Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herei...Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.展开更多
The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano i...The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.展开更多
The rapid development of new energy vehicles and 5G communication technologies has led to higher demands for the safety,energy density,and cycle performance of lithium-ion batteries as power sources.However,the curren...The rapid development of new energy vehicles and 5G communication technologies has led to higher demands for the safety,energy density,and cycle performance of lithium-ion batteries as power sources.However,the currently used liquid carbonate compounds in commercial lithium-ion battery electrolytes pose potential safety hazards such as leakage,swelling,corrosion,and flammability.Solid electrolytes can be used to mitigate these risks and create a safer lithium battery.Furthermore,high-energy density can be achieved by using solid electrolytes along with high-voltage cathode and metal lithium anode.Two types of solid electrolytes are generally used:inorganic solid electrolytes and polymer solid electrolytes.Inorganic solid electrolytes have high ionic conductivity,electrochemical stability window,and mechanical strength,but suffer from large solid/solid contact resistance between the electrode and electrolyte.Polymer solid electrolytes have good flexibility,processability,and contact interface properties,but low room temperature ionic conductivity,necessitating operation at elevated temperatures.Composite solid electrolytes(CSEs) are a promising alternative because they offer light weight and flexibility,like polymers,as well as the strength and stability of inorganic electrolytes.This paper presents a comprehensive review of recent advances in CSEs to help researchers optimize CSE composition and interactions for practical applications.It covers the development history of solid-state electrolytes,CSE properties with respect to nanofillers,morphology,and polymer types,and also discusses the lithium-ion transport mechanism of the composite electrolyte,and the methods of engineering interfaces with the positive and negative electrodes.Overall,the paper aims to provide an outlook on the potential applications of CSEs in solid-state lithium batteries,and to inspire further research aimed at the development of more systematic optimization strategies for CSEs.展开更多
The electrochemical performance of Li metal anode is closely bound up with the interphase between Li and lithium-loaded skeleton as well as solid electrolyte interphase(SEI)on Li surface.Herein,for the first time,we p...The electrochemical performance of Li metal anode is closely bound up with the interphase between Li and lithium-loaded skeleton as well as solid electrolyte interphase(SEI)on Li surface.Herein,for the first time,we propose a novel liquid-source CHBr_(2)F plasma technology to simultaneously construct dual bromine-fluorine-enriched interphases:NiBr_(2)-NiF_(2) interphase on sponge Ni(SN)skeleton and LiBr-LiF-enriched SEI on Li anode,respectively.Based on density functional theory(DFT)calculations and COMSOL multiphysics simulation results,SN skeleton with NiBr_(2)-NiF_(2)interphase can effectively decrease the local current density with good lithiophilicity.And the LiBr-LiF-enriched SEI on Li surface can function to block electron tunneling and hinder side electrochemical reduction of electrolyte components,thus suppressing the growth of dendrite and facilitating the homogeneous transportation of lithium ions.Consequently,the Li/SN electrodes with modified interphases show remarkable stability with a low overpotential of 22.6 mV over 1800 h at 1 mA cm^(-2)/1 mAh cm^(-2)and an exceptional average Coulombic efficiency of 99.6%.When coupled with LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode,the full cells deliver improved cycling stability with a capacity retention of 79.5%even after 350 cycles at 0.5 C.This study provides a facile and new plasma method for the construction of advanced Li anodes for energy storage.展开更多
Metal-ion(Li-,Na-,Zn-,K-,Mg-,and Al-ion)batteries(MIBs)play an important role in realizing the goals of“emission peak and carbon neutralization”because of their green production techniques,lower pollution,high volta...Metal-ion(Li-,Na-,Zn-,K-,Mg-,and Al-ion)batteries(MIBs)play an important role in realizing the goals of“emission peak and carbon neutralization”because of their green production techniques,lower pollution,high voltage,and large energy density.Carbon-based materials are indispensable for developing MIBs and are widely adopted as active or auxiliary materials in the anodes and cathodes.For example,carbon-based materials,includ-ing graphite,Si/C and hard carbon,have been used as anode materials for Li-and Na-ion batteries.Carbon can also be used as a conductive coating for cathodes,such as in LiFePO 4/C,to achieve better performance.In addition,as new high-valence MIBs(Zn-,Al-,and Mg-ion)have emerged,a growing number of novel carbon-based mate-rials have been utilized to construct high-performance MIBs.Herein,we discuss the recent development trends in advanced carbon-based materials for MIBs.The impact of the structure properties of advanced carbon-based materials on energy storage is addressed,and a perspective on their development is also proposed.展开更多
Correction to:Electrochemical Energy Reviews(2023)6:10 https://doi.org/10.1007/s41918-022-00176-0 The publication of this article unfortunately contained mistakes.The conflict of interest of one of the authors was mis...Correction to:Electrochemical Energy Reviews(2023)6:10 https://doi.org/10.1007/s41918-022-00176-0 The publication of this article unfortunately contained mistakes.The conflict of interest of one of the authors was missing.展开更多
Owing to the advantages of high energy density and environmental friendliness,lithium-ion batteries(LIBs)have been widely used as power sources in electric vehicles,energy storage systems and other devices.Conventiona...Owing to the advantages of high energy density and environmental friendliness,lithium-ion batteries(LIBs)have been widely used as power sources in electric vehicles,energy storage systems and other devices.Conventional LIBs composed of liquid electrolytes(LEs)have potential safety hazards;thermal runaway easily leads to battery explosion and spontaneous combustion.To realize a large-scale energy storage system with higher safety and higher energy density,replacing LEs with solid-state electrolytes(SSEs)has been pursued.Among the many SSEs,sulfide SSEs are attractive because of their high ionic conductivities,easy processabilities and high thermostabilities.However,interfacial issues(interfacial reactions,chemo-mechanical failure,lithium dendrite formation,etc.)between sulfide SSEs and electrodes are factors limiting widespread application.In addition,the intrinsic interfacial issues of sulfide SSEs(electrochemical windows,diffusion mechanisms of Li^(+),etc.)should not be ignored.In this review,the behaviors,properties and mechanisms of interfaces in all-solid-state lithium batteries with a variety of sulfide SSEs are comprehensively summarized.Additionally,recent research progress on advanced characterization methods and designs used to stabilize interfaces is discussed.Finally,outlooks,challenges and possible interface engineering strategies are analyzed and proposed.展开更多
Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challe...Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challenges such as volumetric expansion,limited ionic/electronic conductivity properties and complex manufacturing processes hinder its practical applications.Herein,a novel plasma-enhanced reduced graphene oxide fibers/Si(PrGOFs/Si)composite anode is first proposed by using wet-spinning technology followed by plasma-enhanced reduction method.The PrGOFs provide large space to accommodate the volume expansion of Si nanoparticles(SiNPs)by forming a flexible 3D conductive network.Compared to the conventional thermally reduced graphene oxide fibers/Si(TrGOFs/Si)sample,the PrGOFs/Si anodes demonstrate higher conductivity,specific surface area,and superior fabrication efficiency.Accordingly,the Pr GOFs/Si anodes exhibit a reversible capacity of 698.3 mA h/g,and maintain a specific capacity of 602.5m Ah/g at a current density of 200 m A/g after 100 cycles,superior to conventional Tr GOFs/Si counterparts.This research presents a novel strategy for the preparation of high-performance Si/carbon anodes for energy storage applications.展开更多
Highly active transition metal nitrides are desirable for electrocatalytic reactions,but their long-term stability is still unsatisfactory and thus limiting commercial applications.Herein,for the first time,we report ...Highly active transition metal nitrides are desirable for electrocatalytic reactions,but their long-term stability is still unsatisfactory and thus limiting commercial applications.Herein,for the first time,we report a unique and universal room-temperature urea plasma method for controllable synthesis of N-doped carbon coated metal(Fe,Co,Ni,etc.)nitrides arrays electrocatalysts.The preformed metal oxides arrays can be successfully converted into metal nitrides arrays with preserved nanostructures and a thin layer of N-doped carbon(N-C)via one-step urea plasma.Typically,as a representative case,N-C@CoN nanowire arrays are illustrated and corresponding formation mechanism by plasma is proposed.Notably,the designed N-C@Co N catalysts deliver excellent electrocatalytic activity and long-term stability both in oxygen evolution reaction(OER)and urea oxidation reaction(UOR).For OER,a low overpotential(264 mV at 10 mA/cm^(2))and high stability(>50 h at 20 mA/cm^(2))are acquired.For UOR,a current density of100 m A/cm^(2) is achieved at only 1.39 V and maintain over 100 h.Theoretical calculations reveal that the synergetic coupling effect of CoN and N-C can significantly facilitate the charge-transfer process,optimize adsorbed intermediates binding strength and further greatly decrease the energy barrier.This strategy provides a novel method for fabrication of N-C@metal nitrides as highly active and stable catalysts.展开更多
基金Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province,Grant/Award Number:LR20E020001Foundation of State Key Laboratory of Coal Conversion,Grant/Award Number:J20-21-909+4 种基金Science and Technology Department of Zhejiang Province,Grant/Award Number:2023C01231National Natural Science Foundation of China,Grant/Award Numbers:52372235,52073252,52002052,22379020,U20A20253,21972127,22279116Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment,Grant/Award Number:SKLPEE-KF202206Key Research and Development Project of Science and Technology Department of Sichuan Province,Grant/Award Number:2022YFSY0004Ministry of Education,Grant/Award Number:KFM 202202。
文摘Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.
基金supported by the National Natural Science Foundation of China(22279116 and U20A20253)the Natural Science Foundationof Zhejiang Province(LD22E020006 and LQ24E020012)+3 种基金the Science and Technology Development of Zhejiang Province(2023C01231 and 2024C01095)the Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation(LBMHD24E020001)the China Postdoctoral Science Foundation(2020M671785 and 2020T130597)the Fundamental Research Funds for the Provincial Universities of Zhejiang(2022YW54).
文摘The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.
基金the support of the Zhejiang Provincial Natural Science Foundation of China (LR20E020002, LD22E020006)the National Natural Science Foundation of China (NSFC) (U20A20253, 21972127, 22279116)。
文摘The rapid development of new energy vehicles and 5G communication technologies has led to higher demands for the safety,energy density,and cycle performance of lithium-ion batteries as power sources.However,the currently used liquid carbonate compounds in commercial lithium-ion battery electrolytes pose potential safety hazards such as leakage,swelling,corrosion,and flammability.Solid electrolytes can be used to mitigate these risks and create a safer lithium battery.Furthermore,high-energy density can be achieved by using solid electrolytes along with high-voltage cathode and metal lithium anode.Two types of solid electrolytes are generally used:inorganic solid electrolytes and polymer solid electrolytes.Inorganic solid electrolytes have high ionic conductivity,electrochemical stability window,and mechanical strength,but suffer from large solid/solid contact resistance between the electrode and electrolyte.Polymer solid electrolytes have good flexibility,processability,and contact interface properties,but low room temperature ionic conductivity,necessitating operation at elevated temperatures.Composite solid electrolytes(CSEs) are a promising alternative because they offer light weight and flexibility,like polymers,as well as the strength and stability of inorganic electrolytes.This paper presents a comprehensive review of recent advances in CSEs to help researchers optimize CSE composition and interactions for practical applications.It covers the development history of solid-state electrolytes,CSE properties with respect to nanofillers,morphology,and polymer types,and also discusses the lithium-ion transport mechanism of the composite electrolyte,and the methods of engineering interfaces with the positive and negative electrodes.Overall,the paper aims to provide an outlook on the potential applications of CSEs in solid-state lithium batteries,and to inspire further research aimed at the development of more systematic optimization strategies for CSEs.
基金National Natural Science Foun-dation of China(Grant Nos.52372235,52073252,52002052 and 22379020)Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province(Grant No.LR20E020001)+5 种基金Zhejiang Provincial Natural Science Foundation of China(No.LQ23E020009)Science and Technology Department of Zhejiang Province(Grant No.2023C01231)Key Research and Development Project of Science and Technology Department of Sichuan Province(No.2022YFSY0004)Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology)Min-istry of Education(Grant No.KFM 202202)Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(Grant No.SKLPEE-KF202206),Fuzhou University.
文摘The electrochemical performance of Li metal anode is closely bound up with the interphase between Li and lithium-loaded skeleton as well as solid electrolyte interphase(SEI)on Li surface.Herein,for the first time,we propose a novel liquid-source CHBr_(2)F plasma technology to simultaneously construct dual bromine-fluorine-enriched interphases:NiBr_(2)-NiF_(2) interphase on sponge Ni(SN)skeleton and LiBr-LiF-enriched SEI on Li anode,respectively.Based on density functional theory(DFT)calculations and COMSOL multiphysics simulation results,SN skeleton with NiBr_(2)-NiF_(2)interphase can effectively decrease the local current density with good lithiophilicity.And the LiBr-LiF-enriched SEI on Li surface can function to block electron tunneling and hinder side electrochemical reduction of electrolyte components,thus suppressing the growth of dendrite and facilitating the homogeneous transportation of lithium ions.Consequently,the Li/SN electrodes with modified interphases show remarkable stability with a low overpotential of 22.6 mV over 1800 h at 1 mA cm^(-2)/1 mAh cm^(-2)and an exceptional average Coulombic efficiency of 99.6%.When coupled with LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode,the full cells deliver improved cycling stability with a capacity retention of 79.5%even after 350 cycles at 0.5 C.This study provides a facile and new plasma method for the construction of advanced Li anodes for energy storage.
基金This work was supported by the Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province(Grant No.LR20E020001)the National Natural Science Foundation of China(Grant Nos.52073252,52002052,U20A20253,21972127,22279116)+5 种基金the Science and Technology Department of Zhejiang Province(Grant No.2023C01231)the Key Research and Development Project of Sci-ence and Technology Department of Sichuan Province(Grant no.2022YFSY0004)the Natural Science Foundation of Zhejiang Province(Grant Nos.LY21E040001,LD22E020006,and LY21E020005)the Foundation of the State Key Laboratory of Coal Conversion(Grant No.J20-21-909)the State Key Laboratory of Silicon Materials(Grant No.SKL2021-12)the Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),Ministry of Education(Grant No.KFM 202202).
文摘Metal-ion(Li-,Na-,Zn-,K-,Mg-,and Al-ion)batteries(MIBs)play an important role in realizing the goals of“emission peak and carbon neutralization”because of their green production techniques,lower pollution,high voltage,and large energy density.Carbon-based materials are indispensable for developing MIBs and are widely adopted as active or auxiliary materials in the anodes and cathodes.For example,carbon-based materials,includ-ing graphite,Si/C and hard carbon,have been used as anode materials for Li-and Na-ion batteries.Carbon can also be used as a conductive coating for cathodes,such as in LiFePO 4/C,to achieve better performance.In addition,as new high-valence MIBs(Zn-,Al-,and Mg-ion)have emerged,a growing number of novel carbon-based mate-rials have been utilized to construct high-performance MIBs.Herein,we discuss the recent development trends in advanced carbon-based materials for MIBs.The impact of the structure properties of advanced carbon-based materials on energy storage is addressed,and a perspective on their development is also proposed.
文摘Correction to:Electrochemical Energy Reviews(2023)6:10 https://doi.org/10.1007/s41918-022-00176-0 The publication of this article unfortunately contained mistakes.The conflict of interest of one of the authors was missing.
基金support from the Zhejiang Provincial Natural Science Foundation of China under Grant Nos.LR20E020002,LD22E020006Zhe-jiang Provincial Ten-thousand Talents Plan under Grant No.2020R51004+1 种基金the National Natural Science Foundation of China(NSFC)under Grant Nos.U20A20253,21972127,51677170Dr.Fan thanks the support by the U.S.Department of Energy's Office of Energy Efficiency and Renewable Energy(EERE)under the Vehicle Technology Program under Contact DE EE0008864.
文摘Owing to the advantages of high energy density and environmental friendliness,lithium-ion batteries(LIBs)have been widely used as power sources in electric vehicles,energy storage systems and other devices.Conventional LIBs composed of liquid electrolytes(LEs)have potential safety hazards;thermal runaway easily leads to battery explosion and spontaneous combustion.To realize a large-scale energy storage system with higher safety and higher energy density,replacing LEs with solid-state electrolytes(SSEs)has been pursued.Among the many SSEs,sulfide SSEs are attractive because of their high ionic conductivities,easy processabilities and high thermostabilities.However,interfacial issues(interfacial reactions,chemo-mechanical failure,lithium dendrite formation,etc.)between sulfide SSEs and electrodes are factors limiting widespread application.In addition,the intrinsic interfacial issues of sulfide SSEs(electrochemical windows,diffusion mechanisms of Li^(+),etc.)should not be ignored.In this review,the behaviors,properties and mechanisms of interfaces in all-solid-state lithium batteries with a variety of sulfide SSEs are comprehensively summarized.Additionally,recent research progress on advanced characterization methods and designs used to stabilize interfaces is discussed.Finally,outlooks,challenges and possible interface engineering strategies are analyzed and proposed.
基金supported by Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province(No.LR20E020001)National Natural Science Foundation of China(Nos.52372235,52073252,22379020,52002052,U20A20253,21972127,22279116)+3 种基金Science and Technology Department of Zhejiang Province(Nos.2023C01231,Q23E020046,LD22E020006,and LY21E020005)Key Research and Development Project of Science and Technology Department of Sichuan Province(No.2022YFSY0004)Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),Ministry of Education(No.KFM 202202)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEEKF202206),Fuzhou University。
文摘Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challenges such as volumetric expansion,limited ionic/electronic conductivity properties and complex manufacturing processes hinder its practical applications.Herein,a novel plasma-enhanced reduced graphene oxide fibers/Si(PrGOFs/Si)composite anode is first proposed by using wet-spinning technology followed by plasma-enhanced reduction method.The PrGOFs provide large space to accommodate the volume expansion of Si nanoparticles(SiNPs)by forming a flexible 3D conductive network.Compared to the conventional thermally reduced graphene oxide fibers/Si(TrGOFs/Si)sample,the PrGOFs/Si anodes demonstrate higher conductivity,specific surface area,and superior fabrication efficiency.Accordingly,the Pr GOFs/Si anodes exhibit a reversible capacity of 698.3 mA h/g,and maintain a specific capacity of 602.5m Ah/g at a current density of 200 m A/g after 100 cycles,superior to conventional Tr GOFs/Si counterparts.This research presents a novel strategy for the preparation of high-performance Si/carbon anodes for energy storage applications.
基金supported by National Natural Science Foundation of China(No.52073252)Science and Technology Department of Zhejiang Province(No.2023C01231)+2 种基金Key Research and Development Project of Science and Technology Department of Sichuan Province(No.2022YFSY0004)Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology)Ministry of Education(No.KFM 202202),and the Open Project Program of the State Key Laboratory of New textile Materials and Advanced Processing Technologies(No.FZ2021009)。
文摘Highly active transition metal nitrides are desirable for electrocatalytic reactions,but their long-term stability is still unsatisfactory and thus limiting commercial applications.Herein,for the first time,we report a unique and universal room-temperature urea plasma method for controllable synthesis of N-doped carbon coated metal(Fe,Co,Ni,etc.)nitrides arrays electrocatalysts.The preformed metal oxides arrays can be successfully converted into metal nitrides arrays with preserved nanostructures and a thin layer of N-doped carbon(N-C)via one-step urea plasma.Typically,as a representative case,N-C@CoN nanowire arrays are illustrated and corresponding formation mechanism by plasma is proposed.Notably,the designed N-C@Co N catalysts deliver excellent electrocatalytic activity and long-term stability both in oxygen evolution reaction(OER)and urea oxidation reaction(UOR).For OER,a low overpotential(264 mV at 10 mA/cm^(2))and high stability(>50 h at 20 mA/cm^(2))are acquired.For UOR,a current density of100 m A/cm^(2) is achieved at only 1.39 V and maintain over 100 h.Theoretical calculations reveal that the synergetic coupling effect of CoN and N-C can significantly facilitate the charge-transfer process,optimize adsorbed intermediates binding strength and further greatly decrease the energy barrier.This strategy provides a novel method for fabrication of N-C@metal nitrides as highly active and stable catalysts.