The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy s...The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.展开更多
The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
MXene-based aqueous symmetric supercapacitors(SSCs)are attractive due to their good rate performances and green nature.However,it remains a challenge to reach voltages much over 1.2 V,which significantly diminishes th...MXene-based aqueous symmetric supercapacitors(SSCs)are attractive due to their good rate performances and green nature.However,it remains a challenge to reach voltages much over 1.2 V,which significantly diminishes their energy density.Herein,we report on Mo_(1.33)CTz MXene-based SSCs possessing high voltages in a 19.5 M LiCl electrolyte.Benefiting from the vacancy-rich structure and high stable potential window of Mo_(1.33)CTz,the obtained SSCs deliver a maximum energy density of>38.2 mWh cm^(-3) at a power density of 196.6 mW cm^(-3) under an operating voltage of 1.4 V,along with excellent rate performance and impressive cycling stability.This highly concentrated LiCl electrolyte is also applicable to Ti_(3)C_(2)Tz,the most widely studied MXene,achieving a maximum energy density of>41.3 mWh cm^(-3) at a power density of 165.2 mW cm^(-3) with an operating voltage of 1.8 V.The drop in energy density with increasing power in the Ti_(3)C_(2)Tz cells was steeper than for the Mo-based cells.This work provides a roadmap to develop superior SSCs with high voltages and high energy densities.展开更多
Thermal energy storage(TES)solutions offer opportunities to reduce energy consumption,greenhouse gas emissions,and cost.Specifically,they can help reduce the peak load and address the intermittency of renewable energy...Thermal energy storage(TES)solutions offer opportunities to reduce energy consumption,greenhouse gas emissions,and cost.Specifically,they can help reduce the peak load and address the intermittency of renewable energy sources by time shifting the load,which are critical toward zero energy buildings.Thermochemical materials(TCMs)as a class of TES undergo a solid-gas reversible chemical reaction with water vapor to store and release energy with high storage capacities(600 kWh m^(-3))and negligible self-discharge that makes them uniquely suited as compact,stand-alone units for daily or seasonal storage.However,TCMs suffer from instabilities at the material(salt particles)and reactor level(packed beds of salt),resulting in poor multi-cycle efficiency and high-levelized cost of storage.In this study,a model is developed to predict the pulverization limit or Rcrit of various salt hydrates during thermal cycling.This is critical as it provides design rules to make mechanically stable TCM composites as well as enables the use of more energy-efficient manufacturing process(solid-state mixing)to make the composites.The model is experimentally validated on multiple TCM salt hydrates with different water content,and effect of Rcrit on hydration and dehydration kinetics is also investigated.展开更多
Efficient energy storage devices with suitable electrode materials,that integrate high power and high energy,are the crucial requisites of the renewable power source,which have unwrapped new possibilities in the susta...Efficient energy storage devices with suitable electrode materials,that integrate high power and high energy,are the crucial requisites of the renewable power source,which have unwrapped new possibilities in the sustainable development of energy and the environment.Herein,a facile collagen microstructure modulation strategy is proposed to construct a nitrogen/oxygen dual-doped hierarchically porous carbon fiber with ultrahigh specific surface area(2788 m^(2)g^(-1))and large pore volume(4.56 cm^(3)g^(-1))via local microfibrous breakage/disassembly of natural structured proteins.Combining operando spectroscopy and density functional theory unveil that the dual-heteroatom doping could effectively regulate the electronic structure of carbon atom framework with enhanced electric conductivity and electronegativity as well as decreased diffusion resistance in favor of rapid pseudocapacitive-dominated Li^(+)-storage(353 mAh g^(-1)at 10 A g^(-1)).Theoretical calculations reveal that the tailored micro-/mesoporous structures favor the rapid charge transfer and ion storage,synergistically realizing high capacity and superior rate performance for NPCF-H cathode(75.0 mAh g^(-1)at 30 A g^(-1)).The assembled device with NPCF-H as both anode and cathode achieves extremely high energy density(200 Wh kg^(-1))with maximum power density(42600 W kg^(-1))and ultralong lifespan(80%capacity retention over 10000 cycles).展开更多
Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising...Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising due to its intrinsic high hydrogen capacity.Hydrolysis reaction of LSHS materials occurs at moderate conditions,indicating the potential for portable applications.At present,most of review work focuses on the improvement of material performance,especially the catalysts design.This part is important,but the others,such as operation modes,are also vital to to make full use of material potential in the practical applications.Different operation modes of hydrolysis reaction have an impact on hydrogen capacity to various degrees.For example,hydrolysis in solution would decrease the hydrogen capacity of hydrogen generator to a low value due to the excessive water participating in the reaction.Therefore,application-oriented operation modes could become a key problem for hydrolysis reaction of LSHS materials.In this paper,the operation modes of hydrolysis reaction and their practical applications are mainly reviewed.The implements of each operation mode are discussed and compared in detail to determine the suitable one for practical applications with the requirement of high energy density.The current challenges and future directions are also discussed.展开更多
Although room temperature ionic liquids(ILs)have emerged as potential next-generation electrolytes for their wide electrochemical stability window(ESW),the trade-off between this window and viscosity has hindered thei...Although room temperature ionic liquids(ILs)have emerged as potential next-generation electrolytes for their wide electrochemical stability window(ESW),the trade-off between this window and viscosity has hindered their widespread use in energy storage devices.Here,we present for the first time that such a trade-off can be balanced by mixing two ILs with the common anion([NTf_(2)]^(-))but different cations([EMIM]^(+) and[N1114]^(+))together.The[EMIM]cation-based IL possesses low viscosity while the[N1114]cation-based IL exhibits wide ESW.Since the concentrations of each IL in the mixtures can result in different electrolyte properties,we demonstrate a systematic approach by exploring the properties of various concentration combinations.In addition,the corresponding cell voltage of their resulting graphene supercapacitors(SCs)accompanied based on the interaction between the binary ionic liquid and the electrodes,and the associated electrochemical performance were studied to determine the optimum electrolyte system for the highest SC energy density.The well-balanced viscosity/ESW trade-off is achieved in binary IL consisting 50 vol%[EMIM][NTf_(2)]and 50 vol%[N1114][NTf_(2)]as evident from the extraordinary electrode specific capacitance of 293.1 F g^(-1) and the ultrahigh SC energy density of 177 Wh kg^(-1),which approaches that of a lithium-ion battery.展开更多
Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform a...Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform an extensive structure search of ternary carbon-nitrogen-oxygen(CNO)compound under high pressure with the CALYPSO method and first principles calculations,and successfully identify three polymeric CNO compounds with Pbam,C2/m and I4m2symmetries under 100 GPa.More interestingly,these structures are also dynamically stable at ambient pressure,and are potential high energy density materials(HEDMs).The energy densities of Pbam,C2/m and I4m2 phases of CNO are about2.30 kJ/g,1.37 kJ/g and 2.70 kJ/g,respectively,with the decompositions of graphitic carbon and molecular carbon dioxide andα-N(molecular N_(2))at ambient pressure.The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures,which offer crucial insights for designs and syntheses of novel HEDMs.展开更多
The limited energy density of lithium-ion capacitors poses a significant obstacle to their widespread application,primarily stemming from the inability of the electrodes to simultaneously fulfill both high energy dens...The limited energy density of lithium-ion capacitors poses a significant obstacle to their widespread application,primarily stemming from the inability of the electrodes to simultaneously fulfill both high energy density and rapid charging requirements.Experimental data demonstrate that a directional particle configuration can enhance charging speed while maintaining high-capacity density,but it is rarely discussed.Here,we have developed a particle-level electrochemical model capable of reconstructing an electrode with a directional particle configuration.By employing this method,an investigation was conducted to explore how the spatial morphology characteristics of particle configuration impact the energy storage characteristics of electrodes.Results demonstrate that rational particle configuration can effectively enhance the transport of lithium ions and create additional space for lithium-ion storage.With the same particle size distribution,the best electrode can increase the discharge capacity by up to132.4% and increase the charging SOC by 11.3% compared to the ordinary electrode under the condition of 6 C.These findings provide a further understanding of the energy storage mechanism inside the anisotropic particle distribution electrode,which is important for developing high-performance lithium-ion capacitors.展开更多
Preparation of hierarchically porous, heteroatom-rich nanostructured carbons through green and scalable routes plays a key role for practical energy storage applications. In this work, naturally abundant lignocellulos...Preparation of hierarchically porous, heteroatom-rich nanostructured carbons through green and scalable routes plays a key role for practical energy storage applications. In this work, naturally abundant lignocellulosic agricultural waste with high initial oxygen content, hazelnut shells, were hydrothermally carbonized and converted into nanostructured ‘hydrochar’. Environmentally benign ceramic/magnesium oxide(Mg O) templating was used to introduce porosity into the hydrochar. Electrochemical performance of the resulting material(HM700) was investigated in aqueous solutions of 1 M H;SO;, 6 M KOH and1 M Na;SO;, using a three-electrode cell. HM700 achieved a high specific capacitance of 323.2 F/g in 1 M H;SO;(at 1 A/g,-0.3 to 0.9 V vs. Ag/Ag Cl) due to the contributions of oxygen heteroatoms(13.5 wt%)to the total capacitance by pseudo-capacitive effect. Moreover, a maximum energy density of 11.1 Wh/kg and a maximum power density of 3686.2 W/kg were attained for the symmetric supercapacitor employing HM700 as electrode material(1 M Na;SO;, E = 2 V), making the device promising for green supercapacitor applications.展开更多
Designing high-performance electrodes via 3D printing for advanced energy storage is appealing but remains challenging.In normal cases,light-weight carbonaceous materials harnessing excellent electrical conductivity h...Designing high-performance electrodes via 3D printing for advanced energy storage is appealing but remains challenging.In normal cases,light-weight carbonaceous materials harnessing excellent electrical conductivity have served as electrode candidates.However,they struggle with undermined areal and volumetric energy density of supercapacitor devices,thereby greatly impeding the practical applications.Herein,we demonstrate the in situ coupling of NiCoP bimetallic phosphide and Ti3C2 MXene to build up heavy NCPM electrodes affording tunable mass loading throughout 3D printing technology.The resolution of prints reaches 50μm and the thickness of device electrodes is ca.4 mm.Thus-printed electrode possessing robust open framework synergizes favorable capacitance of NiCoP and excellent conductivity of MXene,readily achieving a high areal and volumetric capacitance of 20 F cm^-2 and 137 F cm^-3 even at a high mass loading of^46.3 mg cm^-2.Accordingly,an asymmetric supercapacitor full cell assembled with 3D-printed NCPM as a positive electrode and 3D-printed activated carbon as a negative electrode harvests remarkable areal and volumetric energy density of 0.89 mWh cm^-2 and 2.2 mWh cm^-3,outperforming the most of state-of-the-art carbon-based supercapacitors.The present work is anticipated to offer a viable solution toward the customized construction of multifunctional architectures via 3D printing for high-energy-density energy storage systems.展开更多
Paraffin/γ-Al2O3 composites as phase change energy storage materials were prepared by absorbing paraffin in porous network of γ-Al2O3.In the composite materials,paraffin was used as a phase change material(PCM)for t...Paraffin/γ-Al2O3 composites as phase change energy storage materials were prepared by absorbing paraffin in porous network of γ-Al2O3.In the composite materials,paraffin was used as a phase change material(PCM)for thermal energy storage,and γ-Al2O3 acted as supporting materials.Characterizations were conducted to evaluate the energy storage performance of the composites,and differential scanning calorimeter results showed that the PCM-3 composite has melting latent heat of 112.9 kJ/kg with a melting temperature of 62.9 ℃.Due to strong capillary force and surface tension between paraffin and γ-Al2O3,the leakage of melted paraffin from the composites can be effectively prevented.Therefore,the paraffin/γ-Al2O3 composites have a good thermal stability and can be used repeatedly.展开更多
Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulo...Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of LIBs.Herein,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the CNTs.More importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.展开更多
Zinc ion hybrid supercapacitor (ZIHSC) with promising energy and power densities is an excellent answer to the ever-growing demand for energy storage devices.The restricted lifespan due to the dendrite formation on me...Zinc ion hybrid supercapacitor (ZIHSC) with promising energy and power densities is an excellent answer to the ever-growing demand for energy storage devices.The restricted lifespan due to the dendrite formation on metallic zinc (Zn) is one of the main roadblocks.Herein,we investigate the electrochemical capability of oxygen-enriched porous carbon nanofibers (A-CNF) and nitrogen,oxygen-enriched porous carbon nanofibers (N-CNF) cathode materials for structural ZIHSCs.To this end,a series of samples with different chemical compositions (N and O contents) are prepared to present deep insight into the electrochemical mechanism between N/O doping and Zn-ion storage.The as-prepared ZIHSC in the presence of N-CNF cathode and Zn Cl_(2) electrolyte offers a battery-level gravimetric energy density of 143.2 Wh kg^(-1)at a power density of 367.1 W kg^(-1).The free-standing N-CNF electrodes in ZIHSCs enjoy delivering an outstanding areal energy density of 110.4μWh cm^(-2)at 0.24 m W cm^(-2),excellent rate capability,and noticeable cycling stability over 10,000 cycles at 10 A g^(-1)with less than 7%decay.It was also concluded that active pyrrolic N dopants might deliver and facilitate more pseudocapacitance in ZIHSCs than other N configurations,resulting in higher adsorption/desorption and insertion/extraction process of Zn Cl^(+).Taking advantage of the beneficial properties of a free-standing continuous cathode,this novel generation of structural cathode material offers high areal and gravimetric energy densities and mechanical properties in a single zinc-ion-based package.展开更多
Benefiting from high flexibility and weavability,the wire-shaped supercapacitors(SCs)arouse tremendous interests for the applications in wearable/portable electronics.Graphene fiber(GF)is considered as a promising lin...Benefiting from high flexibility and weavability,the wire-shaped supercapacitors(SCs)arouse tremendous interests for the applications in wearable/portable electronics.Graphene fiber(GF)is considered as a promising linear electrode for wire-shaped SCs.However,the bottleneck is how to develop the GF-based linear electrode with facile fabrication process while wellmaintaining satisfactory electrochemical performance.Herein,a novel Fe_(3)O_(4)@GF composite linear electrode is proposed via a chemical reduction-induced assembly approach,in which the GO and Fe_(3)O_(4) nanoparticles(NPs)realize the efficient selfassembly owing to the electrostatic and van der Waals interactions,as well as the sufficient reduction of GO during the preparation process.The resultant fiber-shaped architecture shows boosted charge-transfer kinetics,high flexibility and structural integrity.Such Fe_(3)O_(4)@GF linear electrode exhibits excellent electrochemical behaviors including a large volumetric specific capacitance(~250.75 F cm^(−3)),remarkable rate capability and favorable electrochemical kinetics in aqueous electrolyte,superior than previously reported GF-based linear electrodes.For real application,a high-performance wire-shaped SC with excellent flexibility and weavability is fabricated based on such Fe_(3)O_(4)@GF linear electrode and gel electrolyte,demonstrating ultrahigh volumetric energy density(18.8 mWh cm^(−3)),power density(4000 mW cm^(−3))and strong durability(~93.5%retention after 10000 cycles).Prospectively,the fabricated wire-shaped SC can maintain reliable electrochemical behaviors in various deformation states,showing its potentials in future portable and wearable devices.展开更多
Electrode material based on a novel core–shell structure consisting of NiCoS(NCS) solid fiber core and Mn S(MS) sheet shell(NCS@MS) in situ grown on carbon cloth(CC) has been successfully prepared by a simple...Electrode material based on a novel core–shell structure consisting of NiCoS(NCS) solid fiber core and Mn S(MS) sheet shell(NCS@MS) in situ grown on carbon cloth(CC) has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor(ASC) is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly(vinyl alcohol)(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.展开更多
Supercapacitors based on carbon materials have advantages such as high power density,fast charging/discharging capability,and long lifetime stability,playing a vital role in the field of electrochemical energy storage...Supercapacitors based on carbon materials have advantages such as high power density,fast charging/discharging capability,and long lifetime stability,playing a vital role in the field of electrochemical energy storage technologies.To further expand the practical applications of carbon-based supercapacitors,their energy density,which is essentially determined by the specific capacitance and operating voltage,should be improved.This review provides fundamental knowledge on achieving high energy density of supercapacitors.We first address the relationship of the features of carbon materials,such as the surface area,pore size distribution,and surface functional groups,with their electrochemical performances,such as the gravimetric and volumetric capacitance,surface pseudocapacitance,and operating voltage.Then,we discuss the properties of electrolytes from nonaqueous and aqueous to hybrid one from the thermodynamic and kinetic aspects,and present their effects on capacitance and operating voltage.Finally,we illustrate different cell design strategies and their basic principles for increasing operating voltage.We also highlight the recent advances related to these fields and provide our insight into high-energy supercapacitors.展开更多
High discharged energy density and excellent flexible properties in dielectric materials are significantly sought to meet the rapid advancements in the electronics industry. In this study, covalent bonds are construct...High discharged energy density and excellent flexible properties in dielectric materials are significantly sought to meet the rapid advancements in the electronics industry. In this study, covalent bonds are constructed between poly(vinylidene fluoride-chlorotrifluoroethylene), which contains olefinic bonds, and thiol-modified BaTiO_(3) at the interface before the nanocomposite films are fabricated. The presence of the covalent bonds is proved to promote the dispersibility of the modified BaTiO_(3) and enhance the interfacial adhesion between the modified BaTiO_(3) and the polymer, followed by a remarkably positive effect in suppressing the dielectric loss(tanδ) and increasing the breakdown strength(Eb) of the nanocomposite films. In addition, the cross-linking treatment in the preparation process is found to be favourable for improving the mechanical properties of the nanocomposite films, which benefits the enhancement of Eb. Furthermore, at 400% elongation, the stretched nanocomposite film doped with 5 vol% modified BaTiO_(3) exhibits an Eb15.6% greater than that of the unstretched film, and the discharged energy density reaches 11.4 J/cm^(3) with a high discharge energy efficiency of 84.5%. This study provides a novel strategy for preparing flexible nanocomposites with powerful interfacial adhesion at high filler content to achieve high discharged energy density.展开更多
Redox-flow batteries(RFBs)are a promising energy storage technology with remarkable scalability and safety for storing vast amounts of renewable energy and mitigating outputfluctuations of renewable power grids.We demon...Redox-flow batteries(RFBs)are a promising energy storage technology with remarkable scalability and safety for storing vast amounts of renewable energy and mitigating outputfluctuations of renewable power grids.We demonstrate a neutral pH aqueous RFB using a custom-designed 1’,1’’’,1’’’’’-(benzene-1,3,5-triyltris(methylene))tris(1-(3-(trimethyl ammonio)propyl)-[4’’,4’’’-bipyridine]-1,1’-diium)nonachloride(BTTMPB)as a 3 e-storage anolyte.The custom design with the high polarization in charge density has led to the excellent water solubility of 4.0 M in H_(2)O(321.6 A h L^(-1))and 2.4 M in 2.0 M NaCl(192.9 A h L^(-1)).The density functional theory(DFT)calculations and electrochemical experiments have shown 3 e-storage response of BTTMPB with a diffusion coefficient of 3.1×10^(-6)cm^(2) s^(-1)and rate con-stant of 1.6×10^(-2)cm s^(-1) for thefirst reduction process.The synthesized anolyte was paired with(Ferrocenylmethyl)trimethylammonium chloride(FcNCl)as catholyte enabling a 0.92 V aqueous RFB with 125.9 W h L^(-1)theoretical energy density.The aqueous RFB has an excellent cycling performance from 10-30 m A cm^(-2),energy efficiency up to 80%,capacity retention of 99.96%per cycle at 20 m A cm^(-2),and a high demonstrated energy density of 29.1 W h L^(-1).展开更多
Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.Ho...Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.However,it remains a great challenge to understand the fundamental structure–performance relationship and achieve quantitative crystal structure design for efficient energy storage.In this review,we introduce the concept of crystal packing factor(PF),which can quantify crystal packing density.We then present and classify the typical crystal structures of attractive cathode/anode materials.Comparative PF analyses of different materials,including polymorphs,isomorphs,and others,are performed to clarify the influence of crystal packing density on energy storage performance through electronic and ionic conductivities.Notably,the practical electronic/ionic conductivities of energy storage materials are based on their intrinsic characteristics related to the PF yet are also affected by extrinsic factors.The PF provides a novel avenue for understanding the electrochemical performance of pristine materials and may offer guidance on designing better materials.Additional approaches involve size regulation,doping,carbon additives,and other methods.We also propose extended PF concepts to understand charge storage and transport behavior at different scales.Finally,we provide our insights on the major challenges and prospective solutions in this highly exciting field.展开更多
基金financial support provided by Projects(no.2020CDJXZ001)the Fundamental Research Funds for the Central Universities+1 种基金the Technology Innovation and Application Development Special Project of Chongqing(Z20211350 and Z20211351)Scientific Research Project of Chongqing Ecological Environment Bureau(no.CQEE2022-STHBZZ118)。
文摘The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金supported by the Swedish Foundation for Strategic Research(SSF)EM16-0004.
文摘MXene-based aqueous symmetric supercapacitors(SSCs)are attractive due to their good rate performances and green nature.However,it remains a challenge to reach voltages much over 1.2 V,which significantly diminishes their energy density.Herein,we report on Mo_(1.33)CTz MXene-based SSCs possessing high voltages in a 19.5 M LiCl electrolyte.Benefiting from the vacancy-rich structure and high stable potential window of Mo_(1.33)CTz,the obtained SSCs deliver a maximum energy density of>38.2 mWh cm^(-3) at a power density of 196.6 mW cm^(-3) under an operating voltage of 1.4 V,along with excellent rate performance and impressive cycling stability.This highly concentrated LiCl electrolyte is also applicable to Ti_(3)C_(2)Tz,the most widely studied MXene,achieving a maximum energy density of>41.3 mWh cm^(-3) at a power density of 165.2 mW cm^(-3) with an operating voltage of 1.8 V.The drop in energy density with increasing power in the Ti_(3)C_(2)Tz cells was steeper than for the Mo-based cells.This work provides a roadmap to develop superior SSCs with high voltages and high energy densities.
基金supported by the Energy Efficiency and Renewable Energy,Building Technologies Program,of the US Department of Energy,under contract no.DE-AC02-05CH11231the support on the DSC/TGA 3+supported by the Office of Science,Office of Basic Energy Sciences,of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231
文摘Thermal energy storage(TES)solutions offer opportunities to reduce energy consumption,greenhouse gas emissions,and cost.Specifically,they can help reduce the peak load and address the intermittency of renewable energy sources by time shifting the load,which are critical toward zero energy buildings.Thermochemical materials(TCMs)as a class of TES undergo a solid-gas reversible chemical reaction with water vapor to store and release energy with high storage capacities(600 kWh m^(-3))and negligible self-discharge that makes them uniquely suited as compact,stand-alone units for daily or seasonal storage.However,TCMs suffer from instabilities at the material(salt particles)and reactor level(packed beds of salt),resulting in poor multi-cycle efficiency and high-levelized cost of storage.In this study,a model is developed to predict the pulverization limit or Rcrit of various salt hydrates during thermal cycling.This is critical as it provides design rules to make mechanically stable TCM composites as well as enables the use of more energy-efficient manufacturing process(solid-state mixing)to make the composites.The model is experimentally validated on multiple TCM salt hydrates with different water content,and effect of Rcrit on hydration and dehydration kinetics is also investigated.
基金financial support from the National Natural Science Foundation of China(21878192 and 51904193)the Fundamental Research Funds for the Central Universities(YJ2021141)the Science and Technology Cooperation Special Fund of Sichuan University and Zigong City(2021CDZG-14)
文摘Efficient energy storage devices with suitable electrode materials,that integrate high power and high energy,are the crucial requisites of the renewable power source,which have unwrapped new possibilities in the sustainable development of energy and the environment.Herein,a facile collagen microstructure modulation strategy is proposed to construct a nitrogen/oxygen dual-doped hierarchically porous carbon fiber with ultrahigh specific surface area(2788 m^(2)g^(-1))and large pore volume(4.56 cm^(3)g^(-1))via local microfibrous breakage/disassembly of natural structured proteins.Combining operando spectroscopy and density functional theory unveil that the dual-heteroatom doping could effectively regulate the electronic structure of carbon atom framework with enhanced electric conductivity and electronegativity as well as decreased diffusion resistance in favor of rapid pseudocapacitive-dominated Li^(+)-storage(353 mAh g^(-1)at 10 A g^(-1)).Theoretical calculations reveal that the tailored micro-/mesoporous structures favor the rapid charge transfer and ion storage,synergistically realizing high capacity and superior rate performance for NPCF-H cathode(75.0 mAh g^(-1)at 30 A g^(-1)).The assembled device with NPCF-H as both anode and cathode achieves extremely high energy density(200 Wh kg^(-1))with maximum power density(42600 W kg^(-1))and ultralong lifespan(80%capacity retention over 10000 cycles).
基金financially supported by the National Key R&D Program of China(2022YFE0101300)the National Natural Science Foundation of China(52176203 and 52050027)the China Education Association for International Exchange(202006)。
文摘Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising due to its intrinsic high hydrogen capacity.Hydrolysis reaction of LSHS materials occurs at moderate conditions,indicating the potential for portable applications.At present,most of review work focuses on the improvement of material performance,especially the catalysts design.This part is important,but the others,such as operation modes,are also vital to to make full use of material potential in the practical applications.Different operation modes of hydrolysis reaction have an impact on hydrogen capacity to various degrees.For example,hydrolysis in solution would decrease the hydrogen capacity of hydrogen generator to a low value due to the excessive water participating in the reaction.Therefore,application-oriented operation modes could become a key problem for hydrolysis reaction of LSHS materials.In this paper,the operation modes of hydrolysis reaction and their practical applications are mainly reviewed.The implements of each operation mode are discussed and compared in detail to determine the suitable one for practical applications with the requirement of high energy density.The current challenges and future directions are also discussed.
基金Baohua Jia and Han Lin acknowledges the Australia Research Council through the Discovery Project Scheme(DP190103186,DP220100603,FT210100806)the Industrial Transformation Training Centre Scheme(Grant No.IC180100005)The authors wish to express gratitude to the Swinburne Melbourne and Swinburne Sarawak for funding this project under the‘Melbourne-Sarawak Research Collaboration Scheme’(MSRSC)grant.
文摘Although room temperature ionic liquids(ILs)have emerged as potential next-generation electrolytes for their wide electrochemical stability window(ESW),the trade-off between this window and viscosity has hindered their widespread use in energy storage devices.Here,we present for the first time that such a trade-off can be balanced by mixing two ILs with the common anion([NTf_(2)]^(-))but different cations([EMIM]^(+) and[N1114]^(+))together.The[EMIM]cation-based IL possesses low viscosity while the[N1114]cation-based IL exhibits wide ESW.Since the concentrations of each IL in the mixtures can result in different electrolyte properties,we demonstrate a systematic approach by exploring the properties of various concentration combinations.In addition,the corresponding cell voltage of their resulting graphene supercapacitors(SCs)accompanied based on the interaction between the binary ionic liquid and the electrodes,and the associated electrochemical performance were studied to determine the optimum electrolyte system for the highest SC energy density.The well-balanced viscosity/ESW trade-off is achieved in binary IL consisting 50 vol%[EMIM][NTf_(2)]and 50 vol%[N1114][NTf_(2)]as evident from the extraordinary electrode specific capacitance of 293.1 F g^(-1) and the ultrahigh SC energy density of 177 Wh kg^(-1),which approaches that of a lithium-ion battery.
基金the National Natural Science Foundation of China(Grant Nos.12174352 and 12111530103)the Fundamental Research Funds for the Central UniversitiesChina University of Geosciences(Wuhan)(Grant No.G1323523065)。
文摘Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform an extensive structure search of ternary carbon-nitrogen-oxygen(CNO)compound under high pressure with the CALYPSO method and first principles calculations,and successfully identify three polymeric CNO compounds with Pbam,C2/m and I4m2symmetries under 100 GPa.More interestingly,these structures are also dynamically stable at ambient pressure,and are potential high energy density materials(HEDMs).The energy densities of Pbam,C2/m and I4m2 phases of CNO are about2.30 kJ/g,1.37 kJ/g and 2.70 kJ/g,respectively,with the decompositions of graphitic carbon and molecular carbon dioxide andα-N(molecular N_(2))at ambient pressure.The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures,which offer crucial insights for designs and syntheses of novel HEDMs.
基金This work is supported by the National Key R&D Program of China(2021YFB2400400).
文摘The limited energy density of lithium-ion capacitors poses a significant obstacle to their widespread application,primarily stemming from the inability of the electrodes to simultaneously fulfill both high energy density and rapid charging requirements.Experimental data demonstrate that a directional particle configuration can enhance charging speed while maintaining high-capacity density,but it is rarely discussed.Here,we have developed a particle-level electrochemical model capable of reconstructing an electrode with a directional particle configuration.By employing this method,an investigation was conducted to explore how the spatial morphology characteristics of particle configuration impact the energy storage characteristics of electrodes.Results demonstrate that rational particle configuration can effectively enhance the transport of lithium ions and create additional space for lithium-ion storage.With the same particle size distribution,the best electrode can increase the discharge capacity by up to132.4% and increase the charging SOC by 11.3% compared to the ordinary electrode under the condition of 6 C.These findings provide a further understanding of the energy storage mechanism inside the anisotropic particle distribution electrode,which is important for developing high-performance lithium-ion capacitors.
基金supported by the Scientific and Technological Research Council of Turkey(TüBTAK)under Grant 112T570
文摘Preparation of hierarchically porous, heteroatom-rich nanostructured carbons through green and scalable routes plays a key role for practical energy storage applications. In this work, naturally abundant lignocellulosic agricultural waste with high initial oxygen content, hazelnut shells, were hydrothermally carbonized and converted into nanostructured ‘hydrochar’. Environmentally benign ceramic/magnesium oxide(Mg O) templating was used to introduce porosity into the hydrochar. Electrochemical performance of the resulting material(HM700) was investigated in aqueous solutions of 1 M H;SO;, 6 M KOH and1 M Na;SO;, using a three-electrode cell. HM700 achieved a high specific capacitance of 323.2 F/g in 1 M H;SO;(at 1 A/g,-0.3 to 0.9 V vs. Ag/Ag Cl) due to the contributions of oxygen heteroatoms(13.5 wt%)to the total capacitance by pseudo-capacitive effect. Moreover, a maximum energy density of 11.1 Wh/kg and a maximum power density of 3686.2 W/kg were attained for the symmetric supercapacitor employing HM700 as electrode material(1 M Na;SO;, E = 2 V), making the device promising for green supercapacitor applications.
基金supported by the National Natural Science Foundation of China(51702225)the Natural Science Foundation of Jiangsu Province(BK20170336)。
文摘Designing high-performance electrodes via 3D printing for advanced energy storage is appealing but remains challenging.In normal cases,light-weight carbonaceous materials harnessing excellent electrical conductivity have served as electrode candidates.However,they struggle with undermined areal and volumetric energy density of supercapacitor devices,thereby greatly impeding the practical applications.Herein,we demonstrate the in situ coupling of NiCoP bimetallic phosphide and Ti3C2 MXene to build up heavy NCPM electrodes affording tunable mass loading throughout 3D printing technology.The resolution of prints reaches 50μm and the thickness of device electrodes is ca.4 mm.Thus-printed electrode possessing robust open framework synergizes favorable capacitance of NiCoP and excellent conductivity of MXene,readily achieving a high areal and volumetric capacitance of 20 F cm^-2 and 137 F cm^-3 even at a high mass loading of^46.3 mg cm^-2.Accordingly,an asymmetric supercapacitor full cell assembled with 3D-printed NCPM as a positive electrode and 3D-printed activated carbon as a negative electrode harvests remarkable areal and volumetric energy density of 0.89 mWh cm^-2 and 2.2 mWh cm^-3,outperforming the most of state-of-the-art carbon-based supercapacitors.The present work is anticipated to offer a viable solution toward the customized construction of multifunctional architectures via 3D printing for high-energy-density energy storage systems.
文摘Paraffin/γ-Al2O3 composites as phase change energy storage materials were prepared by absorbing paraffin in porous network of γ-Al2O3.In the composite materials,paraffin was used as a phase change material(PCM)for thermal energy storage,and γ-Al2O3 acted as supporting materials.Characterizations were conducted to evaluate the energy storage performance of the composites,and differential scanning calorimeter results showed that the PCM-3 composite has melting latent heat of 112.9 kJ/kg with a melting temperature of 62.9 ℃.Due to strong capillary force and surface tension between paraffin and γ-Al2O3,the leakage of melted paraffin from the composites can be effectively prevented.Therefore,the paraffin/γ-Al2O3 composites have a good thermal stability and can be used repeatedly.
基金financially supported by the National Key Research and Development Program of China(2022YFB4002103)the National Natural Science Foundation of China(22279107)。
文摘Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of LIBs.Herein,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the CNTs.More importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.
文摘Zinc ion hybrid supercapacitor (ZIHSC) with promising energy and power densities is an excellent answer to the ever-growing demand for energy storage devices.The restricted lifespan due to the dendrite formation on metallic zinc (Zn) is one of the main roadblocks.Herein,we investigate the electrochemical capability of oxygen-enriched porous carbon nanofibers (A-CNF) and nitrogen,oxygen-enriched porous carbon nanofibers (N-CNF) cathode materials for structural ZIHSCs.To this end,a series of samples with different chemical compositions (N and O contents) are prepared to present deep insight into the electrochemical mechanism between N/O doping and Zn-ion storage.The as-prepared ZIHSC in the presence of N-CNF cathode and Zn Cl_(2) electrolyte offers a battery-level gravimetric energy density of 143.2 Wh kg^(-1)at a power density of 367.1 W kg^(-1).The free-standing N-CNF electrodes in ZIHSCs enjoy delivering an outstanding areal energy density of 110.4μWh cm^(-2)at 0.24 m W cm^(-2),excellent rate capability,and noticeable cycling stability over 10,000 cycles at 10 A g^(-1)with less than 7%decay.It was also concluded that active pyrrolic N dopants might deliver and facilitate more pseudocapacitance in ZIHSCs than other N configurations,resulting in higher adsorption/desorption and insertion/extraction process of Zn Cl^(+).Taking advantage of the beneficial properties of a free-standing continuous cathode,this novel generation of structural cathode material offers high areal and gravimetric energy densities and mechanical properties in a single zinc-ion-based package.
基金supported by the National Natural Science Foundation of China(Grant Nos.61904116,52002157)the Natural Science Foundation of Jiangsu Province(Grant No.BK20190976)the Science and Technology Project of State Grid Corporation of China(Grant No.5455DW190009).
文摘Benefiting from high flexibility and weavability,the wire-shaped supercapacitors(SCs)arouse tremendous interests for the applications in wearable/portable electronics.Graphene fiber(GF)is considered as a promising linear electrode for wire-shaped SCs.However,the bottleneck is how to develop the GF-based linear electrode with facile fabrication process while wellmaintaining satisfactory electrochemical performance.Herein,a novel Fe_(3)O_(4)@GF composite linear electrode is proposed via a chemical reduction-induced assembly approach,in which the GO and Fe_(3)O_(4) nanoparticles(NPs)realize the efficient selfassembly owing to the electrostatic and van der Waals interactions,as well as the sufficient reduction of GO during the preparation process.The resultant fiber-shaped architecture shows boosted charge-transfer kinetics,high flexibility and structural integrity.Such Fe_(3)O_(4)@GF linear electrode exhibits excellent electrochemical behaviors including a large volumetric specific capacitance(~250.75 F cm^(−3)),remarkable rate capability and favorable electrochemical kinetics in aqueous electrolyte,superior than previously reported GF-based linear electrodes.For real application,a high-performance wire-shaped SC with excellent flexibility and weavability is fabricated based on such Fe_(3)O_(4)@GF linear electrode and gel electrolyte,demonstrating ultrahigh volumetric energy density(18.8 mWh cm^(−3)),power density(4000 mW cm^(−3))and strong durability(~93.5%retention after 10000 cycles).Prospectively,the fabricated wire-shaped SC can maintain reliable electrochemical behaviors in various deformation states,showing its potentials in future portable and wearable devices.
基金supported by the Grant-in-Aid for Scientific Research (KAKENHI) program, Japan (C, Grant Number 15K05597)Takahashi Industrial and Economic Research Foundation (Takahashi Grant Number 06-003-154)
文摘Electrode material based on a novel core–shell structure consisting of NiCoS(NCS) solid fiber core and Mn S(MS) sheet shell(NCS@MS) in situ grown on carbon cloth(CC) has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor(ASC) is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly(vinyl alcohol)(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(NRF-2020R1A3B2079803)
文摘Supercapacitors based on carbon materials have advantages such as high power density,fast charging/discharging capability,and long lifetime stability,playing a vital role in the field of electrochemical energy storage technologies.To further expand the practical applications of carbon-based supercapacitors,their energy density,which is essentially determined by the specific capacitance and operating voltage,should be improved.This review provides fundamental knowledge on achieving high energy density of supercapacitors.We first address the relationship of the features of carbon materials,such as the surface area,pore size distribution,and surface functional groups,with their electrochemical performances,such as the gravimetric and volumetric capacitance,surface pseudocapacitance,and operating voltage.Then,we discuss the properties of electrolytes from nonaqueous and aqueous to hybrid one from the thermodynamic and kinetic aspects,and present their effects on capacitance and operating voltage.Finally,we illustrate different cell design strategies and their basic principles for increasing operating voltage.We also highlight the recent advances related to these fields and provide our insight into high-energy supercapacitors.
基金supported by the Major Science and Technology Innovation Project of Shandong Province of China(2019JZZY020231 and 2019JZZY020232)。
文摘High discharged energy density and excellent flexible properties in dielectric materials are significantly sought to meet the rapid advancements in the electronics industry. In this study, covalent bonds are constructed between poly(vinylidene fluoride-chlorotrifluoroethylene), which contains olefinic bonds, and thiol-modified BaTiO_(3) at the interface before the nanocomposite films are fabricated. The presence of the covalent bonds is proved to promote the dispersibility of the modified BaTiO_(3) and enhance the interfacial adhesion between the modified BaTiO_(3) and the polymer, followed by a remarkably positive effect in suppressing the dielectric loss(tanδ) and increasing the breakdown strength(Eb) of the nanocomposite films. In addition, the cross-linking treatment in the preparation process is found to be favourable for improving the mechanical properties of the nanocomposite films, which benefits the enhancement of Eb. Furthermore, at 400% elongation, the stretched nanocomposite film doped with 5 vol% modified BaTiO_(3) exhibits an Eb15.6% greater than that of the unstretched film, and the discharged energy density reaches 11.4 J/cm^(3) with a high discharge energy efficiency of 84.5%. This study provides a novel strategy for preparing flexible nanocomposites with powerful interfacial adhesion at high filler content to achieve high discharged energy density.
基金the Department of Science and Technology(DST),Ministry of Science and Technology,Government of India,for sponsoring this study under project no.DST/TMD/MES/2k18/02CSIR,Gov.of India,for the Senior Research Fellowship。
文摘Redox-flow batteries(RFBs)are a promising energy storage technology with remarkable scalability and safety for storing vast amounts of renewable energy and mitigating outputfluctuations of renewable power grids.We demonstrate a neutral pH aqueous RFB using a custom-designed 1’,1’’’,1’’’’’-(benzene-1,3,5-triyltris(methylene))tris(1-(3-(trimethyl ammonio)propyl)-[4’’,4’’’-bipyridine]-1,1’-diium)nonachloride(BTTMPB)as a 3 e-storage anolyte.The custom design with the high polarization in charge density has led to the excellent water solubility of 4.0 M in H_(2)O(321.6 A h L^(-1))and 2.4 M in 2.0 M NaCl(192.9 A h L^(-1)).The density functional theory(DFT)calculations and electrochemical experiments have shown 3 e-storage response of BTTMPB with a diffusion coefficient of 3.1×10^(-6)cm^(2) s^(-1)and rate con-stant of 1.6×10^(-2)cm s^(-1) for thefirst reduction process.The synthesized anolyte was paired with(Ferrocenylmethyl)trimethylammonium chloride(FcNCl)as catholyte enabling a 0.92 V aqueous RFB with 125.9 W h L^(-1)theoretical energy density.The aqueous RFB has an excellent cycling performance from 10-30 m A cm^(-2),energy efficiency up to 80%,capacity retention of 99.96%per cycle at 20 m A cm^(-2),and a high demonstrated energy density of 29.1 W h L^(-1).
基金supported by the National Natural Science Foundation of China(52202327)Science and Technology Commission of Shanghai Municipality(22ZR1471300)the Key Research Program of Frontier Science,Chinese Academy of Sciences(Grant No.QYZDJ-SSW-JSC013 and KGZD-EW-T06).
文摘Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material design.To date,hundreds of electrode materials have been developed to pursue superior performance.However,it remains a great challenge to understand the fundamental structure–performance relationship and achieve quantitative crystal structure design for efficient energy storage.In this review,we introduce the concept of crystal packing factor(PF),which can quantify crystal packing density.We then present and classify the typical crystal structures of attractive cathode/anode materials.Comparative PF analyses of different materials,including polymorphs,isomorphs,and others,are performed to clarify the influence of crystal packing density on energy storage performance through electronic and ionic conductivities.Notably,the practical electronic/ionic conductivities of energy storage materials are based on their intrinsic characteristics related to the PF yet are also affected by extrinsic factors.The PF provides a novel avenue for understanding the electrochemical performance of pristine materials and may offer guidance on designing better materials.Additional approaches involve size regulation,doping,carbon additives,and other methods.We also propose extended PF concepts to understand charge storage and transport behavior at different scales.Finally,we provide our insights on the major challenges and prospective solutions in this highly exciting field.