Orthorhombic molybdenum trioxide(α-MoO_(3)) electrode material experiences severe capacity fading and poor cycling stability in aqueous electrolytes.We investigated the charge-storage performance of α-MoO_(3) electr...Orthorhombic molybdenum trioxide(α-MoO_(3)) electrode material experiences severe capacity fading and poor cycling stability in aqueous electrolytes.We investigated the charge-storage performance of α-MoO_(3) electrode in aluminium trifluoromethanesulfonate(Al(OTf)_(3))-based salt-in-water electrolyte(SiWE) and water-in-salt electrolyte(WiSE).It was found that α-MoO_(3) electrode exhibits significantly different cycling stabilities in both electrolytes with capacity retentions of 8% using the former and87% using the latter.This is because α-MoO_(3) electrode maintains its crystal structure upon cycling in WiSE,but experiences substantial structural collapses and partial dissolution upon cycling in SiWE.This behaviour was inferred from both operando electrogravimetry and ex situ analyses.Research results suggest that the predominant charge-storage mechanism in a-MoO_(3) electrode using WiSE is the intercalation of protons produced from electrolyte hydrolysis with some contribution from surface pseudocapacitance enabled by Al3+ions.A two-volt full cell fabricated from α-MoO_(3) electrode as anode and copper hexacyanoferrate(CuHCF) electrode as cathode using WiSE delivers volumetric and gravimetric energies of 10.4 Wh/L and 26.5 Wh/kg,respectively,with 78% capacity retention after 2500 cycles.This study provides an insightful understanding of the electrochemical performance of α-MoO_(3) electrode in Al(OTf)_(3)-based electrolytes.展开更多
Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt&qu...Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt"(WiS) electrolytes has received significant interest for the development of advanced high performance ESDs.The WiS electrolyte exhibits wide electrochemical stability window(ESW),highsafety,non-flammability and superior electrochemical performance compared to the conventional "salt-in-water" electrolytes.This review aims to provide a comprehensive discussion on WiS electrolyte based on theoretical,electrochemical and physicochemical characteristics.A strategic way for the usage of WiS electrolyte in rechargeable metal-ion batteries and supercapacitors with potentially improved electrochemical performance has been reviewed systematically.This review also discussed the unique advantages of WiS electrolytes as well as the future scope and challenges.展开更多
Low-cost,flexible and safe battery technology is the key to the widespread usage of wearable electronics,among which the aqueous Al ion battery with water-in-salt electrolyte is a promising candidate.In this work,a fl...Low-cost,flexible and safe battery technology is the key to the widespread usage of wearable electronics,among which the aqueous Al ion battery with water-in-salt electrolyte is a promising candidate.In this work,a flexible aqueous Al ion battery is developed using cellulose paper as substrate.The water-in-salt electrolyte is stored inside the paper,while the electrodes are either printed or attached on the paper surface,leading to a lightweight and thin-film battery prototype.Currently,this battery can tolerate a charge and discharge rate as high as 4 A g^(-1) without losing its storage capacity.The charge voltage is around 2.2 V,while the discharge plateau of 1.6–1.8 V is among the highest in reported aqueous Al ion batteries,together with a high discharge specific capacity of~140 mAh g^(-1).However,due to the water electrolysis side reaction,the faradaic efficiency can only reach 85%with a cycle life of 250 due to the dry out of electrolyte.Benefited from using flexible materials and aqueous electrolyte,this paper-based Al ion battery can tolerate various deformations such as bending,rolling and even puncturing without losing its performance.When two single cells are connected in series,the battery pack can provide a charge voltage of 4.3 V and a discharge plateau as high as 3–3.6 V,which are very close to commercial Li ion batteries.Such a cheap,flexible and safe battery technology may be widely applied in low-cost and large-quantity applications,such as RFID tags,smart packages and wearable biosensors in the future.展开更多
While transition-metal oxides such as α-MoO_(3)provide high capacity,their use is limited by modest electronic conductivity and electrochemical instability in aqueous electrolytes.Two-dimensional(2D)MXenes,offer meta...While transition-metal oxides such as α-MoO_(3)provide high capacity,their use is limited by modest electronic conductivity and electrochemical instability in aqueous electrolytes.Two-dimensional(2D)MXenes,offer metallic conductivity,but their capacitance is limited in aqueous electrolytes.Insertion of partially solvated cations into Ti_(3)C_(2)MXene from lithium-based water-in-salt(WIS)electrolytes enables charge storage at positive potentials,allowing a wider potential window and higher capacitance.Herein,we demonstrate that α-MoO_(3)/Ti_(3)C_(2)hybrids combine the high capacity of α-MoO_(3)and conductivity of Ti_(3)C_(2)in WIS(19.8 m LiCI)electrolyte in a wide1.8 V voltage window.Cyclic voltammograms reveal multiple redox peaks from α-MoO_(3)in addition to the well-separated peaks of Ti_(3)C_(2)in the hybrid electrode.This leads to a higher specific charge and a higher rate capability compared to a carbon and binder containing α-MoO_(3)electrode.These results demonstrate that the addition of MXene to less conductive oxides eliminates the need for conductive carbon additives and binders,leads to a larger amount of charge stored,and increases redox capacity at higher rates.In addition,MXene encapsulated α-MoO_(3)showed improved electrochemical stability,which was attributed to the suppressed dissolution of α-MoO_(3).The work suggests that oxide/MXene hybrids are promising for energy storage.展开更多
Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, ...Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, such as higher freezing point depression(FPD) and robustness. Besides the traditional organic-and aqueous-based(salt-in-water) electrolytes used in SCs, water-in-salt(WISE) sodium perchlorate electrolytes offer high FPD, non-flammability, and low-toxicity conditions, allowing the fabrication of safer, environmentally friendly, and more robust devices. For the first time, this work reports a comprehensive study regarding WISE system’s charge-storage capabilities and physicochemical properties under low-temperature conditions(T < 0 ℃) using mesoporous carbon-based electrodes. The effect of temperature reduction on the electrolyte viscosity and electrical properties was investigated using different techniques and the in-situ(or operando) Raman spectroscopy under dynamic polarization conditions.The cell voltage, equivalent series resistance, and specific capacitance were investigated as a function of the temperature. The cell voltage(U) increased ~ 50%, while the specific capacitance decreased ~20%when the temperature was reduced from 25 ℃ to -10 ℃. As a result, the maximum specific energy(E = CU^(2)/2) increased ~ 100%. Therefore, low-temperature WISEs are promising candidates to improve the energy-storage characteristics in SCs.展开更多
Pore size and distribution in carbon-based materials are regarded to be a key factor to affect the electrochemical capacitive performances of the resultant electrodes.In this study,nitrogen and oxygen codoped porous c...Pore size and distribution in carbon-based materials are regarded to be a key factor to affect the electrochemical capacitive performances of the resultant electrodes.In this study,nitrogen and oxygen codoped porous carbons(NOPCs) are fabricated based on a simple Schiff-base reaction between m-phenylenediamine and terephthalaldehyde.The NOPCs have tunable morphologies,high surface areas,abundant heteroatom doping.More importantly,the carbons show a dominant micropores of 0.5-0.8 nm,comparable to the ionic sizes of LiTFSI(Li^+0.069 nm;TFSI-0.79 nm) water-in-salt electrolyte with a high potential window of 2.2 V.Consequently,the fabricated symmetric supercapacitor gives a high energy output of 30.5 Wh/kg at 1 kW/kg,and high stability after successive 10,000 cycles with ^96.8% retention.This study provides promising potential to develop high-energy supercapacitors.展开更多
A facile fabrication strategy is reported to obtain N/O codoped porous carbon nanosheets for pur-pose of ameliorating the charge transfer and accumulation in the concentrated LiTFSI(lithium bis(trifluoromethane sulfon...A facile fabrication strategy is reported to obtain N/O codoped porous carbon nanosheets for pur-pose of ameliorating the charge transfer and accumulation in the concentrated LiTFSI(lithium bis(trifluoromethane sulfonyl)imide)electrolyte.By tunning the feed ratio of comonomers,the porous nanosheet structure is endowed with a significant ion-adsorption surface area(1630 m^(2)/g)and intercon-nected hierarchical porosity;meanwhile,high-level N/O dopants(N:3.58 at%,O:12.91 at%)increase the effective contact area for electrolyte ions,and further facilitate rapid ion/electron transfer.Benefiting from the advantageous features,carbon nanosheets electrode reveal an enhanced specific capacitance(375 F/g)in three-electrode configuration and the H_(2)SO_(4)-based device yields a high gravimetric energy density of 11.4 Wh/kg.Particularly,the ion-diffusion highways in porous carbon nanosheets contribute to the 2.25 V LiTFSI-based symmetric device with a high energy delivery up to 33.1 Wh/kg.This work offers an in-spiring strategy for facile fabrication of carbon nanosheets,and demonstrates their promising application in“water-in-salt”electrolyte-based supercapacitor systems.展开更多
Aqueous hybrid supercapacitors are attracting increasing attention due to their potential low cost,high safety and eco-friendliness.However,the narrow operating potential window of aqueous electrolyte and the lack of ...Aqueous hybrid supercapacitors are attracting increasing attention due to their potential low cost,high safety and eco-friendliness.However,the narrow operating potential window of aqueous electrolyte and the lack of suitable negative electrode materials seriously hinder its future applications.Here,we explore high concentrated lithium acetate with high ionic conductivity of 65.5 mS cm−1 as a green“water-in-salt”electrolyte,providing wide voltage window up to 2.8 V.It facilitates the reversible function of niobium tungsten oxide,Nb18W16O93,that otherwise only operations in organic electrolytes previously.The Nb18W16O93 with lithium-ion intercalation pseudocapacitive behavior exhibits excellent rate performance,high areal capacity,and ultra-long cycling stability.An aqueous lithium-ion hybrid capacitor is developed by using Nb18W16O93 as negative electrode combined with graphene as positive electrode in lithium acetate-based“water-in-salt”electrolyte,delivering a high energy density of 41.9 W kg−1,high power density of 20,000 W kg−1 and unexceptionable stability of 50,000 cycles.展开更多
A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyt...A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert.The electrolyte comprises primarily ZnCl_(2) and LiCl as an additive,both of which are inexpensive salts.The O-H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn-Cl superhalides,as suggested by integrated characterization and simulation.As a result,the average Coulombic efficiency of zincmetal anode is raised to an unprecedented>99.7%at 1mA cm^(−2).In the new electrolyte,the plating/stripping processes leave the zinc-metal anode dendrite-free,and the zinc-metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm^(−2) at 2mA cm^(−2).Furthermore,the high Coulombic efficiency of zinc-metal anode in the ZnCl_(2)-LiCl mixture electrolyte is demonstrated in full cells with a limited anode.The V_(2)O_(5)·H_(2)O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles,and the LiMn_(2)O_(4)||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.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
Aqueous rechargeable batteries have attracted enormous attention owning to their intrinsic characteristics of non-flammability, low cost, and the superior ionic conductivity of the aqueous electrolyte.However, the nar...Aqueous rechargeable batteries have attracted enormous attention owning to their intrinsic characteristics of non-flammability, low cost, and the superior ionic conductivity of the aqueous electrolyte.However, the narrow electrochemical stability window(1.23 V), imposed by hydrogen and oxygen evolution, constrains the overall energy density of batteries. The revolutionary "water-in-salt” electrolytes considerably expand the electrochemical stability window to 3 or even 4 volts, giving rise to a new series of high-voltage aqueous metal-ion chemistries. Herein, the recent advances in "water-in-salt” electrolytes for aqueous monovalent-ion(Li^(+), Na^(+), K^(+)) rechargeable batteries have been systematically reviewed. Meanwhile, the corresponding reaction mechanisms, electrochemical performances and the existing challenges and opportunities are also highlighted.展开更多
Ammonium-ion batteries are promising solutions for large-scale energy storage systems owing to their costeffectiveness,safety,and sustainability.Herein,we propose an aqueous ammonium-ion battery based on an organic po...Ammonium-ion batteries are promising solutions for large-scale energy storage systems owing to their costeffectiveness,safety,and sustainability.Herein,we propose an aqueous ammonium-ion battery based on an organic poly(1,5-naphthalenediamine)anode and an inorganic Prussian blue cathode in 19 M(M:mol kg^(-1))CH3COONH_(4)electrolyte.Its operation involves a reversible coordination reaction(C=N/C-N-conversion)in the anode and the NH_(4)^(+)insertion/extraction reaction in the cathode,along with NH_(4)^(+)acting as the charge carrier in a rocking-chair battery.Benefiting from the fast kinetics and stability of both electrodes,this aqueous ammoniumion battery shows an excellent rate capability and long cycle stability for 500 cycles.Moreover,an energy density as high as 31.8 Wh kg^(-1) can be achieved,based on the total mass of the cathode and anode.Surprisingly,this aqueous ammonium-ion battery works well over a wide temperature range from-40 to 80℃.This work will provide new opportunities to build wide-temperature aqueous batteries and broaden the horizons for large-scale energy storage systems.展开更多
The bio-nanotechnological fabrication of high-surface-area carbons has attracted widespread interest in supercapacitor applications by using readily-available natural products as raw materials or bio-templates,and is ...The bio-nanotechnological fabrication of high-surface-area carbons has attracted widespread interest in supercapacitor applications by using readily-available natural products as raw materials or bio-templates,and is expected to refine on pore accessibility for compact energy storage. Here, a renovated design strategy of semi-biomass interpenetrating polymer network(IPN) derived carbon is demonstrated through physically knitting the biomacromolecule(sodium alginate, SA) polymeric chains into the highly crosslinked resorcinol-formaldehyde(RF) network and subsequent thermochemical conversion. Moleculelevel interlacing forces in such IPN efficiently relieve the RF skeleton shrinkage when producing carbon,while the other SA network addresses the macrophase separation issue to sacrifice as an in-knitted porogen and a morphology-directing agent. As a result, porous carbon globules are equipped with moss-like surfaces and interconnected pore architecture for high accessible electrode surface(1013 m^(2)/g), and efficient electrochemical responses are reached with the specific capacitance of 312 F/g at 1 A/g. Taking the advantage of 9 mol/kg NaClO_(4) complex-solvent electrolyte, the voltage window is extended to 2.4 V,endowing the two-electrode device with the high energy delivery of 32.3 Wh/kg at 240 W/kg.展开更多
Hydrous electrolytes with high electrochemical potentials were obtained by hydrating water molecules into solutes to form high Li:water molar ratio electrolytes(HMRE).Solid polyethylene glycol(PEG) were e mployed to e...Hydrous electrolytes with high electrochemical potentials were obtained by hydrating water molecules into solutes to form high Li:water molar ratio electrolytes(HMRE).Solid polyethylene glycol(PEG) were e mployed to enha nce the molar ratio of Li^(+) to water in the electrolytes while reducing the consumption of Li-salt.The obtained mole ratio of Li^(+) to wa ter molecules in the hydrous electrolytes was greater than 1:1;however,the mass fraction of Li-salt was reduced to 61%(approximately 5.5 mol/kg,based on water and PEG).Compared with that of water-in-salt electrolytes,the mass fraction of Li-salt could be remarkably reduced by adding solid PEG.The electrochemical stability of the electrolytes improved considerably because of the strong hydration of Li^(+) by the water molecules.A beneficial passivation effect,arising from the decomposition of the electrolyte,at a wide potential window was observed.展开更多
基金supported by the Australian Research Council under the ARC Laureate Fellowship program(FL170100101)。
文摘Orthorhombic molybdenum trioxide(α-MoO_(3)) electrode material experiences severe capacity fading and poor cycling stability in aqueous electrolytes.We investigated the charge-storage performance of α-MoO_(3) electrode in aluminium trifluoromethanesulfonate(Al(OTf)_(3))-based salt-in-water electrolyte(SiWE) and water-in-salt electrolyte(WiSE).It was found that α-MoO_(3) electrode exhibits significantly different cycling stabilities in both electrolytes with capacity retentions of 8% using the former and87% using the latter.This is because α-MoO_(3) electrode maintains its crystal structure upon cycling in WiSE,but experiences substantial structural collapses and partial dissolution upon cycling in SiWE.This behaviour was inferred from both operando electrogravimetry and ex situ analyses.Research results suggest that the predominant charge-storage mechanism in a-MoO_(3) electrode using WiSE is the intercalation of protons produced from electrolyte hydrolysis with some contribution from surface pseudocapacitance enabled by Al3+ions.A two-volt full cell fabricated from α-MoO_(3) electrode as anode and copper hexacyanoferrate(CuHCF) electrode as cathode using WiSE delivers volumetric and gravimetric energies of 10.4 Wh/L and 26.5 Wh/kg,respectively,with 78% capacity retention after 2500 cycles.This study provides an insightful understanding of the electrochemical performance of α-MoO_(3) electrode in Al(OTf)_(3)-based electrolytes.
基金the Council of Scientific & Industrial Research(CSIR) for the financial support through the HCP-44/02/1 projectthe DST-INSPIRE Faculty Scheme,Department of Science and Technology,New Delhi,Govt.of India(IFA20-MS-168) for the financial supports。
文摘Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt"(WiS) electrolytes has received significant interest for the development of advanced high performance ESDs.The WiS electrolyte exhibits wide electrochemical stability window(ESW),highsafety,non-flammability and superior electrochemical performance compared to the conventional "salt-in-water" electrolytes.This review aims to provide a comprehensive discussion on WiS electrolyte based on theoretical,electrochemical and physicochemical characteristics.A strategic way for the usage of WiS electrolyte in rechargeable metal-ion batteries and supercapacitors with potentially improved electrochemical performance has been reviewed systematically.This review also discussed the unique advantages of WiS electrolytes as well as the future scope and challenges.
基金The authors would like to acknowledge the CRF grant of the Hong Kong Research Grant Council(C5031-20G)the CRCG grant of the University of Hong Kong(201910160008)the research start-up fund of Harbin Institute of Technology,Shenzhen(CA45001039)for providing funding support to this project.
文摘Low-cost,flexible and safe battery technology is the key to the widespread usage of wearable electronics,among which the aqueous Al ion battery with water-in-salt electrolyte is a promising candidate.In this work,a flexible aqueous Al ion battery is developed using cellulose paper as substrate.The water-in-salt electrolyte is stored inside the paper,while the electrodes are either printed or attached on the paper surface,leading to a lightweight and thin-film battery prototype.Currently,this battery can tolerate a charge and discharge rate as high as 4 A g^(-1) without losing its storage capacity.The charge voltage is around 2.2 V,while the discharge plateau of 1.6–1.8 V is among the highest in reported aqueous Al ion batteries,together with a high discharge specific capacity of~140 mAh g^(-1).However,due to the water electrolysis side reaction,the faradaic efficiency can only reach 85%with a cycle life of 250 due to the dry out of electrolyte.Benefited from using flexible materials and aqueous electrolyte,this paper-based Al ion battery can tolerate various deformations such as bending,rolling and even puncturing without losing its performance.When two single cells are connected in series,the battery pack can provide a charge voltage of 4.3 V and a discharge plateau as high as 3–3.6 V,which are very close to commercial Li ion batteries.Such a cheap,flexible and safe battery technology may be widely applied in low-cost and large-quantity applications,such as RFID tags,smart packages and wearable biosensors in the future.
基金supported by the Fluid Interface Reacions and Transport(FIRST)Centeran Energy Frontier Research Center supported by the U.S.Department of Energy,Office of Science,Basic Energy Sciences+1 种基金Synthesis,XRD,and SEM characterization of α-MoO_(3) were supported as a part of the Center for Mesoscale Transport PropertiesEnergy Frontier Research Center supported by the U.S.Department of Energy,Office of Science,Basic Energy Sciences,under award#DE-SC0012673
文摘While transition-metal oxides such as α-MoO_(3)provide high capacity,their use is limited by modest electronic conductivity and electrochemical instability in aqueous electrolytes.Two-dimensional(2D)MXenes,offer metallic conductivity,but their capacitance is limited in aqueous electrolytes.Insertion of partially solvated cations into Ti_(3)C_(2)MXene from lithium-based water-in-salt(WIS)electrolytes enables charge storage at positive potentials,allowing a wider potential window and higher capacitance.Herein,we demonstrate that α-MoO_(3)/Ti_(3)C_(2)hybrids combine the high capacity of α-MoO_(3)and conductivity of Ti_(3)C_(2)in WIS(19.8 m LiCI)electrolyte in a wide1.8 V voltage window.Cyclic voltammograms reveal multiple redox peaks from α-MoO_(3)in addition to the well-separated peaks of Ti_(3)C_(2)in the hybrid electrode.This leads to a higher specific charge and a higher rate capability compared to a carbon and binder containing α-MoO_(3)electrode.These results demonstrate that the addition of MXene to less conductive oxides eliminates the need for conductive carbon additives and binders,leads to a larger amount of charge stored,and increases redox capacity at higher rates.In addition,MXene encapsulated α-MoO_(3)showed improved electrochemical stability,which was attributed to the suppressed dissolution of α-MoO_(3).The work suggests that oxide/MXene hybrids are promising for energy storage.
基金the financial support from the Brazilian funding agencies CNPq(310544/2019-0),FAPESP(2014/02163-7&2017/11958-1)FAPEMIG(Financial support for the LMMA/UFVJM Laboratory)and CNPq(PQ-2 grant:Process 301095/2018-3)the support from Shell and the strategic importance of the support given by ANP(Brazil’s National Oil,Natural Gas,and Biofuels Agency)through the R&D levy regulation。
文摘Supercapacitors(SCs) are high-power energy storage devices with ultra-fast charge/discharge properties.SCs using concentrated aqueous-based electrolytes can work at low temperatures due to their intrinsic properties, such as higher freezing point depression(FPD) and robustness. Besides the traditional organic-and aqueous-based(salt-in-water) electrolytes used in SCs, water-in-salt(WISE) sodium perchlorate electrolytes offer high FPD, non-flammability, and low-toxicity conditions, allowing the fabrication of safer, environmentally friendly, and more robust devices. For the first time, this work reports a comprehensive study regarding WISE system’s charge-storage capabilities and physicochemical properties under low-temperature conditions(T < 0 ℃) using mesoporous carbon-based electrodes. The effect of temperature reduction on the electrolyte viscosity and electrical properties was investigated using different techniques and the in-situ(or operando) Raman spectroscopy under dynamic polarization conditions.The cell voltage, equivalent series resistance, and specific capacitance were investigated as a function of the temperature. The cell voltage(U) increased ~ 50%, while the specific capacitance decreased ~20%when the temperature was reduced from 25 ℃ to -10 ℃. As a result, the maximum specific energy(E = CU^(2)/2) increased ~ 100%. Therefore, low-temperature WISEs are promising candidates to improve the energy-storage characteristics in SCs.
基金financially supported by the National Natural Science Foundation of China(Nos.21875165,51772216 and 21703161)the Science and Technology Commission of Shanghai Municipality,China(No.14DZ2261100)the Fundamental Research Funds for the Central Universities。
文摘Pore size and distribution in carbon-based materials are regarded to be a key factor to affect the electrochemical capacitive performances of the resultant electrodes.In this study,nitrogen and oxygen codoped porous carbons(NOPCs) are fabricated based on a simple Schiff-base reaction between m-phenylenediamine and terephthalaldehyde.The NOPCs have tunable morphologies,high surface areas,abundant heteroatom doping.More importantly,the carbons show a dominant micropores of 0.5-0.8 nm,comparable to the ionic sizes of LiTFSI(Li^+0.069 nm;TFSI-0.79 nm) water-in-salt electrolyte with a high potential window of 2.2 V.Consequently,the fabricated symmetric supercapacitor gives a high energy output of 30.5 Wh/kg at 1 kW/kg,and high stability after successive 10,000 cycles with ^96.8% retention.This study provides promising potential to develop high-energy supercapacitors.
基金financially supported by the National Natural Science Foundation of China (Nos. 21875165, 51772216, 22172111 and 21905207)the Science and Technology Commission of Shanghai Municipality, China (Nos. 20ZR1460300, 14DZ2261100)+2 种基金Anhui University of Science and Technology Introduced Talent Research Startup Fund (No. 13210572)Zhejiang Provincial Natural Science Foundation of China (No. LY19B010003)the Fundamental Research Funds for the Central Universities and the Large Equipment Test Foundation of Tongji University
文摘A facile fabrication strategy is reported to obtain N/O codoped porous carbon nanosheets for pur-pose of ameliorating the charge transfer and accumulation in the concentrated LiTFSI(lithium bis(trifluoromethane sulfonyl)imide)electrolyte.By tunning the feed ratio of comonomers,the porous nanosheet structure is endowed with a significant ion-adsorption surface area(1630 m^(2)/g)and intercon-nected hierarchical porosity;meanwhile,high-level N/O dopants(N:3.58 at%,O:12.91 at%)increase the effective contact area for electrolyte ions,and further facilitate rapid ion/electron transfer.Benefiting from the advantageous features,carbon nanosheets electrode reveal an enhanced specific capacitance(375 F/g)in three-electrode configuration and the H_(2)SO_(4)-based device yields a high gravimetric energy density of 11.4 Wh/kg.Particularly,the ion-diffusion highways in porous carbon nanosheets contribute to the 2.25 V LiTFSI-based symmetric device with a high energy delivery up to 33.1 Wh/kg.This work offers an in-spiring strategy for facile fabrication of carbon nanosheets,and demonstrates their promising application in“water-in-salt”electrolyte-based supercapacitor systems.
基金Shengyang Dong and Yi Wang contributed equally to this work.This work was supported by the National Natural Science Foundation of China(Nos.U1802256,51672128,51802154)the Key Research and Development Program in Jiangsu Province(BE2018122)+1 种基金Jiangsu Specially-Appointed Professors Program,the Fundamental Research Funds for the Central Universities(NE2016005)the Startup Foundation for Introducing Talent of NUIST(1441622001004).
文摘Aqueous hybrid supercapacitors are attracting increasing attention due to their potential low cost,high safety and eco-friendliness.However,the narrow operating potential window of aqueous electrolyte and the lack of suitable negative electrode materials seriously hinder its future applications.Here,we explore high concentrated lithium acetate with high ionic conductivity of 65.5 mS cm−1 as a green“water-in-salt”electrolyte,providing wide voltage window up to 2.8 V.It facilitates the reversible function of niobium tungsten oxide,Nb18W16O93,that otherwise only operations in organic electrolytes previously.The Nb18W16O93 with lithium-ion intercalation pseudocapacitive behavior exhibits excellent rate performance,high areal capacity,and ultra-long cycling stability.An aqueous lithium-ion hybrid capacitor is developed by using Nb18W16O93 as negative electrode combined with graphene as positive electrode in lithium acetate-based“water-in-salt”electrolyte,delivering a high energy density of 41.9 W kg−1,high power density of 20,000 W kg−1 and unexceptionable stability of 50,000 cycles.
基金XJ thanks Oregon State University for AID program support.J-XJ thanks the financial support from the National Natural Science Foundation of China(21574077 and 21304055)111 project(B14041)+3 种基金the Fundamental Research Funds for the Central Universities(GK201801001)CZ is supported by a fellowship from the China Scholarship Council(201706870033)CF is grateful to the U.S.National Science Foundation CAREER grant(CHE-1455353)the support of the femtosecond stimulated Raman instrumentation and the NSF MRI grant(DMR-1920368)for additional support.
文摘A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert.The electrolyte comprises primarily ZnCl_(2) and LiCl as an additive,both of which are inexpensive salts.The O-H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn-Cl superhalides,as suggested by integrated characterization and simulation.As a result,the average Coulombic efficiency of zincmetal anode is raised to an unprecedented>99.7%at 1mA cm^(−2).In the new electrolyte,the plating/stripping processes leave the zinc-metal anode dendrite-free,and the zinc-metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm^(−2) at 2mA cm^(−2).Furthermore,the high Coulombic efficiency of zinc-metal anode in the ZnCl_(2)-LiCl mixture electrolyte is demonstrated in full cells with a limited anode.The V_(2)O_(5)·H_(2)O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles,and the LiMn_(2)O_(4)||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.
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support from the China Postdoctoral Science Foundation Funded Project (2019M661464)the supported by the Australian Research Council (ARC) through the Discovery Project (DP180102297)+1 种基金the Future Fellow Project (FT180100705)the ARC Research Hub for Integrated Energy Storage Solutions (IH180100020)。
文摘Aqueous rechargeable batteries have attracted enormous attention owning to their intrinsic characteristics of non-flammability, low cost, and the superior ionic conductivity of the aqueous electrolyte.However, the narrow electrochemical stability window(1.23 V), imposed by hydrogen and oxygen evolution, constrains the overall energy density of batteries. The revolutionary "water-in-salt” electrolytes considerably expand the electrochemical stability window to 3 or even 4 volts, giving rise to a new series of high-voltage aqueous metal-ion chemistries. Herein, the recent advances in "water-in-salt” electrolytes for aqueous monovalent-ion(Li^(+), Na^(+), K^(+)) rechargeable batteries have been systematically reviewed. Meanwhile, the corresponding reaction mechanisms, electrochemical performances and the existing challenges and opportunities are also highlighted.
基金The authors acknowledge funding support from the National Key Research and Development Program of China(2018YFE0201702)the National Natural Science Foundation of China(21975052,21935003,21805126)Chenguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(19CG01).
文摘Ammonium-ion batteries are promising solutions for large-scale energy storage systems owing to their costeffectiveness,safety,and sustainability.Herein,we propose an aqueous ammonium-ion battery based on an organic poly(1,5-naphthalenediamine)anode and an inorganic Prussian blue cathode in 19 M(M:mol kg^(-1))CH3COONH_(4)electrolyte.Its operation involves a reversible coordination reaction(C=N/C-N-conversion)in the anode and the NH_(4)^(+)insertion/extraction reaction in the cathode,along with NH_(4)^(+)acting as the charge carrier in a rocking-chair battery.Benefiting from the fast kinetics and stability of both electrodes,this aqueous ammoniumion battery shows an excellent rate capability and long cycle stability for 500 cycles.Moreover,an energy density as high as 31.8 Wh kg^(-1) can be achieved,based on the total mass of the cathode and anode.Surprisingly,this aqueous ammonium-ion battery works well over a wide temperature range from-40 to 80℃.This work will provide new opportunities to build wide-temperature aqueous batteries and broaden the horizons for large-scale energy storage systems.
基金financially supported by the National Natural Science Foundation of China (Nos. 51772216, 21905207, 21875165 and 21703161)the Science and Technology Commission of Shanghai Municipality, China (Nos. 20ZR1460300, 14DZ2261100)+2 种基金Zhejiang Provincial Natural Science Foundation of China (No. LY19B010003)the Fundamental Research Funds for the Central Universitiesthe Large Equipment Test Foundation of Tongji University。
文摘The bio-nanotechnological fabrication of high-surface-area carbons has attracted widespread interest in supercapacitor applications by using readily-available natural products as raw materials or bio-templates,and is expected to refine on pore accessibility for compact energy storage. Here, a renovated design strategy of semi-biomass interpenetrating polymer network(IPN) derived carbon is demonstrated through physically knitting the biomacromolecule(sodium alginate, SA) polymeric chains into the highly crosslinked resorcinol-formaldehyde(RF) network and subsequent thermochemical conversion. Moleculelevel interlacing forces in such IPN efficiently relieve the RF skeleton shrinkage when producing carbon,while the other SA network addresses the macrophase separation issue to sacrifice as an in-knitted porogen and a morphology-directing agent. As a result, porous carbon globules are equipped with moss-like surfaces and interconnected pore architecture for high accessible electrode surface(1013 m^(2)/g), and efficient electrochemical responses are reached with the specific capacitance of 312 F/g at 1 A/g. Taking the advantage of 9 mol/kg NaClO_(4) complex-solvent electrolyte, the voltage window is extended to 2.4 V,endowing the two-electrode device with the high energy delivery of 32.3 Wh/kg at 240 W/kg.
基金supported by the National Natural Science Foundation of China (No.11975043)the Natural Science Foundation of Shandong Province (No.ZR2017LEM011)。
文摘Hydrous electrolytes with high electrochemical potentials were obtained by hydrating water molecules into solutes to form high Li:water molar ratio electrolytes(HMRE).Solid polyethylene glycol(PEG) were e mployed to enha nce the molar ratio of Li^(+) to water in the electrolytes while reducing the consumption of Li-salt.The obtained mole ratio of Li^(+) to wa ter molecules in the hydrous electrolytes was greater than 1:1;however,the mass fraction of Li-salt was reduced to 61%(approximately 5.5 mol/kg,based on water and PEG).Compared with that of water-in-salt electrolytes,the mass fraction of Li-salt could be remarkably reduced by adding solid PEG.The electrochemical stability of the electrolytes improved considerably because of the strong hydration of Li^(+) by the water molecules.A beneficial passivation effect,arising from the decomposition of the electrolyte,at a wide potential window was observed.
