can be further utilized to synthesize other hollow mesoporous polymers, including poly(tris(4-aminophenyl)amine), poly(1,3,5-triaminobenzene) and their copolymers, demonstrative of excellent universality. The structurally optimized mPPy-nb exhibits high specific surface area of 122 m^(2) g^(−1)and large capacitance of 225 F g^(−1) at 1 mV s^(−1). Furthermore, the MSCs assembled by mPPy-nbs deliver impressive volumetric capacitance of 90 F cm^(−3) and energy density of 2.0 mWh cm^(−3), superior to the most reported polymers-based MSCs. Also, the fabricated MSCs present excellent flexibility with almost no capacitance decay under varying bending states, and robust serial/parallel self-integration for boosting voltage and capacitance output. Therefore, this work will inspire the new design of mesoporous conducting polymer materials toward high-performance microscale supercapacitive devices.展开更多
Microscale electrochemical energy storage devices,e.g., micro-supercapacitors(MSCs),possessing tailored performance and diversified form factors of lightweight,miniaturization,flexibility and exceptional integration a...Microscale electrochemical energy storage devices,e.g., micro-supercapacitors(MSCs),possessing tailored performance and diversified form factors of lightweight,miniaturization,flexibility and exceptional integration are highly necessary for the smart power sources-unitized electronics.Despite the great progress,the fabrication of MSCs combining high integration with high volumetric performance remains largely unsolved.Herein,we develop a simple,fast and scalable strategy to fabricate graphene based highly integrated MSCs by a new effective continuous centrifugal coating technique.Notably,the resulting highly conductive graphene films can act as not only patterned microelectrodes but also metal-free current collectors and interconnects,endowing modular MSCs with high integrity,remarkable flexibility,tailored voltage and capacitance output,and outstanding performance uniformity.More importantly,the strong centrifugal force and shear force generated in continuous centrifugal coating process lead to graphene films with high alignment,compactness and packing density,contributing to excellent volumetric capacitance of ~31.8 F cm^(-3) and volumetric energy density of ~2.8 mWh cm^(-3),exceeding most reported integrated MSCs.Therefore,our work paves a novel way for simple and scalable fabrication of integrated MSCs and offers promising opportunities as standalone microscale power sources for new-generation electronics.展开更多
Harnessing energy from the environment promotes the rapid development of micro-power generators and relevant power management modules of alternating current (AC) line-filtering to obtain a stabilized direct current (D...Harnessing energy from the environment promotes the rapid development of micro-power generators and relevant power management modules of alternating current (AC) line-filtering to obtain a stabilized direct current (DC) output for storage and use. Micro-supercapacitors (MSCs) with miniaturized volume and high-frequency response are regarded as a critical component in filtering circuits for microscale power conversion. Here, we reported the fabrication of the wafer-sized planar MSCs (M-MSCs) based on 2D Ti_(2)C_(2)T_(6) MXene using a photolithography technique. The M-MSCs exhibited an areal capacitance of 153 μF cm^(-2) and a frequency characteristic (f_(0)) of 5.6 k Hz in aqueous electrolyte. Moreover, by employing suitable ionic liquid as electrolyte, the voltage window was expanded to 2 V and the f_(0) could be pushed to 6.6 k Hz relying on the electrical double-layer mechanism and lower adsorption energy while maintaining quasi-rectangular cyclic voltammogram curves at 5000 V s^(-1). Furthermore, the integrated MSCs pack was constructed and exhibited excellent rectifying ability by filtering various highfrequency 5000 Hz AC signals with different waveforms into stable DC outputs. Such ultrahigh-rate and high-voltage M-MSCs module for k Hz AC line-filtering would be potentially integrated with customizable electronics to realize on-chip rectifiers in high-density integrated circuit.展开更多
With the rapid development of integrated and miniaturized electronics,the planar energy storage devices with high capacitance and energy density are in enormous demand.Hence,the advanced manufacture and fast fabricati...With the rapid development of integrated and miniaturized electronics,the planar energy storage devices with high capacitance and energy density are in enormous demand.Hence,the advanced manufacture and fast fabrication of microscale planar energy units are of great significance.Herein,we develop aqueous planar micro-supercapacitors(MSCs) with ultrahigh areal capacitance and energy density via an efficient all-3 D-printing strategy,which can directly extrude the active material ink and gel electrolyte onto the substrate to prepare electrochemical energy storage devices.Both the printed active carbon/exfoliated graphene(AC/EG) electrode ink and electrolyte gel are highly processable with outstanding conductivity(~97 S cm^(-1) of electrode;-34.8 mS cm^(-1) of electrolyte),thus benefiting the corresponding shaping and electrochemical performances.Furthermore,the 3 D-printed symmetric MSCs can be operated stably at a high voltage up to 2.0 V in water-in-salt gel electrolyte,displaying ultrahigh areal capacitance of2381 mF cm^(-2) and exceptional energy density of 331 μWh cm^(-2),superior to previous printed micro energy units.In addition,we can further tailor the integrated 3 D-printed MSCs in parallel and series with various voltage and current outputs,enabling metal-free interconnection.Therefore,our all-3 D-printed MSCs place a great potential in developing high-power micro-electronics fabrication and integration.展开更多
Micro-supercapacitors(MSCs)are considered as highly competitive power sources for miniaturized electronics.However,narrow voltage window and poor anti-freezing properties of MSCs in conventional aqueous electrolytes l...Micro-supercapacitors(MSCs)are considered as highly competitive power sources for miniaturized electronics.However,narrow voltage window and poor anti-freezing properties of MSCs in conventional aqueous electrolytes lead to low energy density and limited environmental adaption.Herein,we report the construction of low-temperature and high-energy-density MSCs based on anti-freezing hybrid gel electrolytes(HGE)through introducing ethylene glycol(EG)additives into aqueous LiCl electrolyte.Since EG partially destroys hydrogen bond network among water molecules,the HGE exhibits maximum electrochemical stability window of 2.7 V and superior anti-freezing features with a glass transition temperature of-62.8℃.Further,the optimized MSCs using activated carbon microelectrodes possess impressive volumetric capacitance of 28.9 F cm^(-3)and energy density of 10.3 mWh cm^(-3)in the voltage of 1.6 V,2.6 times higher than MSCs tested in 1.2 V.Importantly,the MSCs display 68.3%capacitance retention even at-30℃ compared to the value at 25℃,and ultra-long cyclability with 85.7%of initial capacitance after 15,000 times,indicating extraordinary low-temperature performance.Besides,our devices offer favorable flexibility and modular integration.Therefore,this work provides a general strategy of realizing flexible,safe and anti-freezing microscale power sources,holding great potential towards subzero-temperature microelectronic applications.展开更多
Due to the rapid development of portable,wearable and implantable electronics in the fields of mobile communications,biomonitoring,and aerospace or defense,there is an increasing demand for miniaturized and lightweigh...Due to the rapid development of portable,wearable and implantable electronics in the fields of mobile communications,biomonitoring,and aerospace or defense,there is an increasing demand for miniaturized and lightweight energy storage devices.Micro-supercapacitors(MSCs)possessing long lifetime,high power density,environment friendliness and safety,have attracted great attention recently.Since the performance of the MSCs is mainly related to the structure of the active electrode,there is a great need to explore the efficient fabricating strategies to deterministically coordinate the structure and functionality of microdevices.Considering that laser technology possesses many superior features of facility,high-precision,low-cost,high-efficiency,shape-adaptability and maneuverability,herein we summarize the development of laser technologies in MSCs manufacturing,along with their strengths and weaknesses.The current achievements and challenges are also highlighted and discussed,aiming to provide a valuable reference for the rational design and manufacture of MSCs in the future.展开更多
Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin fi...Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.展开更多
Printed micro-supercapacitor exhibits its flexibility in geometry design and integration,showing unprecedented potential in powering the internet of things and portable devices.However,the printing process brings unde...Printed micro-supercapacitor exhibits its flexibility in geometry design and integration,showing unprecedented potential in powering the internet of things and portable devices.However,the printing process brings undesired processing defects(e.g.,coffee ring effect),resulting in severe self-discharge of the printed micro-supercapacitors.The impact of such problems on device performance is poorly understood,limiting further development of microsupercapacitors.Herein,by analyzing the self-discharge behavior of fully printed micro-supercapacitors,the severe self-discharge problem is accelerated by the ohmic leakage caused by the coffee ring effect on an ultrathin polymer electrolyte.Based on this understanding,the coffee ring effect was successfully eradicated by introducing graphene oxide in the polymer electrolyte,achieving a decline of 99%in the self-discharge rate.Moreover,the micro-supercapacitors with uniformly printed polymer electrolyte present 7.64 F cm^(-3)volumetric capacitance(14.37 mF cm^(-2)areal capacitance),exhibiting about 50%increase compared to the one without graphene oxide addition.This work provides a new insight to understand the relationship between processing defects and device performance,which will help improve the performance and promote the application of printed micro-supercapacitors.展开更多
Biomass carbon and small redox biomolecules are attractive materials for green,sustainable energy storage devices owing to their environmentally friendly,low-cost,scalable,and novel sources.However,most devices manufa...Biomass carbon and small redox biomolecules are attractive materials for green,sustainable energy storage devices owing to their environmentally friendly,low-cost,scalable,and novel sources.However,most devices manufactured using these materials have low specific capacitance,poor cycle stability,short lifetime,complexity,and low precision of device fabrication.Herein,we report the directed self-assembly of mononuclear anthraquinone(MAQ)derivatives and porous lignin-based graphene oxide(PLGO)into a renewable colloidal gel through noncovalent interactions.These self-assembled gel electrode materials exhibited high capacitance(484.8 F g^(−1) at a current density of 1 A g^(−1))and could be further printed as flexible micro-supercapacitors(FMSCs)with arbitrary patterns and a relatively high resolution on specific substrates.The FMSCs exhibited excellent areal capacitance(43.6 mF cm^(−2)),energy and power densities(6.1μWh cm^(−2) and 50μW cm^(−2),respectively),and cycle stability(>10,000 cycles).Furthermore,the printed FMSCs and integrated FMSC arrays exhibited remarkable flexibility while maintaining a stable capacitance.The proposed approach can be applied to other quinone biomolecules and biomass-based carbon materials.This study provides a basis for fabricating green and sustainable energy storage device architectures with high capacitance,long-term cycling,high scalability,and high precision.展开更多
Graphene-based electrodes with rational structural design have shown extraordinary prospect for en-hanced electrical double-layer capacitance of micro-supercapacitors(MSCs).Herein,a facile fabrication method for flexi...Graphene-based electrodes with rational structural design have shown extraordinary prospect for en-hanced electrical double-layer capacitance of micro-supercapacitors(MSCs).Herein,a facile fabrication method for flexible planar MSCs based on hierarchical graphene was demonstrated by using a laser-treated membrane for electrode patterning,complemented with hierarchical electrode configuration tak-ing full advantages of size-determined functional graphene.The in-plane interdigital shape of MSCs was defined through vacuum filtration with the assistance of the functionalized polypropylene(PP)mem-brane.The hierarchical graphene films were built by macroscopic assembly based on size effect of differ-ent lateral sized graphene sheets(rGO-LSL).The sample of MSCs based on rGO-L SL(MSCs-LSL)exhibited excellent volumetric capacitance of 6.7 F cm^(−3) and high energy density of 0.37 mWh cm−3.The MSCs-LSL presented superb flexibility and cycling stability with no capacitance deteroriated after 2000 cycles.This newly developed fabrication strategy is of good scalability and designability to manufacture flexible elec-trode for MSCs with customized shapes,while the construction of hierarchical graphene can enlighten the structural design of analogous two-dimensional materials for potential advanced electronics.展开更多
Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage...Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage of energy density is the main stumbling block for their practical applications.To solve this energy issue,constructing a three-dimensional(3D)electrode within the limited footprint area is proposed as a new solution for improving the energy storage capacity ofMSCs.In the last few years,extensive efforts have been devoted to developing 3D electrodes for MSCs,and significant progress and breakthrough have been achieved.While,there is still lack of systematic summary on the 3D electrode design strategies.To this end,it is imperative to outline the basic design conception,summarize the current states,and discuss the future research about 3D electrodes in MSCs based on the latest development.展开更多
Recently,micro-supercapacitors(MSCs)have undergone major development as next-generation micro-electrochemical energy storage devices for self-powered,integrated,and wearable systems,thanks to their excellent performan...Recently,micro-supercapacitors(MSCs)have undergone major development as next-generation micro-electrochemical energy storage devices for self-powered,integrated,and wearable systems,thanks to their excellent performance capability.In particular,their rapid frequency response characteristics make them potential candidates to replace conventional capacitors and function as alternating current(AC)line filters to rectify pulse energy or as current ripple filters in the kHz range.However,few papers have been published about the associated fundamental device components,architectures,and correct characterization of MSCs applied in filter applications.In addition,it is a huge challenge to achieve a balance between capacitance and frequency response,not yet to be overcome.This review comprehensively summarizes recent advances in MSCs for AC line-filtering,from fundamental mechanisms to appropriate characterization and emerging applications.Special attention is given to progress in microfabrication strategies,electrode materials,and electrolytes for high-frequency MSCs.We also present perspectives and insights into the development of MSCs in different frequency ranges for AC line-filtering applications.展开更多
Recently,two-dimensional(2D)transition metal carbides and carbonitrides(MXenes),have shown great potential in micro-supercapacitors(MSCs).However,the maximum voltage output of symmetric MXene MSCs is limited to 0.6 V ...Recently,two-dimensional(2D)transition metal carbides and carbonitrides(MXenes),have shown great potential in micro-supercapacitors(MSCs).However,the maximum voltage output of symmetric MXene MSCs is limited to 0.6 V due to the oxidation effects at high anodic potentials.Herein,we developed asymmetric micro-supercapacitors(AMSCs)based on titanium carbide MXene(Ti_(3)C_(2)Tx)and MXene-MoO_(2) electrodes with an enlarged voltage window of 1.2 V,which is twice wider than that of symmetric MXene MSCs.The 2D-0D MXene-MoO_(2) microelectrode is fabricated by homogenous dispersing zerodimensional(0D)MoO_(2) nanoparticles into MXene layers to impede layers stacking and MoO_(2) nanoparticles aggregation.Notably,the AMSCs delivered good electrochemical performances of areal capacitance of ~19 mF cm^(-2) and volumetric capacitance of 63 F cm^(-3) at a scan rate of 2 mV s^(-1),and high energy density of 9.7 mW h cm^(-3) at a power density of 0.198 W cm^(-3).The AMSCs also presented exceptionally mechanical flexibility under different bending states and excellent cyclic stability,with 88% capacitance retention after 10000 cycles at a discharge current density of 0.5 mA cm^(-2).For practical application,the serially connected AMSCs are fully affordable to power electronics,which is beneficial for soft and wearable power devices.展开更多
Owing to high power density and long cycle life,micro-supercapacitors(MSCs)are regarded as a prevalent energy storage unit for miniaturized electronics in modern life.A major bottleneck is achieving enhanced energy de...Owing to high power density and long cycle life,micro-supercapacitors(MSCs)are regarded as a prevalent energy storage unit for miniaturized electronics in modern life.A major bottleneck is achieving enhanced energy density without sacrificing both power density and cycle life.To this end,designing electrodes in a“smart”way has emerged as an effective strategy to achieve a trade-off between the energy and power densities of MSCs.In the past few years,considerable research efforts have been devoted to exploring new electrode materials for high capacitance,but designing clever configurations for electrodes has rarely been investigated from a structural point of view,which is also important for MSCs within a limited footprint area,in particular.This review article categorizes and arranges these“smart”design strategies of electrodes into three design concepts:layer-by-layer,scaffoldassisted and rolling origami.The corresponding strengths and challenges are comprehensively summarized,and the potential solutions to resolve these challenges are pointed out.Finally,the smart design principle of the electrodes of MSCs and key perspectives for future research in this field are outlined.展开更多
Ultracompact and customizable micro-supercapacitors(MSCs)are highly demanded for powering microscale electronics of 5G and Internet of Things technologies.So far,tremendous efforts have been concentrated on fabricatin...Ultracompact and customizable micro-supercapacitors(MSCs)are highly demanded for powering microscale electronics of 5G and Internet of Things technologies.So far,tremendous efforts have been concentrated on fabricating high-performance MSCs;however,compatible fabrication and monolithic integration of MSCs with microelectronic systems still remains a huge challenge taking into full consideration the factors such as electrode film fabrication,high-resolution microelectrode pattern,and electrolyte precise deposition.In this review,we summarize the recent advances of ultrasmall and integrated MSCs with tunable performance and customizable function,including key microfabrication technologies for patterning microelectrodes with superior resolution,precise deposition of customized electrolytes in an extremely small space,and feasible strategies for improving electrochemical performance by constructing thick microelectrodes and special electrode structure.Finally,the related challenges and key prospects of ultracompact and customizable MSCs,including compatible microfabrication methods for electrode materials and films,patterning microelectrodes,customizing shape-conformable electrolytes,performance optimization,and efficient integration with microelectronic systems,are put forward for further promoting their practical application.展开更多
Micro-supercapacitors(MSCs)show great potential as on-chip energy storage devices for portable electronics.The major flaw of thin-film MSCs is their low energy density.To improve the energy density,thicker electrodes ...Micro-supercapacitors(MSCs)show great potential as on-chip energy storage devices for portable electronics.The major flaw of thin-film MSCs is their low energy density.To improve the energy density,thicker electrodes are required.However,the fabrication of MSCs with thick electrodes remains a challenge.In this work,a novel 3D printing method is employed to fabricate high-performance MSCs with interdigitated exfoliated graphene(EG)/carbon nanotube(CNT)/silver nanowire(Ag NW)electrodes.The nanowelding of Ag NW junction plays a critical role in the realization of 3D printing.To enhance the electrochemical performances of EG,phosphorus atoms are incorporated into the carbon framework with 1.7 at%.The areal capacitance of the 3D printed MSC is 21.6 mF cm^(-2)at a scan rate of 0.01 V s^(-1).The areal energy density of the MSC ranges from 0.5 to 2μWh cm^(-2)with a maximum power density of 2.5 mW cm^(-2).展开更多
A novel type of sulfur-doped graphene fibers (S-GFs) were prepared by the hydrothermal strategy, the in situ interfacial polymerization method and the annealing method. Two S-GFs were assembled into an all-solid-state...A novel type of sulfur-doped graphene fibers (S-GFs) were prepared by the hydrothermal strategy, the in situ interfacial polymerization method and the annealing method. Two S-GFs were assembled into an all-solid-state fibriform micro-supercapacitor (micro-SC) that is flexible and has a high specific capacitance (4.55 mF·cm^-2) with the current density of 25.47 pA·cm^-2. The cyclic voltammetry (CV) curve of this micro-SC kept the rectangular shape well even when the scan rate reached 2 V·s^-1. There is a great potential for this type of S-GFs used in flexible wearable electronics.展开更多
基金financially supported by the National Natural Science Foundation of China (Grants. 22075279, 22279137, 22125903, 22109040)National Key R&D Program of China (Grant 2022YFA1504100)+2 种基金Dalian Innovation Support Plan for High Level Talents (2019RT09)Dalian National Labo- ratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL202016, DNL202019), DICP (DICP I2020032)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (YLU-DNL Fund 2021002, YLU- DNL Fund 2021009)。
文摘Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative electrode.Herein, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate capability.Benefiting from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.
基金the National Natural Science Foundation of China,China (Grant Nos.22125903,51872283,22109040)the“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No.XDA21000000)+4 种基金the Dalian Innovation Support Plan for High Level Talents,China (2019RT09)DICP,China (DICP I202032)the Dalian National Laboratory For Clean Energy (DNL),CAS,DNL Cooperation Fund,CAS,China (DNL202016,DNL202019)the Top-Notch Talent Program of Henan Agricultural University,China (30500947)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy,China (YLU-DNL Fund 2021002,YLU-DNL Fund 2021009)。
文摘The popularization of portable,implantable and wearable microelectronics has greatly stimulated the rapid development of high-power planar micro-supercapacitors(PMSCs).Particularly,the introduction of new functionalities(e.g.,high voltage,flexibility,stretchability,self-healing,electrochromism and photo/thermal response)to PMSCs is essential for building multifunctional PMSCs and their smart selfpowered integrated microsystems.In this review,we summarized the latest advances in PMSCs from various functional microdevices to their smart integrated microsystems.Primarily,the functionalities of PMSCs are characterized by three major factors to emphasize their electrochemical behavior and unique scope of application.These include but are not limited to high-voltage outputs(realized through asymmetric configuration,novel electrolyte and modular integration),mechanical resilience that includes various feats of flexibility or stretchability,and response to stimuli(self-healing,electrochromic,photo-responsive,or thermal-responsive properties).Furthermore,three representative integrated microsystems including energy harvester-PMSC,PMSC-energy consumption,and all-in-one selfpowered microsystems are elaborately overviewed to understand the emerging intelligent interaction models.Finally,the key perspectives,challenges and opportunities of PMSCs for powering smart microelectronics are proposed in brief.
基金supported by National Natural Science Foundation of China(Grant Nos.11274308 and 21401202)
文摘By means of inkjet printing technique, flexible and all-solid-state micro-supercapacitors(MSCs) were fabricated with carbon-based hybrid ink composed of graphene oxide(GO,98.0vol.%) ink and commercial pen ink(2.0vol.%). A small amount of commercial pen ink was added to effectively reduce the agglomeration of theGO sheets during solvent evaporation and the following reduction processes in which the presence of graphite carbon nanoparticles served as nano-spacer to separate GO sheets. The printed device fabricated using the hybrid ink,combined with the binder-free microelectrodes and interdigital microelectrode configuration, exhibits nearly 780%enhancement in areal capacitance compared with that of pure GO ink. It also shows excellent flexibility and cycling stability with nearly 100% retention of the areal capacitance after 10,000 cycles. The all-solid-state device can be optionally connected in series or in parallel to meet the voltage and capacity requirements for a given application.This work demonstrates a promising future of the carbonbased hybrid ink for directly large-scale inkjet printing MSCs for disposable energy storage devices.
基金This work was financially supported by the Natural Science Foundation of China(Grant No.51773062,61831021,51872283,21805273,22075279,22005297,22005298)the China Postdoctoral Science Foundation(Project No.2019M661421)+9 种基金the National Key R@D Program of China(Grants 2016YBF0100100,2016YFA0200200)the Liaoning BaiQianWan Talents Program,Liaoning Revitalization Talents Program(Grant XLYC1807153)the Natural Science Foundation of Liaoning Province,Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science(Grant 20180510038)the Dalian Innovation Support Plan for High Level Talents(2019RT09)DICP(DICP ZZBS201708,DICP ZZBS201802,and DICP 1202032)the DICP&QIBEBT(Grant DICP&QjBEBT UN201702)the Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL180310,DNL180308,DNL201912,and DNL201915)We thank Yucen Li and Prof.Ming Hu(East China Normal University,China)for the kind help in nitrogen absorption-desorption isotherms measurementalso thank the Material structure analysis center and Multifunctional Platform for Innovation of East China Normal University(003,004,006)the Center for Advanced Electronic Materials and Devices(AEMD)of Shanghai Jiao Tong University.
文摘Rational design and precise regulation over the morphology, structure, and pore size of functional conducting mesoporous polymers with enriched active sites and shorten electron–ion transport pathway are extremely important for developing high-performance micro-supercapacitors (MSCs), but still remain a great challenge. Herein, a general dual-colloid interface co-assembly strategy is proposed to fabricate hollow mesoporous polypyrrole nano-bowls (mPPy-nbs) for high-energy-density solid-state planar MSCs. By simply adjusting the size of block copolymer micelles, the diameter of polystyrene nanospheres and the amount of pyrrole monomer, mesopore size of the shell, void and shell thickness of mPPy-nbs can be simultaneously controlled. Importantly, this strategy can be further utilized to synthesize other hollow mesoporous polymers, including poly(tris(4-aminophenyl)amine), poly(1,3,5-triaminobenzene) and their copolymers, demonstrative of excellent universality. The structurally optimized mPPy-nb exhibits high specific surface area of 122 m^(2) g^(−1)and large capacitance of 225 F g^(−1) at 1 mV s^(−1). Furthermore, the MSCs assembled by mPPy-nbs deliver impressive volumetric capacitance of 90 F cm^(−3) and energy density of 2.0 mWh cm^(−3), superior to the most reported polymers-based MSCs. Also, the fabricated MSCs present excellent flexibility with almost no capacitance decay under varying bending states, and robust serial/parallel self-integration for boosting voltage and capacitance output. Therefore, this work will inspire the new design of mesoporous conducting polymer materials toward high-performance microscale supercapacitive devices.
基金financially supported by the National Key R&D Program of China (Grants 2016YFB0100100, 2016YFA0200200)the National Natural Science Foundation of China (Grants 51702078, 51572259, and 51872283)+4 种基金Natural Science Foundation of Liaoning ProvinceJoint Research Fund Liaoning-Shenyang National Laboratory for Materials Science (Grant 20180510038)Liao Ning Revitalization Talents Program (Grant XLYC1807153), DICP (DICP ZZBS201708, DICP ZZBS201802)DICP&QIBEBT (Grant DICP&QIBEBT UN201702)Dalian National Laboratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL180310, DNL180308, DNL201912, and DNL201915)。
文摘Microscale electrochemical energy storage devices,e.g., micro-supercapacitors(MSCs),possessing tailored performance and diversified form factors of lightweight,miniaturization,flexibility and exceptional integration are highly necessary for the smart power sources-unitized electronics.Despite the great progress,the fabrication of MSCs combining high integration with high volumetric performance remains largely unsolved.Herein,we develop a simple,fast and scalable strategy to fabricate graphene based highly integrated MSCs by a new effective continuous centrifugal coating technique.Notably,the resulting highly conductive graphene films can act as not only patterned microelectrodes but also metal-free current collectors and interconnects,endowing modular MSCs with high integrity,remarkable flexibility,tailored voltage and capacitance output,and outstanding performance uniformity.More importantly,the strong centrifugal force and shear force generated in continuous centrifugal coating process lead to graphene films with high alignment,compactness and packing density,contributing to excellent volumetric capacitance of ~31.8 F cm^(-3) and volumetric energy density of ~2.8 mWh cm^(-3),exceeding most reported integrated MSCs.Therefore,our work paves a novel way for simple and scalable fabrication of integrated MSCs and offers promising opportunities as standalone microscale power sources for new-generation electronics.
基金financially supported by the Natural Science Basic Research Plan in Shaanxi Province of China (2019ZDLGY1602)the Youth Science and Technology Nova Program of Shaanxi Province (2020KJXX-068)+8 种基金the Fundamental Research Funds for the Central Universities (JBF201101)the National Key R@D Program of China (2016YFA0200200)the National Natural Science Foundation of China (22125903, 51872283, 22075279, 21805273, 22109160)the Liao Ning Revitalization Talents Program (XLYC1807153)the Liaoning Bai Qian Wan Talents Program, Dalian Innovation Support Plan for High Level Talents (2019RT09)the Dalian National Laboratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL201912, DNL201915, DNL202016, DNL202019)DICP (DICP ZZBS201708, DICP ZZBS201802, DICP I2020032)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (YLU-DNL Fund 2021002, 2021009)the China Postdoctoral Science Foundation (2021M693126, 2021M693127, 2019M661141, 2020M680995)。
文摘Harnessing energy from the environment promotes the rapid development of micro-power generators and relevant power management modules of alternating current (AC) line-filtering to obtain a stabilized direct current (DC) output for storage and use. Micro-supercapacitors (MSCs) with miniaturized volume and high-frequency response are regarded as a critical component in filtering circuits for microscale power conversion. Here, we reported the fabrication of the wafer-sized planar MSCs (M-MSCs) based on 2D Ti_(2)C_(2)T_(6) MXene using a photolithography technique. The M-MSCs exhibited an areal capacitance of 153 μF cm^(-2) and a frequency characteristic (f_(0)) of 5.6 k Hz in aqueous electrolyte. Moreover, by employing suitable ionic liquid as electrolyte, the voltage window was expanded to 2 V and the f_(0) could be pushed to 6.6 k Hz relying on the electrical double-layer mechanism and lower adsorption energy while maintaining quasi-rectangular cyclic voltammogram curves at 5000 V s^(-1). Furthermore, the integrated MSCs pack was constructed and exhibited excellent rectifying ability by filtering various highfrequency 5000 Hz AC signals with different waveforms into stable DC outputs. Such ultrahigh-rate and high-voltage M-MSCs module for k Hz AC line-filtering would be potentially integrated with customizable electronics to realize on-chip rectifiers in high-density integrated circuit.
基金financially supported by the National Key R@D Program of China (2016YFB0100100, 2016YFA0200200)the National Natural Science Foundation of China (51872283,22075279, 21805273, 22005297, 22005298)+7 种基金the Liao Ning Revitalization Talents Program (XLYC1807153)the Central Government of Liaoning Province Guides The Funds for Local Science and Technology Development (2021JH6/10500112)the Dalian Innovation Support Plan for High Level Talents (2019RT09)the Dalian National Laboratory For Clean Energy (DNL),CASDNL Cooperation Fund,CAS (DNL201912, DNL201915, DNL202016, DNL202019)DICP (DICP ZZBS201708, DICP ZZBS201802, DICP I2020032)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (YLU-DNL Fund 2021002)the China Postdoctoral Science Foundation (2019 M661141, 2020 M680995)。
文摘With the rapid development of integrated and miniaturized electronics,the planar energy storage devices with high capacitance and energy density are in enormous demand.Hence,the advanced manufacture and fast fabrication of microscale planar energy units are of great significance.Herein,we develop aqueous planar micro-supercapacitors(MSCs) with ultrahigh areal capacitance and energy density via an efficient all-3 D-printing strategy,which can directly extrude the active material ink and gel electrolyte onto the substrate to prepare electrochemical energy storage devices.Both the printed active carbon/exfoliated graphene(AC/EG) electrode ink and electrolyte gel are highly processable with outstanding conductivity(~97 S cm^(-1) of electrode;-34.8 mS cm^(-1) of electrolyte),thus benefiting the corresponding shaping and electrochemical performances.Furthermore,the 3 D-printed symmetric MSCs can be operated stably at a high voltage up to 2.0 V in water-in-salt gel electrolyte,displaying ultrahigh areal capacitance of2381 mF cm^(-2) and exceptional energy density of 331 μWh cm^(-2),superior to previous printed micro energy units.In addition,we can further tailor the integrated 3 D-printed MSCs in parallel and series with various voltage and current outputs,enabling metal-free interconnection.Therefore,our all-3 D-printed MSCs place a great potential in developing high-power micro-electronics fabrication and integration.
基金financially supported by the National Natural Science Foundation of China(22125903,51872283,22109160,22005297)the Dalian Innovation Support Plan for High Level Talents(2019RT09)+6 种基金the The Joint Fund of the Yulin University and the Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL201912,DNL201915,DNL202016,DNL202019),DICP(DICP ZZBS201802,DICP I2020032)The Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002,YLU-DNL Fund 2021009)the China Postdoctoral Science Foundation(2021M693126,2020M680995,2021M703145,2021M693127)the International Postdoctoral Exchange Fellowship Program(Talent-Introduction Program)(YJ20210311)the Plan for promoting innovative talents of Education Department of Liaoning Province(LCR2018015)the Shenyang Youth Science and Technology Project(RC200444)the Natural Science Foundation of Liaoning Province(2021-MS-234)。
文摘Micro-supercapacitors(MSCs)are considered as highly competitive power sources for miniaturized electronics.However,narrow voltage window and poor anti-freezing properties of MSCs in conventional aqueous electrolytes lead to low energy density and limited environmental adaption.Herein,we report the construction of low-temperature and high-energy-density MSCs based on anti-freezing hybrid gel electrolytes(HGE)through introducing ethylene glycol(EG)additives into aqueous LiCl electrolyte.Since EG partially destroys hydrogen bond network among water molecules,the HGE exhibits maximum electrochemical stability window of 2.7 V and superior anti-freezing features with a glass transition temperature of-62.8℃.Further,the optimized MSCs using activated carbon microelectrodes possess impressive volumetric capacitance of 28.9 F cm^(-3)and energy density of 10.3 mWh cm^(-3)in the voltage of 1.6 V,2.6 times higher than MSCs tested in 1.2 V.Importantly,the MSCs display 68.3%capacitance retention even at-30℃ compared to the value at 25℃,and ultra-long cyclability with 85.7%of initial capacitance after 15,000 times,indicating extraordinary low-temperature performance.Besides,our devices offer favorable flexibility and modular integration.Therefore,this work provides a general strategy of realizing flexible,safe and anti-freezing microscale power sources,holding great potential towards subzero-temperature microelectronic applications.
基金supported by the National Key R&D Program of China(2017YFB1104300)NSFC(22075019,21604003)+1 种基金the Beijing Natural Science Foundation(2152028,2164070)the Beijing Municipal Science and Technology Commission(Z161100002116022)。
文摘Due to the rapid development of portable,wearable and implantable electronics in the fields of mobile communications,biomonitoring,and aerospace or defense,there is an increasing demand for miniaturized and lightweight energy storage devices.Micro-supercapacitors(MSCs)possessing long lifetime,high power density,environment friendliness and safety,have attracted great attention recently.Since the performance of the MSCs is mainly related to the structure of the active electrode,there is a great need to explore the efficient fabricating strategies to deterministically coordinate the structure and functionality of microdevices.Considering that laser technology possesses many superior features of facility,high-precision,low-cost,high-efficiency,shape-adaptability and maneuverability,herein we summarize the development of laser technologies in MSCs manufacturing,along with their strengths and weaknesses.The current achievements and challenges are also highlighted and discussed,aiming to provide a valuable reference for the rational design and manufacture of MSCs in the future.
基金financial support of the Swedish Research Council through the Marie Sklodowska-Curie International Career Grant (No.2015-00395,co-funded by Marie Sklodowska-Curie Actions, through the Project INCA 600398)the Formas Foundation through the Future Research Leaders Grant (No.2016-00496)+3 种基金the AForsk Foundation (Grant No.17-352)the Olle Engkvist Byggmastare Foundation (Grant No.2014/799)the Academy of Finland (Grant No.288945 and 319408)Academy of Finland Research Infrastructure "Printed Intelligence Infrastructure" (PII-FIRI,Grant No. 320019)
文摘Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.
基金the financial support of this work by the Science,Technology,and Innovation Commission of Shenzhen Municipality(Program No.JCYJ20180508151856806,No.JCYJ20180306171355233)the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(Program No.CX201944)。
文摘Printed micro-supercapacitor exhibits its flexibility in geometry design and integration,showing unprecedented potential in powering the internet of things and portable devices.However,the printing process brings undesired processing defects(e.g.,coffee ring effect),resulting in severe self-discharge of the printed micro-supercapacitors.The impact of such problems on device performance is poorly understood,limiting further development of microsupercapacitors.Herein,by analyzing the self-discharge behavior of fully printed micro-supercapacitors,the severe self-discharge problem is accelerated by the ohmic leakage caused by the coffee ring effect on an ultrathin polymer electrolyte.Based on this understanding,the coffee ring effect was successfully eradicated by introducing graphene oxide in the polymer electrolyte,achieving a decline of 99%in the self-discharge rate.Moreover,the micro-supercapacitors with uniformly printed polymer electrolyte present 7.64 F cm^(-3)volumetric capacitance(14.37 mF cm^(-2)areal capacitance),exhibiting about 50%increase compared to the one without graphene oxide addition.This work provides a new insight to understand the relationship between processing defects and device performance,which will help improve the performance and promote the application of printed micro-supercapacitors.
基金supported by the National Natural Science Foundation of China(Grant Nos.21905069 and U21A20307)the Shenzhen Science and Technology Innovation Committee(Grant Nos.ZDSYS20190902093220279,KQTD20170809110344233,GXWD20201230155427003-20200821181245001,GXWD20201230155427003-20200821181809001,and ZX20200151)+1 种基金the Department of Science and Technology of Guangdong Province(Grant No.2020A1515110879)University Stable Support Foundation of Shenzhen(Grant No.GXWD20201230155427003-20200821181809001).
文摘Biomass carbon and small redox biomolecules are attractive materials for green,sustainable energy storage devices owing to their environmentally friendly,low-cost,scalable,and novel sources.However,most devices manufactured using these materials have low specific capacitance,poor cycle stability,short lifetime,complexity,and low precision of device fabrication.Herein,we report the directed self-assembly of mononuclear anthraquinone(MAQ)derivatives and porous lignin-based graphene oxide(PLGO)into a renewable colloidal gel through noncovalent interactions.These self-assembled gel electrode materials exhibited high capacitance(484.8 F g^(−1) at a current density of 1 A g^(−1))and could be further printed as flexible micro-supercapacitors(FMSCs)with arbitrary patterns and a relatively high resolution on specific substrates.The FMSCs exhibited excellent areal capacitance(43.6 mF cm^(−2)),energy and power densities(6.1μWh cm^(−2) and 50μW cm^(−2),respectively),and cycle stability(>10,000 cycles).Furthermore,the printed FMSCs and integrated FMSC arrays exhibited remarkable flexibility while maintaining a stable capacitance.The proposed approach can be applied to other quinone biomolecules and biomass-based carbon materials.This study provides a basis for fabricating green and sustainable energy storage device architectures with high capacitance,long-term cycling,high scalability,and high precision.
基金financially supported by the National Natural Science Foundation of China (No.51975218 and U22A20193)the Natural Science Foundation of Guangdong Province (No.2021A1515010642)+2 种基金the Science and Technology Planning Project of Guangdong Province (No.2021A0505110002)the Fundamental Research Funds for the Central Universities (No.2022ZYGXZR101)the S&T Innovation Projects of Zhuhai City (No.ZH01110405180034PWC).
文摘Graphene-based electrodes with rational structural design have shown extraordinary prospect for en-hanced electrical double-layer capacitance of micro-supercapacitors(MSCs).Herein,a facile fabrication method for flexible planar MSCs based on hierarchical graphene was demonstrated by using a laser-treated membrane for electrode patterning,complemented with hierarchical electrode configuration tak-ing full advantages of size-determined functional graphene.The in-plane interdigital shape of MSCs was defined through vacuum filtration with the assistance of the functionalized polypropylene(PP)mem-brane.The hierarchical graphene films were built by macroscopic assembly based on size effect of differ-ent lateral sized graphene sheets(rGO-LSL).The sample of MSCs based on rGO-L SL(MSCs-LSL)exhibited excellent volumetric capacitance of 6.7 F cm^(−3) and high energy density of 0.37 mWh cm−3.The MSCs-LSL presented superb flexibility and cycling stability with no capacitance deteroriated after 2000 cycles.This newly developed fabrication strategy is of good scalability and designability to manufacture flexible elec-trode for MSCs with customized shapes,while the construction of hierarchical graphene can enlighten the structural design of analogous two-dimensional materials for potential advanced electronics.
基金China Scholarship CouncilDeutsche Forschungsgemeinschaft,Grant/Award Numbers:LE 2249/4-1,LE 2249/5-1Bundesministerium für Bildung und Forschung,Grant/Award Number:03Z1MN11。
文摘Owing to the high power density,long cycle life and maintain-free,micro-supercapacitors(MSCs)stand out as preferred miniaturized energy source for themiscellaneous autonomous electronic components.However,the shortage of energy density is the main stumbling block for their practical applications.To solve this energy issue,constructing a three-dimensional(3D)electrode within the limited footprint area is proposed as a new solution for improving the energy storage capacity ofMSCs.In the last few years,extensive efforts have been devoted to developing 3D electrodes for MSCs,and significant progress and breakthrough have been achieved.While,there is still lack of systematic summary on the 3D electrode design strategies.To this end,it is imperative to outline the basic design conception,summarize the current states,and discuss the future research about 3D electrodes in MSCs based on the latest development.
基金This work was financially supported by the Natural Science Basic Research Plan in Shaanxi Province of China(Program No.2019ZDLGY16-02)Youth Science and Technology Nova Program of Shaanxi Province(2020KJXX-068)+8 种基金Fundamental Research Funds for the Cornell University(Program No.JBF201101)National Key R@D Program of China(Grant 2016YFA0200200)the National Natural Science Foundation of China(Grant Nos.22125903,51872283,22075279,22109160)the Liao Ning Revitalization Talents Program(Grant XLYC1807153)Dalian Innovation Support Plan for High Level Talents(2019RT09)Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL201912,DNL201915,DNL202016,DNL202019)DICP(DICP ZZBS201708,DICP ZZBS201802,DICP I2020032)The Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002)China Postdoctoral Science Foundation(2021M693126,2019M661141,2020M680995).
文摘Recently,micro-supercapacitors(MSCs)have undergone major development as next-generation micro-electrochemical energy storage devices for self-powered,integrated,and wearable systems,thanks to their excellent performance capability.In particular,their rapid frequency response characteristics make them potential candidates to replace conventional capacitors and function as alternating current(AC)line filters to rectify pulse energy or as current ripple filters in the kHz range.However,few papers have been published about the associated fundamental device components,architectures,and correct characterization of MSCs applied in filter applications.In addition,it is a huge challenge to achieve a balance between capacitance and frequency response,not yet to be overcome.This review comprehensively summarizes recent advances in MSCs for AC line-filtering,from fundamental mechanisms to appropriate characterization and emerging applications.Special attention is given to progress in microfabrication strategies,electrode materials,and electrolytes for high-frequency MSCs.We also present perspectives and insights into the development of MSCs in different frequency ranges for AC line-filtering applications.
基金financially supported by the Australian Research Council Discovery Program(DP190103290)Australian Research Council Discovery Early Career Researcher Award scheme(DE150101617).
文摘Recently,two-dimensional(2D)transition metal carbides and carbonitrides(MXenes),have shown great potential in micro-supercapacitors(MSCs).However,the maximum voltage output of symmetric MXene MSCs is limited to 0.6 V due to the oxidation effects at high anodic potentials.Herein,we developed asymmetric micro-supercapacitors(AMSCs)based on titanium carbide MXene(Ti_(3)C_(2)Tx)and MXene-MoO_(2) electrodes with an enlarged voltage window of 1.2 V,which is twice wider than that of symmetric MXene MSCs.The 2D-0D MXene-MoO_(2) microelectrode is fabricated by homogenous dispersing zerodimensional(0D)MoO_(2) nanoparticles into MXene layers to impede layers stacking and MoO_(2) nanoparticles aggregation.Notably,the AMSCs delivered good electrochemical performances of areal capacitance of ~19 mF cm^(-2) and volumetric capacitance of 63 F cm^(-3) at a scan rate of 2 mV s^(-1),and high energy density of 9.7 mW h cm^(-3) at a power density of 0.198 W cm^(-3).The AMSCs also presented exceptionally mechanical flexibility under different bending states and excellent cyclic stability,with 88% capacitance retention after 10000 cycles at a discharge current density of 0.5 mA cm^(-2).For practical application,the serially connected AMSCs are fully affordable to power electronics,which is beneficial for soft and wearable power devices.
基金Sino‐German Center for Research Promotion,Grant/Award Number:GZ1579China Scholarship Council,Grant/Award Number:201908530218Deutsche Forschungsgemeinschaft,Grant/Award Number:LE 2249/5‐1。
文摘Owing to high power density and long cycle life,micro-supercapacitors(MSCs)are regarded as a prevalent energy storage unit for miniaturized electronics in modern life.A major bottleneck is achieving enhanced energy density without sacrificing both power density and cycle life.To this end,designing electrodes in a“smart”way has emerged as an effective strategy to achieve a trade-off between the energy and power densities of MSCs.In the past few years,considerable research efforts have been devoted to exploring new electrode materials for high capacitance,but designing clever configurations for electrodes has rarely been investigated from a structural point of view,which is also important for MSCs within a limited footprint area,in particular.This review article categorizes and arranges these“smart”design strategies of electrodes into three design concepts:layer-by-layer,scaffoldassisted and rolling origami.The corresponding strengths and challenges are comprehensively summarized,and the potential solutions to resolve these challenges are pointed out.Finally,the smart design principle of the electrodes of MSCs and key perspectives for future research in this field are outlined.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22125903,51872283,22005297,and 22109160)the“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21000000)+4 种基金Dalian Innovation Support Plan for High Level Talents(No.2019RT09)Dalian National Laboratory For Clean Energy(DNL),Chinese Academy of Sciences(CAS),DNL Cooperation Fund,CAS(Nos.DNL201912,DNL201915,DNL202016,and DNL202019)Dalian Institute of Chemical Physics(Nos.DICP ZZBS201802 and DICP I2020032)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Nos.YLU-DNL Fund 2021002 and YLU-DNL Fund 2021009)China Postdoctoral Science Foundation(Nos.2021M693127,2020M680995,and 2021M693126).
文摘Ultracompact and customizable micro-supercapacitors(MSCs)are highly demanded for powering microscale electronics of 5G and Internet of Things technologies.So far,tremendous efforts have been concentrated on fabricating high-performance MSCs;however,compatible fabrication and monolithic integration of MSCs with microelectronic systems still remains a huge challenge taking into full consideration the factors such as electrode film fabrication,high-resolution microelectrode pattern,and electrolyte precise deposition.In this review,we summarize the recent advances of ultrasmall and integrated MSCs with tunable performance and customizable function,including key microfabrication technologies for patterning microelectrodes with superior resolution,precise deposition of customized electrolytes in an extremely small space,and feasible strategies for improving electrochemical performance by constructing thick microelectrodes and special electrode structure.Finally,the related challenges and key prospects of ultracompact and customizable MSCs,including compatible microfabrication methods for electrode materials and films,patterning microelectrodes,customizing shape-conformable electrolytes,performance optimization,and efficient integration with microelectronic systems,are put forward for further promoting their practical application.
基金supported by the National Natural Science Foundation of China(Grant Nos.51925704,51877214,51607187,and 51907203)the Hubei Provincial Natural Science Foundation of China(Grant Nos.2019CFB371,and 2019CFB373)the Special Financial Aid to China Postdoctoral Science Foundation(Grant No.2019T120972)。
文摘Micro-supercapacitors(MSCs)show great potential as on-chip energy storage devices for portable electronics.The major flaw of thin-film MSCs is their low energy density.To improve the energy density,thicker electrodes are required.However,the fabrication of MSCs with thick electrodes remains a challenge.In this work,a novel 3D printing method is employed to fabricate high-performance MSCs with interdigitated exfoliated graphene(EG)/carbon nanotube(CNT)/silver nanowire(Ag NW)electrodes.The nanowelding of Ag NW junction plays a critical role in the realization of 3D printing.To enhance the electrochemical performances of EG,phosphorus atoms are incorporated into the carbon framework with 1.7 at%.The areal capacitance of the 3D printed MSC is 21.6 mF cm^(-2)at a scan rate of 0.01 V s^(-1).The areal energy density of the MSC ranges from 0.5 to 2μWh cm^(-2)with a maximum power density of 2.5 mW cm^(-2).
文摘A novel type of sulfur-doped graphene fibers (S-GFs) were prepared by the hydrothermal strategy, the in situ interfacial polymerization method and the annealing method. Two S-GFs were assembled into an all-solid-state fibriform micro-supercapacitor (micro-SC) that is flexible and has a high specific capacitance (4.55 mF·cm^-2) with the current density of 25.47 pA·cm^-2. The cyclic voltammetry (CV) curve of this micro-SC kept the rectangular shape well even when the scan rate reached 2 V·s^-1. There is a great potential for this type of S-GFs used in flexible wearable electronics.
