With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery ...With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.展开更多
Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,a...Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,and zinc anode.Summarizing the design principles and strategies toward the optimization of cathode,electrolyte,and zinc anode is crucial for the development of AZIBs.Herein,we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs.Firstly,the various reaction mechanisms are summarized and the existing issues associated with the cathode,electrolyte,and zinc anode are discussed to guide the rational design of AZIBs.Subsequently,we provide an in-depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization,and analyze the advantages and disadvantages of various strategies.Importantly,the design principles and strategies of the newly appeared conversion-type AZIBs,such as Zn-S battery and Zn-Se battery,are also discussed and analyzed.The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail.Finally,some research trends and perspectives are provided for designing better AZIBs.展开更多
Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we...Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we prepared amorphous VCrO precursors by using V2O5 and CrO3 and alcohols or mixtures of alcohol and water via solvothermal reaction at 180°C.The precursors were then calcined under nitrogen at various temperatures.The products were characterized by powder X‐ray diffraction,transmission electron microscopy,and X‐ray photoelectron spectroscopy.It was revealed that pure‐phase nanocrystalline orthorhombic CrVO4 was obtained when methanol or methanol/water was used as the solvothermal medium and the precursor was calcined at 700°C.The size of the CrVO4 crystals was around 500 nm when methanol was used,whereas it reduced significantly to less than 50 nm when a mixture of methanol and water was used.The sizes could be effectively tuned from 10 to 50 nm by varying the methanol/water volume ratio.To the best of our knowledge,this is the first report on the synthesis of pure‐phase CrVO4 nanocrystals.The nano‐CrVO4 showed almost the highest catalytic activity for the ammoxidation of 2,6‐dichlorotoluene to 2,6‐dichlorobenzonitrile among the reported bi‐component composite oxides,owing to its smaller particle size,larger specific surface area,and more exposed active centers.展开更多
Novel cobalt Fischer-Tropsch synthesis (FTS) catalysts were prepared from natural halloysite nanotubes (HNT) by double-solvent and wet- impregnation methods, and characterized by TEM, XRD, TPR and N2 adsorption-de...Novel cobalt Fischer-Tropsch synthesis (FTS) catalysts were prepared from natural halloysite nanotubes (HNT) by double-solvent and wet- impregnation methods, and characterized by TEM, XRD, TPR and N2 adsorption-desorption. Comparing with the catalyst prepared by wet- impregnation method, the catalyst prepared by double-solvent method reduces Co3O4 particle migration and agglomeration due to size-induced effect, thus showing higher catalytic activity for Fischer-Tropsch synthesis.展开更多
Global climate changes,such as extreme weather,sea levels rise,and biodiversity decline,have destructive impacts on the global agrofood system,in terms of crop yield,agrofood quality and consumer safety.Those stressed...Global climate changes,such as extreme weather,sea levels rise,and biodiversity decline,have destructive impacts on the global agrofood system,in terms of crop yield,agrofood quality and consumer safety.Those stressed conditions and environmental pollution for crop and agrofood prompt us to take immediate action to develop a whole-new-era agrofood system from the perspective of sustainability[1].展开更多
High-performance energy storage and sensing devices have been undergoing rapid development to meet the demand for portable and wearable electronic products,which require flexibility,extensibility,small volume and ligh...High-performance energy storage and sensing devices have been undergoing rapid development to meet the demand for portable and wearable electronic products,which require flexibility,extensibility,small volume and lightweight.In this study,we construct a lightweight and flexible self-powered sensing system by integrating a highly stretchable strain sensor with a high-performance asymmetric supercapacitor based on ZnSe/CoSe_(2)//ECNT(ECNT:electrochemically activated carbon nanotube film).The ZnSe/CoSe_(2) two-dimentional nanosheets on carbon nanotube(CNT)films are synthesized through a simple and efficient strategy derived from ZnCo-based metal-organic frameworks(MOFs).The density functional theory(DFT)simulations show the higher conductivity of the ZnSe/CoSe_(2)/CNT electrode than the CoSe_(2)/CNT electrode.Due to the synergistic properties of self-supported two-dimentional ZnSe/CoSe_(2) nanosheets with high specific surface area and the high pathway of one-dimention CNTs,the nanocomposite electrode provides efficient transmission and short paths for electron/ion diffusion.The asymmetric supercapacitor provides a stable output power supply to the sensors that can precisely respond to strain and pressure changes.The sensor can also be attached to a garment for measuring a variety of joint movements.展开更多
The development of a high specific capacity and stable manganese(Mn)-based cathode material is very attractive for aqueous zinc-ion(Zn^(2+))batteries(ZIBs).However,the inherent low electrical conductivity and volume e...The development of a high specific capacity and stable manganese(Mn)-based cathode material is very attractive for aqueous zinc-ion(Zn^(2+))batteries(ZIBs).However,the inherent low electrical conductivity and volume expansion challenges limit its stability improvement.Here,a mesoporous ZnMn_(2)O_(4)(ZMO)nanocage(N-ZMO)coupled with nitrogen doping and oxygen vacancies is prepared by defect engineering and rational structural design as a high-performance cathode material for rechargeable ZIBs.The oxygen vacancies enhance the electrical conductivity of the material and the nitrogen doping releases the strong electrostatic force of the material to maintain a higher structural stability.Interestingly,N-ZMO exhibits excellent ability of Zn^(2+)storage(225.4 mAh·g^(−1)at 0.3 A·g^(−1)),good rate,and stable cycling performance(88.4 mAh·g^(−1)after 1,000 cycles at 3 A·g^(−1)).Furthermore,a flexible quasi-solid-state device with high energy density(261.6 Wh·kg^(−1))is assembled,demonstrating long-lasting durability.We believe that the strategy in this study can provide a new approach for developing aqueous ZIBs.展开更多
Electrochemical conversion reactions provide more selections for Na-storage materials, but the reaction suffers from low reversibility and poor cyclability. Introducing an electrochemically inactive component is a com...Electrochemical conversion reactions provide more selections for Na-storage materials, but the reaction suffers from low reversibility and poor cyclability. Introducing an electrochemically inactive component is a common strategy, but the effect is quite limited since it could not stabilize the structure during long-term cycling. In this study, a new approach is developed using an amino group-functioned hyperbranched polymer (AHP) as a template and electrode additive for the design of high-performance FeSe2-AHP composite with chemical interaction. The assembled FeSe2-AHP composite nanoneedles were prepared by the selenylation of FeS-AHP composite microflowers and entirely inherit the polymer network from the precursor. The amino groups of AHP in composite coordinate with iron cations to achieve uniform polymer dispersion in the composite, and maintain the molecular level mixed state during the long-term cycling. Moreover, the in-situ constructed uniform 3D elastic polymer network effectively accommodates volume expansion and alleviates nanoparticle aggregation during sodiation/de-sodiation. FeSe2-AHP composite provides a superior rate capability (584.8 mAh·g−1 at 20 A·g−1) and a remarkable cyclability with a capacity retention rate of 93.3% after 2,000 cycles. FeSe2-AHP composite shows a high pseudocapacitive behavior for the abundant nanometer interface established by AHP, enhancing the solid-state Na+ diffusion. The FeSe2-AHP anode is also compatible with Na3V2(PO4)3/C cathode in a full Na-ion battery, which provides a high-power performance (powering 51 LEDs). The work herein highlights an innovative and efficient strategy for conversion-type material design and demonstrates the function of chemical interaction of polymer additive in the enhancement of long-term cyclability for conversion electrode.展开更多
基金supported by the National Nature Science Foundation of China(22209211 and 52172241)Hong Kong Research Grants Council(CityU 11315622)+1 种基金the research funds from South-Central Minzu University(YZZ22001)the National Key R&D Program of China(2021YFA1501101).
文摘With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.
基金supported by the research funds from South-Central University for Nationalities(Grant No.YZZ19001)financial support from the National Natural Science Foundation of China(51873233)the Hubei Provincial Natural Science Foundation(2018CFA023)。
文摘Aqueous zinc-ion batteries(AZIBs)are an appealing battery system due to their low cost,intrinsic safety,and environmental-friendliness,while their application is plagued by the obstacles from the cathode,electrolyte,and zinc anode.Summarizing the design principles and strategies toward the optimization of cathode,electrolyte,and zinc anode is crucial for the development of AZIBs.Herein,we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs.Firstly,the various reaction mechanisms are summarized and the existing issues associated with the cathode,electrolyte,and zinc anode are discussed to guide the rational design of AZIBs.Subsequently,we provide an in-depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization,and analyze the advantages and disadvantages of various strategies.Importantly,the design principles and strategies of the newly appeared conversion-type AZIBs,such as Zn-S battery and Zn-Se battery,are also discussed and analyzed.The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail.Finally,some research trends and perspectives are provided for designing better AZIBs.
基金supported by the National Natural Science Foundation of China(21172269)Innovation Group of Hubei Natural Science Foundation(2018CFA023)Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(JDGD-201809)~~
文摘Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we prepared amorphous VCrO precursors by using V2O5 and CrO3 and alcohols or mixtures of alcohol and water via solvothermal reaction at 180°C.The precursors were then calcined under nitrogen at various temperatures.The products were characterized by powder X‐ray diffraction,transmission electron microscopy,and X‐ray photoelectron spectroscopy.It was revealed that pure‐phase nanocrystalline orthorhombic CrVO4 was obtained when methanol or methanol/water was used as the solvothermal medium and the precursor was calcined at 700°C.The size of the CrVO4 crystals was around 500 nm when methanol was used,whereas it reduced significantly to less than 50 nm when a mixture of methanol and water was used.The sizes could be effectively tuned from 10 to 50 nm by varying the methanol/water volume ratio.To the best of our knowledge,this is the first report on the synthesis of pure‐phase CrVO4 nanocrystals.The nano‐CrVO4 showed almost the highest catalytic activity for the ammoxidation of 2,6‐dichlorotoluene to 2,6‐dichlorobenzonitrile among the reported bi‐component composite oxides,owing to its smaller particle size,larger specific surface area,and more exposed active centers.
基金supported by the National Natural Science foundation of China (21073238)the National Basic Research Program of China(2011CB211704)the Special Fund for Basic Scientific Research of Central Colleges,South-Central University for Nationalities
文摘Novel cobalt Fischer-Tropsch synthesis (FTS) catalysts were prepared from natural halloysite nanotubes (HNT) by double-solvent and wet- impregnation methods, and characterized by TEM, XRD, TPR and N2 adsorption-desorption. Comparing with the catalyst prepared by wet- impregnation method, the catalyst prepared by double-solvent method reduces Co3O4 particle migration and agglomeration due to size-induced effect, thus showing higher catalytic activity for Fischer-Tropsch synthesis.
基金supported by the National Key Research and Development Program of China(2018YFE0127000)the National Natural Science Foundation of China(21675127 and 31972150)+3 种基金Shaanxi Provincial Science and Technology Innovation Team(2023-CX-TD-55)the Key Industries Innovation Chain Project of Shaanxi Province(2019ZDLSF07-08)the Natural Science Foundation Project in Guangdong Province(2020A1515010778)Qinghai Provincial Key Laboratory of Qinghai-Tibet Plateau Biological Resource(2020-ZJ-T05).
文摘Global climate changes,such as extreme weather,sea levels rise,and biodiversity decline,have destructive impacts on the global agrofood system,in terms of crop yield,agrofood quality and consumer safety.Those stressed conditions and environmental pollution for crop and agrofood prompt us to take immediate action to develop a whole-new-era agrofood system from the perspective of sustainability[1].
基金support of the National Natural Science Foundation of China(Nos.51702369 and 51873233)Hubei Provincial Natural Science Foundation(No.2018CFA023)the Fundamental Research Funds for the Central Universities(No.CZP20006).
文摘High-performance energy storage and sensing devices have been undergoing rapid development to meet the demand for portable and wearable electronic products,which require flexibility,extensibility,small volume and lightweight.In this study,we construct a lightweight and flexible self-powered sensing system by integrating a highly stretchable strain sensor with a high-performance asymmetric supercapacitor based on ZnSe/CoSe_(2)//ECNT(ECNT:electrochemically activated carbon nanotube film).The ZnSe/CoSe_(2) two-dimentional nanosheets on carbon nanotube(CNT)films are synthesized through a simple and efficient strategy derived from ZnCo-based metal-organic frameworks(MOFs).The density functional theory(DFT)simulations show the higher conductivity of the ZnSe/CoSe_(2)/CNT electrode than the CoSe_(2)/CNT electrode.Due to the synergistic properties of self-supported two-dimentional ZnSe/CoSe_(2) nanosheets with high specific surface area and the high pathway of one-dimention CNTs,the nanocomposite electrode provides efficient transmission and short paths for electron/ion diffusion.The asymmetric supercapacitor provides a stable output power supply to the sensors that can precisely respond to strain and pressure changes.The sensor can also be attached to a garment for measuring a variety of joint movements.
基金the National Natural Science Foundation of China(Nos.51702369 and 51873233)Innovation group of National Ethanic Affairs Commission of China(No.MZR20006)+1 种基金Key R&D Plan of Hubei Province(No.2020BAB077)the Fundamental Research Funds for the Central Universities(Nos.CZZ21009 and CZP20006).
文摘The development of a high specific capacity and stable manganese(Mn)-based cathode material is very attractive for aqueous zinc-ion(Zn^(2+))batteries(ZIBs).However,the inherent low electrical conductivity and volume expansion challenges limit its stability improvement.Here,a mesoporous ZnMn_(2)O_(4)(ZMO)nanocage(N-ZMO)coupled with nitrogen doping and oxygen vacancies is prepared by defect engineering and rational structural design as a high-performance cathode material for rechargeable ZIBs.The oxygen vacancies enhance the electrical conductivity of the material and the nitrogen doping releases the strong electrostatic force of the material to maintain a higher structural stability.Interestingly,N-ZMO exhibits excellent ability of Zn^(2+)storage(225.4 mAh·g^(−1)at 0.3 A·g^(−1)),good rate,and stable cycling performance(88.4 mAh·g^(−1)after 1,000 cycles at 3 A·g^(−1)).Furthermore,a flexible quasi-solid-state device with high energy density(261.6 Wh·kg^(−1))is assembled,demonstrating long-lasting durability.We believe that the strategy in this study can provide a new approach for developing aqueous ZIBs.
基金We gratefully acknowledge the financial support of Hubei Provincial Natural Science Foundation(Nos.2019CFB620 and 2019CFB452)Innovation group of Hubei Natural Science Foundation(No.2018CFA023)the Fundamental Research Funds for the Central Universities,South-Central University for Nationalities(No.CZY20022).
文摘Electrochemical conversion reactions provide more selections for Na-storage materials, but the reaction suffers from low reversibility and poor cyclability. Introducing an electrochemically inactive component is a common strategy, but the effect is quite limited since it could not stabilize the structure during long-term cycling. In this study, a new approach is developed using an amino group-functioned hyperbranched polymer (AHP) as a template and electrode additive for the design of high-performance FeSe2-AHP composite with chemical interaction. The assembled FeSe2-AHP composite nanoneedles were prepared by the selenylation of FeS-AHP composite microflowers and entirely inherit the polymer network from the precursor. The amino groups of AHP in composite coordinate with iron cations to achieve uniform polymer dispersion in the composite, and maintain the molecular level mixed state during the long-term cycling. Moreover, the in-situ constructed uniform 3D elastic polymer network effectively accommodates volume expansion and alleviates nanoparticle aggregation during sodiation/de-sodiation. FeSe2-AHP composite provides a superior rate capability (584.8 mAh·g−1 at 20 A·g−1) and a remarkable cyclability with a capacity retention rate of 93.3% after 2,000 cycles. FeSe2-AHP composite shows a high pseudocapacitive behavior for the abundant nanometer interface established by AHP, enhancing the solid-state Na+ diffusion. The FeSe2-AHP anode is also compatible with Na3V2(PO4)3/C cathode in a full Na-ion battery, which provides a high-power performance (powering 51 LEDs). The work herein highlights an innovative and efficient strategy for conversion-type material design and demonstrates the function of chemical interaction of polymer additive in the enhancement of long-term cyclability for conversion electrode.