The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrot...The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.展开更多
Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction ...Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.展开更多
The development of an inorganic electrochemical stable solid-state electrolyte is essentially responsible for future state-of-the-art all-solid-state lithium batteries(ASSLBs).Because of their advantages in safety,wor...The development of an inorganic electrochemical stable solid-state electrolyte is essentially responsible for future state-of-the-art all-solid-state lithium batteries(ASSLBs).Because of their advantages in safety,working temperature,high energy density,and packaging,ASSLBs can develop an ideal energy storage system for modern electric vehicles(EVs).A solid electrolyte(SE)model must have an economical synthesis approach,exhibit electrochemical and chemical stability,high ionic conductivity,and low interfacial resistance.Owing to its highest conductivity of 17 mS·cm^(-1),and deformability,the sulfide-based Li_(7)P_(3)S_(11) solid electrolyte is a promising contender for the high-performance bulk type of ASSLBs.Herein,we present a current glimpse of the progress of synthetic procedures,structural aspects,and ionic conductivity improvement strategies.Structural elucidation and mechanistic approaches have been extensively discussed by using various characterization techniques.The chemical stability of Li_(7)P_(3)S_(11) could be enhanced via oxide doping,and hard and soft acid/base(HSAB)concepts are also discussed.The issues to be undertaken for designing the ideal solid electrolytes,interfacial challenges,and high energy density have been discoursed.This review aims to provide a bird’s eye view of the recent development of Li_(7)P_(3)S_(11)-based solid-state electrolyte applications and explore the strategies for designing new solid electrolytes with a target-oriented approach to enhance the efficiency of high energy density allsolid-state lithium batteries.展开更多
Refining the electromagnetic wave absorption characteristics of traditional metal–organic framework(MOF)-derived carbon composites remains a challenge because of their discontinuous conductive path.To overcome this l...Refining the electromagnetic wave absorption characteristics of traditional metal–organic framework(MOF)-derived carbon composites remains a challenge because of their discontinuous conductive path.To overcome this limitation,in this work,MOF-derived hierarchical Cu_(9)S_(5)/C nanocomposite fibers are fabricated by electrospinning and subsequent carbonization-sulfurization process.Morphological analyses show that MOF-derived octahedral Cu_(9)S_(5)/C particles are evenly monodis-persed inside carbonaceous fibers.This configuration creates a unique hierarchical structure,ranging from Cu_(9)S_(5)particle embedding,MOF-derived skeleton,to a three-dimensional network.The optimized composite fibers(Cu_(9)S_(5)/C-40)exhibit extraordinary electromagnetic wave absorption performance at a low mass fraction(20 wt%):the minimum reflection loss value reaches-69.6 dB,and the maximum effective absorption bandwidth achieves 5.81 GHz with an extremely thin thick-ness of only 1.83 mm.Systematic investigations demonstrate that constructing the three-dimensional conductive network to connect MOF derivatives is crucial for activating performance enhancement.The unique nano-micro hierarchical structure synergized with elaborate-configured components endows the materials with optimal impedance matching and amplifies the loss capacity of each part.This work provides a reliable example and theoretical guidance for fabricating new-generation high-efficiency MOF-derived fibrous electromagnetic wave absorbers.展开更多
Lithium argyrodites Li_(6)PS_(5)X(X=Cl,Br,I)show great potential as solid electrolytes for solid-state lithium batteries due to their high Li-ion conductivities and excellent electrode compatibility.However,the relati...Lithium argyrodites Li_(6)PS_(5)X(X=Cl,Br,I)show great potential as solid electrolytes for solid-state lithium batteries due to their high Li-ion conductivities and excellent electrode compatibility.However,the relatively low conductivity of Li_(6)PS_(5)I(10^(-6)m S/cm)compared to the other two compositions limits its applications.Herein,Si-doped Li_(6.5)P_(0.5)Si_(0.5)S_(5)I electrolyte is designed and synthesized with superior high conductivity of 3.6 mS/cm.Structural characterization proves the increase due to the anion disorder and volume expansion caused by Si-doping.However,the poor interfacial stability between layered oxide cathode Li Ni_(0.6)Co_(0.2)Mn_(0.2)O_(2)and Li_(6.5)P_(0.5)Si_(0.5)S_(5)I inhibits its battery performance.By introducing Li_(3)InCl6electrolyte in the configuration,the corresponding battery delivers high initial discharge capacity of 150.2m Ah/g and superior cyclability during 250 cycles at 0.5 C.This work offers design strategy to obtain Li_(6)PS_(5)I-based electrolytes for high performance solid-state batteries.展开更多
基金This work was supported by the National Natural Science Foundation of China(No.51477002)the University Synergy Innovation Program of Anhui Province,China(No.GXXT-2019-028).
文摘The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.
基金financially supported by the Scientific and Technological Development Program of Jilin Province(20220201138GX)the support of the National Key R&D Program of China(No.2022YFA1503801)+1 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-022)the Young Cross Team Project of CAS(No.JCTD-2021-14)。
文摘Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.
基金the National Natural Science Foundation of China(51772030,21203008,21975025)the Natural Science Foundation of Beijing(2172051)+1 种基金Beijing Outstanding Young Scientists Program(BJJWZYJH01201910007023)the State Key Laboratory funding by the project for Modification of Chemical Fibers and Polymer Materials,Donghou University.
文摘The development of an inorganic electrochemical stable solid-state electrolyte is essentially responsible for future state-of-the-art all-solid-state lithium batteries(ASSLBs).Because of their advantages in safety,working temperature,high energy density,and packaging,ASSLBs can develop an ideal energy storage system for modern electric vehicles(EVs).A solid electrolyte(SE)model must have an economical synthesis approach,exhibit electrochemical and chemical stability,high ionic conductivity,and low interfacial resistance.Owing to its highest conductivity of 17 mS·cm^(-1),and deformability,the sulfide-based Li_(7)P_(3)S_(11) solid electrolyte is a promising contender for the high-performance bulk type of ASSLBs.Herein,we present a current glimpse of the progress of synthetic procedures,structural aspects,and ionic conductivity improvement strategies.Structural elucidation and mechanistic approaches have been extensively discussed by using various characterization techniques.The chemical stability of Li_(7)P_(3)S_(11) could be enhanced via oxide doping,and hard and soft acid/base(HSAB)concepts are also discussed.The issues to be undertaken for designing the ideal solid electrolytes,interfacial challenges,and high energy density have been discoursed.This review aims to provide a bird’s eye view of the recent development of Li_(7)P_(3)S_(11)-based solid-state electrolyte applications and explore the strategies for designing new solid electrolytes with a target-oriented approach to enhance the efficiency of high energy density allsolid-state lithium batteries.
基金supported by the Natural Science Foundation of Shandong Province(ZR2021ME194,2022TSGC2448,2023TSGC0545)the key research and development program of Shandong Province(2021ZLGX01).
文摘Refining the electromagnetic wave absorption characteristics of traditional metal–organic framework(MOF)-derived carbon composites remains a challenge because of their discontinuous conductive path.To overcome this limitation,in this work,MOF-derived hierarchical Cu_(9)S_(5)/C nanocomposite fibers are fabricated by electrospinning and subsequent carbonization-sulfurization process.Morphological analyses show that MOF-derived octahedral Cu_(9)S_(5)/C particles are evenly monodis-persed inside carbonaceous fibers.This configuration creates a unique hierarchical structure,ranging from Cu_(9)S_(5)particle embedding,MOF-derived skeleton,to a three-dimensional network.The optimized composite fibers(Cu_(9)S_(5)/C-40)exhibit extraordinary electromagnetic wave absorption performance at a low mass fraction(20 wt%):the minimum reflection loss value reaches-69.6 dB,and the maximum effective absorption bandwidth achieves 5.81 GHz with an extremely thin thick-ness of only 1.83 mm.Systematic investigations demonstrate that constructing the three-dimensional conductive network to connect MOF derivatives is crucial for activating performance enhancement.The unique nano-micro hierarchical structure synergized with elaborate-configured components endows the materials with optimal impedance matching and amplifies the loss capacity of each part.This work provides a reliable example and theoretical guidance for fabricating new-generation high-efficiency MOF-derived fibrous electromagnetic wave absorbers.
基金supported by the National Key Research and Development Program(No.2021YFB2400300)the National Key Research and Development Program(No.2021YFB2500200)+1 种基金supported by the National Natural Science Foundation of China(No.52177214)China Fujian Energy Devices Science and Technology Innovation Laboratory Open Fund(No.21COP202211)。
文摘Lithium argyrodites Li_(6)PS_(5)X(X=Cl,Br,I)show great potential as solid electrolytes for solid-state lithium batteries due to their high Li-ion conductivities and excellent electrode compatibility.However,the relatively low conductivity of Li_(6)PS_(5)I(10^(-6)m S/cm)compared to the other two compositions limits its applications.Herein,Si-doped Li_(6.5)P_(0.5)Si_(0.5)S_(5)I electrolyte is designed and synthesized with superior high conductivity of 3.6 mS/cm.Structural characterization proves the increase due to the anion disorder and volume expansion caused by Si-doping.However,the poor interfacial stability between layered oxide cathode Li Ni_(0.6)Co_(0.2)Mn_(0.2)O_(2)and Li_(6.5)P_(0.5)Si_(0.5)S_(5)I inhibits its battery performance.By introducing Li_(3)InCl6electrolyte in the configuration,the corresponding battery delivers high initial discharge capacity of 150.2m Ah/g and superior cyclability during 250 cycles at 0.5 C.This work offers design strategy to obtain Li_(6)PS_(5)I-based electrolytes for high performance solid-state batteries.
