The laminated transition metal disulfides(TMDs),which are well known as typical two-dimensional(2D)semiconductive materials,possess a unique layered structure,leading to their wide-spread applications in various field...The laminated transition metal disulfides(TMDs),which are well known as typical two-dimensional(2D)semiconductive materials,possess a unique layered structure,leading to their wide-spread applications in various fields,such as catalysis,energy storage,sensing,etc.In recent years,a lot of research work on TMDs based functional materials in the fields of electromagnetic wave absorption(EMA)has been carried out.Therefore,it is of great significance to elaborate the influence of TMDs on EMA in time to speed up the application.In this review,recent advances in the development of electromagnetic wave(EMW)absorbers based on TMDs,ranging from the VIB group to the VB group are summarized.Their compositions,microstructures,electronic properties,and synthesis methods are presented in detail.Particularly,the modulation of structure engineering from the aspects of heterostructures,defects,morphologies and phases are systematically summarized,focusing on optimizing impedance matching and increasing dielectric and magnetic losses in the EMA materials with tunable EMW absorption performance.Milestones as well as the challenges are also identified to guide the design of new TMDs based dielectric EMA materials with high performance.展开更多
Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage due to the excellent safety, environmental friendliness, natural abundance, high theoretical specific capacity, and low re...Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage due to the excellent safety, environmental friendliness, natural abundance, high theoretical specific capacity, and low redox potential of zinc(Zn) metal. However,several issues such as dendrite formation, hydrogen evolution, corrosion, and passivation of Zn metal anodes cause irreversible loss of the active materials. To solve these issues, researchers often use large amounts of excess Zn to ensure a continuous supply of active materials for Zn anodes. This leads to the ultralow utilization of Zn anodes and squanders the high energy density of AZMBs. Herein, the design strategies for AZMBs with high Zn utilization are discussed in depth, from utilizing thinner Zn foils to constructing anode-free structures with theoretical Zn utilization of 100%, which provides comprehensive guidelines for further research. Representative methods for calculating the depth of discharge of Zn anodes with different structures are first summarized. The reasonable modification strategies of Zn foil anodes, current collectors with pre-deposited Zn, and anode-free aqueous Zn metal batteries(AF-AZMBs) to improve Zn utilization are then detailed. In particular, the working mechanism of AF-AZMBs is systematically introduced. Finally, the challenges and perspectives for constructing high-utilization Zn anodes are presented.展开更多
Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and th...Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and the incompatibility between electrode and electrolytes lead to the deterioration of electrochemical performance of AZMBs during the cycling.The critical point to achieve the stable cycling of AZMBs is to properly regulate the zinc ion solvated structure and transfer behavior between metallic Zn anode and electrolyte.In recent years,numerous achievements have been made to resolve the formation of Zn dendrite and interface incompatible issues faced by AZMBs via optimizing the sheath structure and transport capability of zinc ions at electrode-electrolyte interface.In this review,the challenges for metallic Zn anode and electrode-electrolyte interface in AZMBs including dendrite formation and interface characteristics are presented.Following the influences of different strategies involving designing advanced electrode structu re,artificial solid electrolyte interphase(SEI)on Zn anode and electrolyte engineering to regulate zinc ion solvated sheath structure and transport behavior are summarized and discussed.Finally,the perspectives for the future development of design strategies for dendrite-free Zn metal anode and long lifespan AZMBs are also given.展开更多
The alteration in surface color of metallic glasses(MGs)holds great significance in the context of microstructuredesign and commercial utility.It is essential to accurately describe the structures that are formed duri...The alteration in surface color of metallic glasses(MGs)holds great significance in the context of microstructuredesign and commercial utility.It is essential to accurately describe the structures that are formed during the laser and colorseparation processes in order to develop practical laser coloring applications.Due to the high oxidation sensitivity of Labasedmetallic glass,it can broaden the color range but make it more complex.Structure coloring by laser processing on thesurface of La-based metallic glass can be conducted after thermoplastic forming.It is particularly important to clarify therole of structure and composition in the surface coloring process.The aim is to study the relationship between amorphoussurface structural color,surface geometry,and oxide formation by laser processing in metallic glasses.The findings revealedthat the periodic structure primarily determines the surface color at laser energy densities below 1.0 J/mm^(2).In contrast,thesurface color predominantly depends on the proportion of oxides that are formed when energy densities exceed 1.0 J/mm^(2).Consequently,this study provides a novel concept for the fundamental investigation of laser coloring and establishes a newavenue for practical application.展开更多
The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion devices.Regulating the electronic structure of electrocatalysts by ligands has received partic...The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion devices.Regulating the electronic structure of electrocatalysts by ligands has received particular attention in deriving valid ORR electrocatalysts.Here,the surface electronic structure of Ptbased noble metal aerogels(NMAs)was modulated by various organic ligands,among which the electron-withdrawing ligand of 4-methylphenylene effectively boosted the ORR electrocatalysis.Theoretical calculations suggested the smaller energy barrier for the transformation of O^(*) to OH^(*) and downshift the d-band center of Pt due to the interaction between 4-methylphenylene and the surface metals,thus enhancing the ORR intrinsic activity.Both Pt3Ni and Pt Pd aerogels with 4-methylphenylene decoration performed significant enhancement in ORR activity and durability in different media.Remarkably,the 4-methylphenylene modified Pt Pd aerogel exhibited the higher halfwave potential of 0.952 V and the mass activity of 10.2 times of commercial Pt/C.This work explained the effect of electronic structure on ORR electrocatalytic properties and would promote functionalized NMAs as efficient ORR electrocatalysts.展开更多
Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures....Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures.Herein,a flame-retardant,low-cost and thermally stable long chain phosphate ester based(tributyl phosphate,TBP)electrolyte is reported,which can effectively enhance the cycling stability of highly loaded high-nickel LMBs with high safety through co-solvation strategy.The interfacial compatibility between TBP and electrode is effectively improved using a short-chain ether(glycol dimethyl ether,DME),and a specially competitive solvation structure is further constructed using lithium borate difluorooxalate(LiDFOB)to form the stable and inorganic-rich electrode interphases.Benefiting from the presence of the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)enriched with LiF and Li_(x)PO_(y)F_(z),the electrolyte demonstrates excellent cycling stability assembled using a 50μm lithium foil anode in combination with a high loading NMC811(15.4 mg cm^(-2))cathode,with 88%capacity retention after 120 cycles.Furthermore,the electrolyte exhibits excellent high-temperature characteristics when used in a 1-Ah pouch cell(N/P=0.26),and higher thermal runaway temperature(238℃)in the ARC(accelerating rate calorimeter)demonstrating high safety.This novel electrolyte adopts long-chain phosphate as the main solvent for the first time,and would provide a new idea for the development of extremely high safety and high-temperature electrolytes.展开更多
Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic la...Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.展开更多
Effect of network structure on plasticity and fracture mode of Zr？Al？Ni？Cu bulk metallic glasses （BMGs） was investigated. The microstructures of transversal and longitudinal sections were exposed by chemical etch...Effect of network structure on plasticity and fracture mode of Zr？Al？Ni？Cu bulk metallic glasses （BMGs） was investigated. The microstructures of transversal and longitudinal sections were exposed by chemical etching and observed by scanning electron microscopy （SEM）. The mechanical properties were examined by room-temperature uniaxial compression test. The results show that both plasticity and fracture mode are significantly affected by the network structure and the alteration occurs when the size of the network structure reaches up to a critical value. When the cell size （dc） of the network structure is ~3μm, Zr-based BMGs characterize in plasticity that decreases with increasingdc. The fracture mode gradually transforms from single 45° shear fracture to double 45° shear fracture and then cleavage fracture with increasingdc. In addition, the mechanisms of the transition of the plasticity and the fracture mode for these Zr-based BMGs are also discussed.展开更多
Zirconium-based metallic glasses(Zr-MGs)are demonstrated to exhibit high mechanical strength,low elastic modulus and excellent biocompatibility,making them promising materials for endosseous implants.Meanwhile,tantalu...Zirconium-based metallic glasses(Zr-MGs)are demonstrated to exhibit high mechanical strength,low elastic modulus and excellent biocompatibility,making them promising materials for endosseous implants.Meanwhile,tantalum(Ta)is also well known for its ideal corrosion resistance and biological effects.However,the metal has an elastic modulus as high as 186 GPa which is not comparable to the natural bone(10–30 GPa),and it also has a relative high cost.Here,to fully exploit the advantages of Ta as endosseous implants,a small amount of Ta(as low as 3 at.%)was successfully added into a Zr-MG to generate an advanced functional endosseous implant,Zr58Cu25Al14Ta3 MG,with superior comprehensive properties.Upon carefully dissecting the atomic structure and surface chemistry,the results show that amorphization of Ta enables the uniform distribution in material surface,leading to a significantly improved chemical stability and extensive material-cell contact regulation.Systematical analyses on the immunological,angiogenesis and osteogenesis capability of the material are carried out utilizing the next-generation sequencing,revealing that Zr_(58)Cu_(25)Al_(14)Ta_(3)MG can regulate angiogenesis through VEGF signaling pathway and osteogenesis via BMP signaling pathway.Animal experiment further confirms a sound osseointegration of Zr_(58)Cu_(25)Al_(14)Ta_(3)MG in achieving better bone-implant-contact and inducing faster periimplant bone formation.展开更多
Conventionally,the spatially structured light beams produced by metasurfaces primarily highlight the polarization modulation of the beams propagating along the optical axis or the beams'spatial transmission trajec...Conventionally,the spatially structured light beams produced by metasurfaces primarily highlight the polarization modulation of the beams propagating along the optical axis or the beams'spatial transmission trajectory.In particular,along the optical axis,the polarization state is either constant or varies continuously in each output plane.Here,we develop innovative spatially structured light beams with continually changing polarization along any arbitrary spatial transmission trajectories.With tri-layer metallic metasurfaces,the geometric characteristics of each layer structure can be adjusted to modulate the phase and polarization state of the incident terahertz(THz)wave.The beam will converge to the predefined trajectory along several paths to generate a Bessel-like beam with longitudinal polarization changes.We demonstrate the versatility of the approach by designing two THz-band structured light beams with varying polarization states along the spatial helical transmission trajectory.Continuous linear polarization changes and linear polarization to right circular polarization(RCP)and back to linear polarization changes are realized respectively.The experimental results are basically consistent with the simulated results.Our proposal for arbitrary trajectory structured light beams with longitudinally varying polarization offers a practical method for continuously regulating the characteristics of spatial structured light beams with non-axial transmission.This technique has potential uses in optical encryption,particle manipulation,and biomedical imaging.展开更多
In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment ...In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment is conducive to both morphology and component of the composite,which flower-like ZnO/CoNiO_(2)/CoO/C is obtained.Benefited from good chemical stability of ZnO,high energy capacity of CoNiO_(2) and CoO and good conductivity of C,the as-prepared sample shows promising electrochemical behavior,including the specific capacity of 1435 C·g^(-1) at 1 A·g^(-1),capacity retention of 87.3%at 20 A·g^(-1),and cycling stability of 90.5%for 3000 cycles at 5 A·g^(-1),respectively.Furthermore,the prepared ZnO/CoNiO_(2)/CoO/C/NF//AC aqueous hybrid supercapacitors device delivers the best specific energy of 55.9 W·h·kg^(-1) at 850 W·kg^(-1).The results reflect that the as-prepared ZnO/CoNiO_(2)/CoO/C microflowers are considered as high performance electrode materials for supercapacitor,and the strategy mentioned in this paper is benefit to prepare mixed metal oxides composite for energy conversion and storage.展开更多
A copper-red and silver-white metallic glaze of R_(2)O-RO-Al_(2)O_(3)-SiO_(2)-P_(2)O_(5)system was synthesized by adjusting the firing temperature and glaze components.The coloration mechanism of the metallic glaze wa...A copper-red and silver-white metallic glaze of R_(2)O-RO-Al_(2)O_(3)-SiO_(2)-P_(2)O_(5)system was synthesized by adjusting the firing temperature and glaze components.The coloration mechanism of the metallic glaze was revealed via investigation of the microstructure of the glaze.Our research reveals that the metallic glaze with different colors is mainly due to the amount of Fe_(2)O_(3).The metallic glaze shows a silver-white luster due to a structural color ofα-Fe_(2)O_(3)crystals with a good orientation when the sample contains 0.0939 mol of Fe_(2)O_(3),maintaining temperatures at 1150℃for 0.5 h.The metallic glaze is copper-red which is dominated by the coupling of chemical and structural color ofα-Fe_(2)O_(3)crystals when the sample contains 0.0783 mol of Fe_(2)O_(3).After testing the amount of SiO_(2),we find that 4.0499 mol is the optimal amount to form the ceramic network,and 0.27 mol AlPO_(4)is the best amount to promote phase separation.展开更多
The group V–VI semiconductor material getchellite (crystalline AsSbS_(3)) has garnered extensive attention due to itswonderful electronic and optical properties. The pressure engineering is one of the most effective ...The group V–VI semiconductor material getchellite (crystalline AsSbS_(3)) has garnered extensive attention due to itswonderful electronic and optical properties. The pressure engineering is one of the most effective methods to modulatecrystal structure and physical properties of semiconductor materials. In this study, the structural behavior, optical and electricalproperties of AsSbS_(3) under high pressure have been investigated systematically by in situ high-pressure experimentsfor the first time. The monoclinic structure of AsSbS_(3) remains stable up to 47.0 GPa without phase transition. The graduallattice contraction with increasing pressure results in a continuous narrowing of the bandgap then leads to pressure-inducedmetallization of AsSbS_(3) at 31.5 GPa. Our research presents a high-pressure strategy for tuning the crystal structure andphysical properties of AsSbS_(3) to expand its potential applications in electronic and optoelectronic fields.展开更多
Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering th...Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and transition metal ions in the electrolyte.Consequently,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in stability.Herein,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline Li F,effectively inhibits the undesired Li^(+)/Co^(2+)ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic cobalt.Furthermore,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interphacial stability of the graphite anode.Our findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guidance for designing next-generation electrolytes.展开更多
The dramatic temperature-dependence of liquids dynamics has attracted considerable scientific interests and efforts in the past decades, but the physics of which remains elusive. In addition to temperature, some other...The dramatic temperature-dependence of liquids dynamics has attracted considerable scientific interests and efforts in the past decades, but the physics of which remains elusive. In addition to temperature, some other parameters, such as pressure, loading and size, can also tune the liquid dynamics and induce glass transition, which makes the situation more complicated. Here, we performed molecular dynamics simulations for Ni_(50)Zr_(50) bulk liquid and nanodroplet to study the dynamics evolution in the complex multivariate phase space, especially along the isotherm with the change of pressure or droplet size. It is found that the short-time Debye–Waller factor universally determines the long-time relaxation dynamics no matter how the temperature, pressure or size changes. The basic correlation even holds at the local atomic scale. This finding provides general understanding of the microscopic mechanism of dynamic arrest and dynamic heterogeneity.展开更多
Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construc...Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.展开更多
Lithium metal anode is almost the ultimate choice for high-energy density rechargeable batteries, but its uneven electrochemical dissolution-deposition characteristics lead to poor cycle stability and lithium dendrite...Lithium metal anode is almost the ultimate choice for high-energy density rechargeable batteries, but its uneven electrochemical dissolution-deposition characteristics lead to poor cycle stability and lithium dendrites safety problems. The fundamental solution to the problems is to interfere electrodeposition process of lithium metal so that it can be carried out reversibly and stably. In this work, an inverse-opal structured TiO2membrane with a thickness of only ~1 μm is designed to regulate the electrodeposition behavior of lithium metal, in which the ordered channels homogenize mass transfer process, the anatase TiO_(2)walls of the ion channels reduce desolvation barrier of solvated lithium-ions, and the spherical cavities with a diameter of ~300 nm confine migration of the adsorbed lithium atoms during electrocrystallization to diminish overpotential of lithium. These systematic effects cover and essentially change the whole process of electrodeposition of lithium metal and eliminate the possibility of lithium dendrite formation. The as-obtained lithium metal electrode delivers a Coulombic efficiency of 99.86% in the 100th cycle, and maintains a low deposition overpotential of 0.01 V for 800 h.展开更多
Motivated by the recent experimental work,the pressure-induced structural transition of well-known two-dimensional(2D)1T-Hf Te_(2)was investigated up to 50 GPa through the advanced CALYPSO structure search technique c...Motivated by the recent experimental work,the pressure-induced structural transition of well-known two-dimensional(2D)1T-Hf Te_(2)was investigated up to 50 GPa through the advanced CALYPSO structure search technique combined with the first-principles calculations.Our calculations suggested that the 1T-Hf Te_(2)will first transform to C2/m phase at 3.6 GPa with a volume reduction of 7.6%and then to P62m phase at 9.6 GPa with a volume collapse of 4.6%.The occurrences of 3D C2/m and P62m phases mainly originated from the enhanced Te-Te interlayer coupling and the drastic distortions of Hf-Te polyhedrons in P3m1 phase under compression.Concomitantly,the coordination number of Hf atoms increased from six in P3m1 to eight in C2/m and eventually to nine in P62m at elevated pressure.The metallic and semimetallic nature of C2/m and P62m phases were characterized,and the evidence of the reinforced covalent interactions of Te-Hf and Te-Te orbitals in these two novel high-pressure phases were manifested by the atom-projected electronic DOS and Bader charge.展开更多
We systematically investigate the structures of Cu–Zr metallic glass(MG) by varying the Cu concentration in classic molecular-dynamics simulation. From the pair distribution functions(PDFs), it is found that the near...We systematically investigate the structures of Cu–Zr metallic glass(MG) by varying the Cu concentration in classic molecular-dynamics simulation. From the pair distribution functions(PDFs), it is found that the nearest atomic distance between Zr atom and Zr atom increases significantly after adding Cu, which is related to the composition-dependent coordination behavior between Cu atom and Zr atom in the nearest neighbors. The portion of PDF related to the nearest connection is decomposed into the contributions from quadrilateral structure, pentagonal structure, hexagonal structure,and heptagonal bipyramid structure. Although the population of denser structures, i.e. 5-, 6-, and 7-number sharing ones,increases with Cu addition increasing, the connection distances between the central atoms in all these bipyramids increase for Zr–Zr pairs, leading to the expansion of Zr–Zr nearest atomic distance. These results unveil the effect of the interplay between chemical interaction and geometric packing on the atomic-level structure in Cu–Zr metallic glasses.展开更多
Commercial carbonate-based electrolytes feature highly reactive activities with alkali metals,yielding low Coulombic efficiencies and poor cycle life in lithium metal batteries,which possess much higher chemical activ...Commercial carbonate-based electrolytes feature highly reactive activities with alkali metals,yielding low Coulombic efficiencies and poor cycle life in lithium metal batteries,which possess much higher chemical activity in the rising star sodium metal batteries.To be motivated,we have proposed that decreasing the solvent solvation ability in carbonate-based electrolytes stepwise could enable longterm stable cycling of high-voltage sodium metal batteries.As the solvation capacity reduces,more anions are enticed into the solvation sheath of Na^(+),resulting in the formation of the more desirable interphase layers on the surface of the anode and the cathode.The inorganic-dominated interphases allow highly efficient Na^(+)deposition/stripping processes with a lower rate of dead sodium generation,as well as maintain a stable structure of the high-voltage cathode material.Specifically,the assembled Na||Na_(3)V_(2)(PO_(4))_(2)F_(3)battery exhibits an accelerated ion diffusion kinetics and achieves a higher capacity retention of 85.9%with during the consecutive 200 cycles under the high voltage of 4.5 V.It is anticipated that the tactics we have proposed could be applicable in other secondary metal battery systems as well.展开更多
基金This work was supported by the National Natural Science Foundation of China(52372289,52102368,52072192 and 51977009)Regional Joint Fund for Basic Research and Applied Basic Research of Guangdong Province(No.2020SA001515110905).
文摘The laminated transition metal disulfides(TMDs),which are well known as typical two-dimensional(2D)semiconductive materials,possess a unique layered structure,leading to their wide-spread applications in various fields,such as catalysis,energy storage,sensing,etc.In recent years,a lot of research work on TMDs based functional materials in the fields of electromagnetic wave absorption(EMA)has been carried out.Therefore,it is of great significance to elaborate the influence of TMDs on EMA in time to speed up the application.In this review,recent advances in the development of electromagnetic wave(EMW)absorbers based on TMDs,ranging from the VIB group to the VB group are summarized.Their compositions,microstructures,electronic properties,and synthesis methods are presented in detail.Particularly,the modulation of structure engineering from the aspects of heterostructures,defects,morphologies and phases are systematically summarized,focusing on optimizing impedance matching and increasing dielectric and magnetic losses in the EMA materials with tunable EMW absorption performance.Milestones as well as the challenges are also identified to guide the design of new TMDs based dielectric EMA materials with high performance.
基金the financial support from the National Natural Science Foundation of China (Grant Nos. 52201201, 52372171)the State Key Lab of Advanced Metals and Materials (Grant No. 2022Z-11)+1 种基金the Fundamental Research Funds for the Central Universities (Grant No. 00007747, 06500205)the Initiative Postdocs Supporting Program (Grant No. BX20190002)。
文摘Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage due to the excellent safety, environmental friendliness, natural abundance, high theoretical specific capacity, and low redox potential of zinc(Zn) metal. However,several issues such as dendrite formation, hydrogen evolution, corrosion, and passivation of Zn metal anodes cause irreversible loss of the active materials. To solve these issues, researchers often use large amounts of excess Zn to ensure a continuous supply of active materials for Zn anodes. This leads to the ultralow utilization of Zn anodes and squanders the high energy density of AZMBs. Herein, the design strategies for AZMBs with high Zn utilization are discussed in depth, from utilizing thinner Zn foils to constructing anode-free structures with theoretical Zn utilization of 100%, which provides comprehensive guidelines for further research. Representative methods for calculating the depth of discharge of Zn anodes with different structures are first summarized. The reasonable modification strategies of Zn foil anodes, current collectors with pre-deposited Zn, and anode-free aqueous Zn metal batteries(AF-AZMBs) to improve Zn utilization are then detailed. In particular, the working mechanism of AF-AZMBs is systematically introduced. Finally, the challenges and perspectives for constructing high-utilization Zn anodes are presented.
基金supported by the National Key Research and Development Programs(2021YFB2400400)Major Science and Technology Innovation Project of Hunan Province(2020GK10102020GK1014-4)+7 种基金National Natural Science Foundation of China(32201162)the 70th general grant of China Postdoctoral Science Foundation(2021M702947)Natural Science Foundation of Henan(232300420404)Key Scientific and Technological Project of Henan Province(232102320290,232102311156)Key Research Project Plan for Higher Education Institutions in Henan Province(24A150009,23B430011)Doctor Foundation of Henan University of Engineering(D2022002)the Science and Technology Innovation Program of Hunan Province(2023RC3154)the scientific research projects of Education Department of Hunan Province(23A0188)。
文摘Aqueous Zn metal batteries(AZMBs)with intrinsic safety,high energy density and low cost have been regarded as promising electrochemical energy storage devices.However,the parasitic reaction on metallic Zn anode and the incompatibility between electrode and electrolytes lead to the deterioration of electrochemical performance of AZMBs during the cycling.The critical point to achieve the stable cycling of AZMBs is to properly regulate the zinc ion solvated structure and transfer behavior between metallic Zn anode and electrolyte.In recent years,numerous achievements have been made to resolve the formation of Zn dendrite and interface incompatible issues faced by AZMBs via optimizing the sheath structure and transport capability of zinc ions at electrode-electrolyte interface.In this review,the challenges for metallic Zn anode and electrode-electrolyte interface in AZMBs including dendrite formation and interface characteristics are presented.Following the influences of different strategies involving designing advanced electrode structu re,artificial solid electrolyte interphase(SEI)on Zn anode and electrolyte engineering to regulate zinc ion solvated sheath structure and transport behavior are summarized and discussed.Finally,the perspectives for the future development of design strategies for dendrite-free Zn metal anode and long lifespan AZMBs are also given.
基金supported by the National Natural Science Foundation of China(Grant Nos.52071222 and 52471180)Guangdong Major Project of Basic and Applied Basic Research,China(Grant No.2019B030302010)+2 种基金Guangdong Basic and Applied Basic Research,China(Grant No.2020B1515130007)the National Key Research and Development Program of China(Grant No.2021YFA0716302)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000).
文摘The alteration in surface color of metallic glasses(MGs)holds great significance in the context of microstructuredesign and commercial utility.It is essential to accurately describe the structures that are formed during the laser and colorseparation processes in order to develop practical laser coloring applications.Due to the high oxidation sensitivity of Labasedmetallic glass,it can broaden the color range but make it more complex.Structure coloring by laser processing on thesurface of La-based metallic glass can be conducted after thermoplastic forming.It is particularly important to clarify therole of structure and composition in the surface coloring process.The aim is to study the relationship between amorphoussurface structural color,surface geometry,and oxide formation by laser processing in metallic glasses.The findings revealedthat the periodic structure primarily determines the surface color at laser energy densities below 1.0 J/mm^(2).In contrast,thesurface color predominantly depends on the proportion of oxides that are formed when energy densities exceed 1.0 J/mm^(2).Consequently,this study provides a novel concept for the fundamental investigation of laser coloring and establishes a newavenue for practical application.
基金supported by the National Natural Science Foundation of China(22374119,21902128)the China Postdoctoral Science Foundation(2021M692620)+1 种基金the Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(2021-QZ-01)the Key Project of Natural Science Fund of Shaanxi Province(2023-JC-ZD-06)。
文摘The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion devices.Regulating the electronic structure of electrocatalysts by ligands has received particular attention in deriving valid ORR electrocatalysts.Here,the surface electronic structure of Ptbased noble metal aerogels(NMAs)was modulated by various organic ligands,among which the electron-withdrawing ligand of 4-methylphenylene effectively boosted the ORR electrocatalysis.Theoretical calculations suggested the smaller energy barrier for the transformation of O^(*) to OH^(*) and downshift the d-band center of Pt due to the interaction between 4-methylphenylene and the surface metals,thus enhancing the ORR intrinsic activity.Both Pt3Ni and Pt Pd aerogels with 4-methylphenylene decoration performed significant enhancement in ORR activity and durability in different media.Remarkably,the 4-methylphenylene modified Pt Pd aerogel exhibited the higher halfwave potential of 0.952 V and the mass activity of 10.2 times of commercial Pt/C.This work explained the effect of electronic structure on ORR electrocatalytic properties and would promote functionalized NMAs as efficient ORR electrocatalysts.
基金supported by the National Natural Science Foundation of China (grant No.52072322)the Department of Science and Technology of Sichuan Province (CN) (grant no.23GJHZ0147,23ZDYF0262,2022YFG0294)Research and Innovation Fund for Graduate Students of Southwest Petroleum University (No.:2022KYCX111)。
文摘Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures.Herein,a flame-retardant,low-cost and thermally stable long chain phosphate ester based(tributyl phosphate,TBP)electrolyte is reported,which can effectively enhance the cycling stability of highly loaded high-nickel LMBs with high safety through co-solvation strategy.The interfacial compatibility between TBP and electrode is effectively improved using a short-chain ether(glycol dimethyl ether,DME),and a specially competitive solvation structure is further constructed using lithium borate difluorooxalate(LiDFOB)to form the stable and inorganic-rich electrode interphases.Benefiting from the presence of the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)enriched with LiF and Li_(x)PO_(y)F_(z),the electrolyte demonstrates excellent cycling stability assembled using a 50μm lithium foil anode in combination with a high loading NMC811(15.4 mg cm^(-2))cathode,with 88%capacity retention after 120 cycles.Furthermore,the electrolyte exhibits excellent high-temperature characteristics when used in a 1-Ah pouch cell(N/P=0.26),and higher thermal runaway temperature(238℃)in the ARC(accelerating rate calorimeter)demonstrating high safety.This novel electrolyte adopts long-chain phosphate as the main solvent for the first time,and would provide a new idea for the development of extremely high safety and high-temperature electrolytes.
基金supported by National MCF Energy R&D Program of China(2018YFE0306105)National Key R&D Program of China(2020YFA0406104,2020YFA0406101)+10 种基金Innovative Research Group Project of the National Natural Science Foundation of China(51821002)National Natural Science Foundation of China(52201269,51725204,21771132,51972216,52041202)Natural Science Foundation of Jiangsu Province(BK20210735)Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(21KJB430043)Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 ProjectSuzhou Key Laboratory of Functional Nano&Soft MaterialsJiangsu Key Laboratory for Advanced Negative Carbon Technologiesthe funding from Alexander von Humboldt(AvH)FoundationGusu leading talent plan for scientific and technological innovation and entrepreneurship(ZXL2022487)support from the German Federal Ministry of Education and Research in the framework of the project Catlab(03EW0015A/B)。
文摘Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.
基金Projects(50874045,51301194)supported by the National Natural Science Foundation of ChinaProject(2144057)supported by the Natural Science Foundation of Beijing Municipality,China
文摘Effect of network structure on plasticity and fracture mode of Zr？Al？Ni？Cu bulk metallic glasses （BMGs） was investigated. The microstructures of transversal and longitudinal sections were exposed by chemical etching and observed by scanning electron microscopy （SEM）. The mechanical properties were examined by room-temperature uniaxial compression test. The results show that both plasticity and fracture mode are significantly affected by the network structure and the alteration occurs when the size of the network structure reaches up to a critical value. When the cell size （dc） of the network structure is ~3μm, Zr-based BMGs characterize in plasticity that decreases with increasingdc. The fracture mode gradually transforms from single 45° shear fracture to double 45° shear fracture and then cleavage fracture with increasingdc. In addition, the mechanisms of the transition of the plasticity and the fracture mode for these Zr-based BMGs are also discussed.
基金supported by the National Natural Science Foundation of China(52035001)National Key R&D Program of China(2019YFB1706904)+3 种基金Beijing Training Project for the Leading Talents in S&T(Z191100006119022)National Key Research and Development Plan(2018YFA0703603)National Science 535 Foundation of China(52192602)Youth Fund of the National Natural Science Foundation of China(82201125).
文摘Zirconium-based metallic glasses(Zr-MGs)are demonstrated to exhibit high mechanical strength,low elastic modulus and excellent biocompatibility,making them promising materials for endosseous implants.Meanwhile,tantalum(Ta)is also well known for its ideal corrosion resistance and biological effects.However,the metal has an elastic modulus as high as 186 GPa which is not comparable to the natural bone(10–30 GPa),and it also has a relative high cost.Here,to fully exploit the advantages of Ta as endosseous implants,a small amount of Ta(as low as 3 at.%)was successfully added into a Zr-MG to generate an advanced functional endosseous implant,Zr58Cu25Al14Ta3 MG,with superior comprehensive properties.Upon carefully dissecting the atomic structure and surface chemistry,the results show that amorphization of Ta enables the uniform distribution in material surface,leading to a significantly improved chemical stability and extensive material-cell contact regulation.Systematical analyses on the immunological,angiogenesis and osteogenesis capability of the material are carried out utilizing the next-generation sequencing,revealing that Zr_(58)Cu_(25)Al_(14)Ta_(3)MG can regulate angiogenesis through VEGF signaling pathway and osteogenesis via BMP signaling pathway.Animal experiment further confirms a sound osseointegration of Zr_(58)Cu_(25)Al_(14)Ta_(3)MG in achieving better bone-implant-contact and inducing faster periimplant bone formation.
基金supported by the National Natural Science Foundation of China(Grant Nos.12074094 and 121774271)the Sino-German Mobility Program of the Sino-German Center for Science Funding(Grant No.M-0225)the Capacity Building for Science&Technology Innovation-Fundamental Scientific Research Funds(Grant No.00820531120017).
文摘Conventionally,the spatially structured light beams produced by metasurfaces primarily highlight the polarization modulation of the beams propagating along the optical axis or the beams'spatial transmission trajectory.In particular,along the optical axis,the polarization state is either constant or varies continuously in each output plane.Here,we develop innovative spatially structured light beams with continually changing polarization along any arbitrary spatial transmission trajectories.With tri-layer metallic metasurfaces,the geometric characteristics of each layer structure can be adjusted to modulate the phase and polarization state of the incident terahertz(THz)wave.The beam will converge to the predefined trajectory along several paths to generate a Bessel-like beam with longitudinal polarization changes.We demonstrate the versatility of the approach by designing two THz-band structured light beams with varying polarization states along the spatial helical transmission trajectory.Continuous linear polarization changes and linear polarization to right circular polarization(RCP)and back to linear polarization changes are realized respectively.The experimental results are basically consistent with the simulated results.Our proposal for arbitrary trajectory structured light beams with longitudinally varying polarization offers a practical method for continuously regulating the characteristics of spatial structured light beams with non-axial transmission.This technique has potential uses in optical encryption,particle manipulation,and biomedical imaging.
基金supported by the National Natural Science Foundation of China(22078215)Research Project by Shanxi Scholarship Council of China(2021-055)。
文摘In this work,a new ZnO/CoNiO_(2)/CoO/C metal oxides composite is prepared by cost-effective hydrothermal method coupled with annealing process under N_(2) atmosphere.Notably,the oxidation-defect annealing environment is conducive to both morphology and component of the composite,which flower-like ZnO/CoNiO_(2)/CoO/C is obtained.Benefited from good chemical stability of ZnO,high energy capacity of CoNiO_(2) and CoO and good conductivity of C,the as-prepared sample shows promising electrochemical behavior,including the specific capacity of 1435 C·g^(-1) at 1 A·g^(-1),capacity retention of 87.3%at 20 A·g^(-1),and cycling stability of 90.5%for 3000 cycles at 5 A·g^(-1),respectively.Furthermore,the prepared ZnO/CoNiO_(2)/CoO/C/NF//AC aqueous hybrid supercapacitors device delivers the best specific energy of 55.9 W·h·kg^(-1) at 850 W·kg^(-1).The results reflect that the as-prepared ZnO/CoNiO_(2)/CoO/C microflowers are considered as high performance electrode materials for supercapacitor,and the strategy mentioned in this paper is benefit to prepare mixed metal oxides composite for energy conversion and storage.
基金Funded by the National Natural Science Foundation of China(No.52202231)the College Students Innovation and Entrepreneurship Training Program of Hubei University of Technology(No.202310500039)。
文摘A copper-red and silver-white metallic glaze of R_(2)O-RO-Al_(2)O_(3)-SiO_(2)-P_(2)O_(5)system was synthesized by adjusting the firing temperature and glaze components.The coloration mechanism of the metallic glaze was revealed via investigation of the microstructure of the glaze.Our research reveals that the metallic glaze with different colors is mainly due to the amount of Fe_(2)O_(3).The metallic glaze shows a silver-white luster due to a structural color ofα-Fe_(2)O_(3)crystals with a good orientation when the sample contains 0.0939 mol of Fe_(2)O_(3),maintaining temperatures at 1150℃for 0.5 h.The metallic glaze is copper-red which is dominated by the coupling of chemical and structural color ofα-Fe_(2)O_(3)crystals when the sample contains 0.0783 mol of Fe_(2)O_(3).After testing the amount of SiO_(2),we find that 4.0499 mol is the optimal amount to form the ceramic network,and 0.27 mol AlPO_(4)is the best amount to promote phase separation.
基金Project supported by the National Natural Science Foundation of China(Grant No.42274123)the Special Construction Project Fund for Shandong Provincial Taishan Scholars.
文摘The group V–VI semiconductor material getchellite (crystalline AsSbS_(3)) has garnered extensive attention due to itswonderful electronic and optical properties. The pressure engineering is one of the most effective methods to modulatecrystal structure and physical properties of semiconductor materials. In this study, the structural behavior, optical and electricalproperties of AsSbS_(3) under high pressure have been investigated systematically by in situ high-pressure experimentsfor the first time. The monoclinic structure of AsSbS_(3) remains stable up to 47.0 GPa without phase transition. The graduallattice contraction with increasing pressure results in a continuous narrowing of the bandgap then leads to pressure-inducedmetallization of AsSbS_(3) at 31.5 GPa. Our research presents a high-pressure strategy for tuning the crystal structure andphysical properties of AsSbS_(3) to expand its potential applications in electronic and optoelectronic fields.
基金supported by the National Natural Science Foundation of China(21972049,21573080)。
文摘Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and transition metal ions in the electrolyte.Consequently,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in stability.Herein,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline Li F,effectively inhibits the undesired Li^(+)/Co^(2+)ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic cobalt.Furthermore,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interphacial stability of the graphite anode.Our findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guidance for designing next-generation electrolytes.
基金Project supported by the National Natural Science Foundation of China (Grant No.52031016)。
文摘The dramatic temperature-dependence of liquids dynamics has attracted considerable scientific interests and efforts in the past decades, but the physics of which remains elusive. In addition to temperature, some other parameters, such as pressure, loading and size, can also tune the liquid dynamics and induce glass transition, which makes the situation more complicated. Here, we performed molecular dynamics simulations for Ni_(50)Zr_(50) bulk liquid and nanodroplet to study the dynamics evolution in the complex multivariate phase space, especially along the isotherm with the change of pressure or droplet size. It is found that the short-time Debye–Waller factor universally determines the long-time relaxation dynamics no matter how the temperature, pressure or size changes. The basic correlation even holds at the local atomic scale. This finding provides general understanding of the microscopic mechanism of dynamic arrest and dynamic heterogeneity.
基金National Research Foundation of Korea,Grant/Award Numbers:NRF‐2019M3D1A1079303,NRF‐2021R1A2C1011415,NRF‐2021R1A2C3004019。
文摘Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.
基金Financial supports from the National Key Research and Development Program (2016YFB0100200)National Natural Science Foundation of China (21935006)。
文摘Lithium metal anode is almost the ultimate choice for high-energy density rechargeable batteries, but its uneven electrochemical dissolution-deposition characteristics lead to poor cycle stability and lithium dendrites safety problems. The fundamental solution to the problems is to interfere electrodeposition process of lithium metal so that it can be carried out reversibly and stably. In this work, an inverse-opal structured TiO2membrane with a thickness of only ~1 μm is designed to regulate the electrodeposition behavior of lithium metal, in which the ordered channels homogenize mass transfer process, the anatase TiO_(2)walls of the ion channels reduce desolvation barrier of solvated lithium-ions, and the spherical cavities with a diameter of ~300 nm confine migration of the adsorbed lithium atoms during electrocrystallization to diminish overpotential of lithium. These systematic effects cover and essentially change the whole process of electrodeposition of lithium metal and eliminate the possibility of lithium dendrite formation. The as-obtained lithium metal electrode delivers a Coulombic efficiency of 99.86% in the 100th cycle, and maintains a low deposition overpotential of 0.01 V for 800 h.
基金Project supported by the National Natural Science Foundation of China(Grant No.11964026)the Natural Science Basic Research Plan in Shaanxi Province of China(Grant Nos.2023-JC-YB-021,2022JM-035,and 2022JQ-008)。
文摘Motivated by the recent experimental work,the pressure-induced structural transition of well-known two-dimensional(2D)1T-Hf Te_(2)was investigated up to 50 GPa through the advanced CALYPSO structure search technique combined with the first-principles calculations.Our calculations suggested that the 1T-Hf Te_(2)will first transform to C2/m phase at 3.6 GPa with a volume reduction of 7.6%and then to P62m phase at 9.6 GPa with a volume collapse of 4.6%.The occurrences of 3D C2/m and P62m phases mainly originated from the enhanced Te-Te interlayer coupling and the drastic distortions of Hf-Te polyhedrons in P3m1 phase under compression.Concomitantly,the coordination number of Hf atoms increased from six in P3m1 to eight in C2/m and eventually to nine in P62m at elevated pressure.The metallic and semimetallic nature of C2/m and P62m phases were characterized,and the evidence of the reinforced covalent interactions of Te-Hf and Te-Te orbitals in these two novel high-pressure phases were manifested by the atom-projected electronic DOS and Bader charge.
基金Project supported by the Open Research Fund of Songshan Lake Materials Laboratory, China (Grant No. 2022SLABFN14)。
文摘We systematically investigate the structures of Cu–Zr metallic glass(MG) by varying the Cu concentration in classic molecular-dynamics simulation. From the pair distribution functions(PDFs), it is found that the nearest atomic distance between Zr atom and Zr atom increases significantly after adding Cu, which is related to the composition-dependent coordination behavior between Cu atom and Zr atom in the nearest neighbors. The portion of PDF related to the nearest connection is decomposed into the contributions from quadrilateral structure, pentagonal structure, hexagonal structure,and heptagonal bipyramid structure. Although the population of denser structures, i.e. 5-, 6-, and 7-number sharing ones,increases with Cu addition increasing, the connection distances between the central atoms in all these bipyramids increase for Zr–Zr pairs, leading to the expansion of Zr–Zr nearest atomic distance. These results unveil the effect of the interplay between chemical interaction and geometric packing on the atomic-level structure in Cu–Zr metallic glasses.
基金financial support from the National Natural Science Foundation of China(Grant No.22005172)the Natural Science Foundation of Sichuan Province(Grant No.2023NSFSC1124)+3 种基金the Fundamental Research Funds for the Central Universities(Grant No.YJ2021141)the Science and Technology Cooperation Special Fund of Sichuan University and Zigong City(Grant No.2022CDZG-9)the Natural Science Foundation of Shangdong Province(Grant No.ZR202211280350)the Technological Innovation Project of Tai’an City(Grant No.2022GX064)。
文摘Commercial carbonate-based electrolytes feature highly reactive activities with alkali metals,yielding low Coulombic efficiencies and poor cycle life in lithium metal batteries,which possess much higher chemical activity in the rising star sodium metal batteries.To be motivated,we have proposed that decreasing the solvent solvation ability in carbonate-based electrolytes stepwise could enable longterm stable cycling of high-voltage sodium metal batteries.As the solvation capacity reduces,more anions are enticed into the solvation sheath of Na^(+),resulting in the formation of the more desirable interphase layers on the surface of the anode and the cathode.The inorganic-dominated interphases allow highly efficient Na^(+)deposition/stripping processes with a lower rate of dead sodium generation,as well as maintain a stable structure of the high-voltage cathode material.Specifically,the assembled Na||Na_(3)V_(2)(PO_(4))_(2)F_(3)battery exhibits an accelerated ion diffusion kinetics and achieves a higher capacity retention of 85.9%with during the consecutive 200 cycles under the high voltage of 4.5 V.It is anticipated that the tactics we have proposed could be applicable in other secondary metal battery systems as well.
