The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added chemicals.Yet their complex molecular structures often require multiple active sit...The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added chemicals.Yet their complex molecular structures often require multiple active sites synergy for effective activation and achieving high chemoselectivity.Herein,it is reported that a high-entropy alloy(HEA)on high-entropy oxide(HEO)hetero-structured catalyst for highly active,chemoselective,and robust vanillin hydrodeoxygenation.The heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs(NiZnCuFeAlZrO_(x)),where exsolvable metals(e.g.,Ni,Zn,Cu)in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO matrix.This catalyst exhibits excellent catalytic performance:100%conversion of vanillin and 95%selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120℃,which were attributed to the synergistic effect among HEO matrix(with abundant oxygen vacancies),anchored HEA nanoparticles(having excellent hydrogenolysis capability),and their intimate hetero-interfaces(showing strong electron transferring effect).Therefore,our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion,which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.展开更多
Thermal insulation materials play an increasingly important role in protecting mechanical parts functioning at high temperatures.In this study,a new porous high-entropy(La_(1/6)Ce_(1/6)Pr_(1/6)Sm_(1/6)Eu_(1/6)Gd_(1/6)...Thermal insulation materials play an increasingly important role in protecting mechanical parts functioning at high temperatures.In this study,a new porous high-entropy(La_(1/6)Ce_(1/6)Pr_(1/6)Sm_(1/6)Eu_(1/6)Gd_(1/6))PO_(4)(HE(6RE_(1/6))PO_(4))ceramics was prepared by combining the high-entropy method with the pore-forming agent method and the effect of different starch contents(0–60vol%)on this ceramic properties was systematically investigated.The results show that the porous HE(6RE_(1/6))PO_(4)ceramics with 60vol%starch exhibit the lowest thermal conductivity of 0.061 W·m^(-1)·K^(-1)at room temperature and good pore structure stability with a linear shrinkage of approximately1.67%.Moreover,the effect of large regular spherical pores(>10μm)on its thermal insulation performance was discussed,and an optimal thermal conductivity prediction model was screened.The superior properties of the prepared porous HE(6RE_(1/6))PO_(4)ceramics allow them to be promising insulation materials in the future.展开更多
High-entropy alloys(HEAs),which were introduced as a pioneering concept in 2004,have captured the keen interest of nu-merous researchers.Entropy,in this context,can be perceived as representing disorder and randomness...High-entropy alloys(HEAs),which were introduced as a pioneering concept in 2004,have captured the keen interest of nu-merous researchers.Entropy,in this context,can be perceived as representing disorder and randomness.By contrast,elemental composi-tions within alloy systems occupy specific structural sites in space,a concept referred to as structure.In accordance with Shannon entropy,structure is analogous to information.Generally,the arrangement of atoms within a material,termed its structure,plays a pivotal role in dictating its properties.In addition to expanding the array of options for alloy composites,HEAs afford ample opportunities for diverse structural designs.The profound influence of distinct structural features on the exceptional behaviors of alloys is underscored by numer-ous examples.These features include remarkably high fracture strength with excellent ductility,antiballistic capability,exceptional radi-ation resistance,and corrosion resistance.In this paper,we delve into various unique material structures and properties while elucidating the intricate relationship between structure and performance.展开更多
Specific grades of high-entropy alloys(HEAs)can provide opportunities for optimizing properties toward high-temperature applications.In this work,the Co-based HEA with a chemical composition of Co_(47.5)Cr_(30)Fe_(7.5...Specific grades of high-entropy alloys(HEAs)can provide opportunities for optimizing properties toward high-temperature applications.In this work,the Co-based HEA with a chemical composition of Co_(47.5)Cr_(30)Fe_(7.5)Mn_(7.5)Ni_(7.5)(at%)was chosen.The refractory metallic elements hafnium(Hf)and molybdenum(Mo)were added in small amounts(1.5at%)because of their well-known positive effects on high-temperature properties.Inclusion characteristics were comprehensively explored by using a two-dimensional cross-sectional method and extracted by using a three-dimensional electrolytic extraction method.The results revealed that the addition of Hf can reduce Al_(2)O_(3)inclusions and lead to the formation of more stable Hf-rich inclusions as the main phase.Mo addition cannot influence the inclusion type but could influence the inclusion characteristics by affecting the physical parameters of the HEA melt.The calculated coagulation coefficient and collision rate of Al_(2)O_(3)inclusions were higher than those of HfO_(2)inclusions,but the inclusion amount played a larger role in the agglomeration behavior of HfO_(2)and Al_(2)O_(3)inclusions.The impurity level and active elements in HEAs were the crucial factors affecting inclusion formation.展开更多
The tension and compression of face-centered-cubic high-entropy alloy(HEA) nanowires are significantly asymmetric, but the tension–compression asymmetry in nanoscale body-centered-cubic(BCC) HEAs is still unclear. In...The tension and compression of face-centered-cubic high-entropy alloy(HEA) nanowires are significantly asymmetric, but the tension–compression asymmetry in nanoscale body-centered-cubic(BCC) HEAs is still unclear. In this study,the tension–compression asymmetry of the BCC Al Cr Fe Co Ni HEA nanowire is investigated using molecular dynamics simulations. The results show a significant asymmetry in both the yield and flow stresses, with BCC HEA nanowire stronger under compression than under tension. The strength asymmetry originates from the completely different deformation mechanisms in tension and compression. In compression, atomic amorphization dominates plastic deformation and contributes to the strengthening, while in tension, deformation twinning prevails and weakens the HEA nanowire.The tension–compression asymmetry exhibits a clear trend of increasing with the increasing nanowire cross-sectional edge length and decreasing temperature. In particular, the compressive strengths along the [001] and [111] crystallographic orientations are stronger than the tensile counterparts, while the [110] crystallographic orientation shows the exactly opposite trend. The dependences of tension–compression asymmetry on the cross-sectional edge length, crystallographic orientation,and temperature are explained in terms of the deformation behavior of HEA nanowire as well as its variations caused by the change in these influential factors. These findings may deepen our understanding of the tension–compression asymmetry of the BCC HEA nanowires.展开更多
We describe a novel mechanism for the synthesis of a stable high-entropy alloy powder from an otherwise immiscible Mg-Ti rich metallic mixture by employing high-energy mechanical milling.The presented methodology expe...We describe a novel mechanism for the synthesis of a stable high-entropy alloy powder from an otherwise immiscible Mg-Ti rich metallic mixture by employing high-energy mechanical milling.The presented methodology expedites the synthesis of amorphous alloy powder by strategically injecting entropic disorder through the inclusion of multi-principal elements in the alloy composition.Predictions from first principles and materials theory corroborate the results from microscopic characterizations that reveal a transition of the amorphous phase from a precursor intermetallic structure.This transformation,characterized by the emergence of antisite disorder,lattice expansion,and the presence of nanograin boundaries,signifies a departure from the precursor intermetallic structure.Additionally,this phase transformation is accelerated by the presence of multiple principal elements that induce severe lattice distortion and a higher configurational entropy.The atomic size mismatch of the dissimilar elements present in the alloy produces a stable amorphous phase that resists reverting to an ordered lattice even on annealing.展开更多
Experimental scratch tests and first-principles calculations were used to investigate the adhesion property of AlCrNbSiTi high-entropy alloy(HEA)coatings on zirconium substrates.AlCrNbSiTi HEA and Cr coatings were dep...Experimental scratch tests and first-principles calculations were used to investigate the adhesion property of AlCrNbSiTi high-entropy alloy(HEA)coatings on zirconium substrates.AlCrNbSiTi HEA and Cr coatings were deposited on Zr alloy substrates using multi-arc ion plating technology,and scratch tests were subsequently conducted to estimate the adhesion property of the coatings.The results indicated that Cr coatings had better adhesion strength than HEA coatings,and the HEA coatings showed brittleness.The special quasi-random structure approach was used to build HEA models,and Cr/Zr and HEA/Zr interface models were employed to investigate the cohesion between the coatings and Zr substrate using first-principles calculations.The calculated interface energies showed that the cohesion between the Cr coating and the Zr substrate was stronger than that of the HEA coating with Zr.In contrary to Al or Si in the HEA coating,Cr,Nb,and Ti atoms binded strongly with Zr substrate.Based on the calculated elastic constants,it was found that low Cr and high Al content decreased the mechanical performances of HEA coatings.Finally,this study demonstrated the utilization of a combined approach involving first-principles calculations and experimental studies for future HEA coating development.展开更多
Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass exhibited excellent magnetic refrigeration material with a wide temperature range and high refrigeration capacity(RC)was reported.Er_(20)Ho_(20)Dy_(20)Cu_...Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass exhibited excellent magnetic refrigeration material with a wide temperature range and high refrigeration capacity(RC)was reported.Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass was observed with typical spin glass behavior around 15.5 K.In addition,we find that the magnetic entropy change(-△S_(M))originates from the sample undergoing a ferromagnetic(FM)to paramagnetic(PM)transition around 20 K.Under a field change from 0 T to 7 T,the value of maximum magnetic entropy change(-△S_(M)^(max))reaches 12.5 J/kg·K,and the corresponding value of RC reaches 487.7 J/kg in the temperature range from 6 K to 60 K.The large RC and wide temperature range make the Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass be a promising material for application in magnetic refrigerators.展开更多
This review focuses on thermodynamic and physical parameters,synthesis methods,and reported phases of Magnesium(Mg)containing high-entropy alloys(HEAs).Statistical data of publications concerning Mg-containing HEAs we...This review focuses on thermodynamic and physical parameters,synthesis methods,and reported phases of Magnesium(Mg)containing high-entropy alloys(HEAs).Statistical data of publications concerning Mg-containing HEAs were collected and analyzed.Data on the chemical elements included in Mg-containing HEAs,their theoretical end experimental densities,thermodynamic parameters,physical parameters,fabricated techniques and reported phases were also collected and discussed.On the basis of this information,a new classification for HEAs was proposed.It is also shown that the existing thermodynamic parameters cannot accurately predict the formation of a single phase solid solution for Mg-containing HEAs.The physical parameters of Mg-containing HEAs are within a wide range,and most of the synthesized Mg-containing HEAs have a complex multiphase structure.展开更多
AlCrCuFeMnx(x=0,0.5,1,1.5,and 2)high-entropy alloys were prepared using the vacuum arc melting technology.The microstructure and mechanical properties of AlCrCuFeMnxwere analyzed and tested by XRD,SEM,TEM,nanoindentat...AlCrCuFeMnx(x=0,0.5,1,1.5,and 2)high-entropy alloys were prepared using the vacuum arc melting technology.The microstructure and mechanical properties of AlCrCuFeMnxwere analyzed and tested by XRD,SEM,TEM,nanoindentation,and electronic universal testing.The results indicate that the AlCrCuFeMnxhigh-entropy alloy exhibits a dendritic structure,consisting of dendrites with a BCC structure,interdendrite regions with an FCC structure,and precipitates with an ordered BCC structure that form within the dendrite.Manganese(Mn)has a strong affinity for dendritic,interdendritic,and precipitate structures,allowing it to easily enter these areas.With an increase in Mn content,the size of the precipitated nanoparticles in the dendritic region initially increases and then decreases.Similarly,the area fraction initially decreases and then increases.Additionally,the alloy’s strength and wear resistance decrease,while its plasticity increases.The Al Cr Cu Fe Mn1.5alloy boasts excellent mechanical properties,including a hardness of 360 HV and a wear rate of 2.4×10^(-5)mm^(3)·N^(-1)·mm^(-1).It also exhibits impressive yield strength,compressive strength,and deformation rates of 960 MPa,1,700 MPa,and 27.5%,respectively.展开更多
High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inhere...High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.展开更多
A series of high-entropy alloys(HEAs) containing nanoprecipitates of varying sizes is successfully prepared by a non-consuming vacuum arc melting method.In order to study the irradiation evolution of helium bubbles in...A series of high-entropy alloys(HEAs) containing nanoprecipitates of varying sizes is successfully prepared by a non-consuming vacuum arc melting method.In order to study the irradiation evolution of helium bubbles in the FeCoNiCrbased HE As with γ' precipitates,these samples are irradiated by 100-keV helium ions with a fluence of 5 × 10^(20) ions/m^(2) at 293 K and 673 K,respectively.And the samples irradiated at room temperature are annealed at different temperatures to examine the diffusion behavior of helium bubbles.Transmission electron microscope(TEM) is employed to characterize the structural morphology of precipitated nanoparticles and the evolution of helium bubbles.Experimental results reveal that nanosized,spherical,dispersed,coherent,and ordered L1_(2)-type Ni_(3)Ti γ' precipitations are introduced into FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs by means of ageing treatments at temperatures between 1073 K and 1123 K.Under the ageing treatment conditions adopted in this work,γ' nanoparticles are precipitated in FeCoNiCr(Ni_(3)Ti)_(0.1) HE As,with average diameters of 15.80 nm,37.09 nm,and 62.50 nm,respectively.The average sizes of helium bubbles observed in samples after 673-K irradiation are 1.46 nm,1.65 nm,and 1.58 nm,respectively.The improvement in the irradiation resistance of FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs is evidenced by the diminution in bubbles size.Furthermore,the FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs containing γ' precipitates of 15.8 nm exhibits the minimum size and density of helium bubbles,which can be ascribed to the considerable helium trapping effects of heterogeneous coherent phase boundaries.Subsequently,annealing experiments conducted after 293-K irradiation indicate that HEAs containing precipitated phases exhibits smaller apparent activation energy(E_(a)) for helium bubbles,resulting in larger helium bubble size.This study provides guidance for improving the irradiation resistance of L1_(2)-strengthened high-entropy alloy.展开更多
The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to impr...The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral resources.However,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to date.In addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation technology.In this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral surface.The homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain balance.The flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption decreases.According to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency and stability of the flotation reagents improves refractory mineral flotation.展开更多
Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prosp...Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prospects of high-entropy materials with high structural disorder and strong component controllability in the field of electrochemical energy storage,herein,a novel high-entropy garnet-type oxide solid electrolyte,Li_(5.75)Ga_(0.25)La_(3)Zr_(0.5)Ti_(0.5)Sn_(0.5)Nb_(0.5)O_(12)(LGLZTSNO)was constructed by partially replacing the Li and Zr sites in Li_(7)La_(3)Zr_(2)O_(12)with Ga and Ti/Sn/Nb elements,respectively.The experimental and density functional theory(DFT)calculation results show that the high-entropy LGLZTSNO electrolyte has preferable room temperature ion conductivity,air stability,interface contact performance with lithium anode,and the ability to suppress lithium dendrites.Thanks to the improvement of electrolyte performance,the critical current density of Li/Ag@LGLZTSNO/Li symmetric cell was increased from 0.42 to 1.57 mA cm^(−2),and the interface area specific impedance(IASR)was reduced from 765.2 to 42.3Ωcm^(2).Meanwhile,the Li/Ag@LGLZTSNO/LFP full cell also exhibits excellent rate performance and cycling performance(148 mA h g^(−1)at 0.1 C and 124 mA h g^(−1)at 0.5 C,capacity retention up to 84.8%after 100 cycles at 0.1 C),showing the application prospects of high-entropy LGLZTSNO solid electrolyte in high-performance all solid state lithium batteries.展开更多
lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance....lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance.Here we demonstrate the low-enthalpy and high-entropy(LEHE)electrolytes can intrinsically generate remarkably free ions and high mobility,enabling them to efficiently drive lithium-ion storage.The LEHE electrolytes are constructed on the basis of introducing CsPbl_(3)perovskite quantum dots(PQDs)to strengthen PEO@LiTFSI complexes.An extremely stable cycling>1000 h at 0.3 mA cm^(-2)can be delivered by LEHE electrolytes.Also,the as-developed Li|LEHE|LiFePO_(4)cell retains 92.3%of the initial capacity(160.7 mAh g^(-1))after 200 cycles.This cycling stability is ascribed to the suppressed charge concentration gradient leading to free lithium dendrites.It is realized by a dramatic increment in lithium-ion transference number(0.57 vs 0.19)and a significant decline in ion-transfer activation energy(0.14 eV vs 0.22 eV)for LEHE electrolytes comparing with PEO@LiTFSI counterpart.The CsPbl_(3)PQDs promote highly structural disorder by inhibiting crystallization and hence endow polymer electrolytes with low melting enthalpy and high structural entropy,which in turn facilitate long-term cycling stability and excellent rate-capability of lithium-metal batteries.展开更多
Since the superior mechanical,chemical and physical properties of high-entropy alloys(HEAs)were discovered,they have gradually become new emerging candidates for renewable energy applications.This review presents the ...Since the superior mechanical,chemical and physical properties of high-entropy alloys(HEAs)were discovered,they have gradually become new emerging candidates for renewable energy applications.This review presents the novel applications of HEAs in thermoelectric energy conversion.Firstly,the basic concepts and structural properties of HEAs are introduced.Then,we discuss a number of promising thermoelectric materials based on HEAs.Finally,the conclusion and outlook are presented.This article presents an advanced understanding of the thermoelectric properties of HEAs,which provides new opportunities for promoting their applications in renewable energy.展开更多
Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is rea...Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is realized by doping V^(3+)site with Ga^(3+)/Cr^(3+)/Al^(3+)/Fe^(3+)/In^(3+)simultaneously(i.e.Na_(3)V_(2-x)(GaCrAlFeIn)_x(PO_(4))_(3);x=0,0.04,0.06,and 0.08)to stimulate the V^(5+)■V^(2+)reversible multi-electron redox.Such configuration high-entropy can effectively suppress the structural collapse,enhance the redox reversibility in high working voltage(4.0 V),and optimize the electronic induced effect.The in-situ X-ray powder diffraction and in-situ electrochemical impedance spectroscopy tests efficaciously confirm the robust structu ral recovery and far lower polarization throughout an entire charge-discharge cycle during 1.6-4.3 V,respectively.Moreover,the density functional theory calculations clarify the stronger metallicity of high-entropy electrode than the bare that is derived from the more mobile free electrons surrounding the vicinity of Fermi level.By grace of high-entropy design and multi-electron transfer reactions,the optimal Na_(3)V_(1.7)(GaCrAlFeIn)_(0.06)(PO_(4))_(3)can exhibit perfect cycling/rate performances(90.97%@5000 cycles@30 C;112 mA h g^(-1)@10 C and 109 mA h g^(-1)@30 C,2.0-4.3 V).Furthermore,it can supply ultra-high185 mA h g^(-1)capacity with fa ntastic energy density(522 W h kg^(-1))in half-cells(1.4-4.3 V),and competitive capacity(121 mA h g^(-1))as well as energy density(402 W h kg^(-1))in full-cells(1.6-4.1 V),demonstrating enormous application potential for sodium-ion batteries.展开更多
The concept of multi-principal component has created promising opportunities for the development of novel high-entropy ceramics for extreme environments encountered in advanced turbine engines, nuclear reactors, and h...The concept of multi-principal component has created promising opportunities for the development of novel high-entropy ceramics for extreme environments encountered in advanced turbine engines, nuclear reactors, and hypersonic vehicles, as it expands the compositional space of ceramic materials with tailored properties within a single-phase solid solution. The unique physical properties of some high-entropy carbides and borides, such as higher hardness, high-temperature strength, lower thermal conductivity, and improved irradiation resistance than the constitute ceramics, have been observed. These promising properties may be attributed to the compositional complexity, atomic-level disorder, lattice distortion, and other fundamental processes related to defect formation and phonon scattering.This manuscript serves as a critical review of the recent progress in high-entropy carbides and borides, focusing on synthesis and evaluations of their performance in extreme high-temperature, irradiation, and gaseous environments.展开更多
Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market.Here,an ultrahigh energy storage density of~13.8 J cm^(-3)and a large efficiency of~82.4%are achie...Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market.Here,an ultrahigh energy storage density of~13.8 J cm^(-3)and a large efficiency of~82.4%are achieved in high-entropy lead-free relaxor ferroelectrics by increasing configuration entropy,named high-entropy strategy,realizing nearly ten times growth of energy storage density compared with low-entropy material.Evolution of energy storage performance and domain structure with increasing configuration entropy is systematically revealed for the first time.The achievement of excellent energy storage properties should be attributed to the enhanced random field,decreased nanodomain size,strong multiple local distortions,and improved breakdown field.Furthermore,the excellent frequency and fatigue stability as well as charge/discharge properties with superior thermal stability are also realized.The significantly enhanced comprehensive energy storage performance by increasing configuration entropy demonstrates that high entropy is an effective but convenient strategy to design new high-performance dielectrics,promoting the development of advanced capacitors.展开更多
Sulfur element possesses an ultrahigh theoretical specific capacity,while the utilization of sulfur in the whole cathode is lower obviously owing to the sluggish kinetics of sulfur and discharged products,limiting the...Sulfur element possesses an ultrahigh theoretical specific capacity,while the utilization of sulfur in the whole cathode is lower obviously owing to the sluggish kinetics of sulfur and discharged products,limiting the enhancement on energy density of lithium-sulfur batteries.Herein,for the first time,Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy is introduced as the core catalytic host to activate the electrochemical performance of the sulfur cathode for lithium-sulfur batteries.It is manifested that Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy nanocrystallites distributed on nitrogen-doped carbon exhibit high electrocatalytic activity toward the conversion of solid sulfur to solid discharged products across soluble intermediate lithium polysulfides.In particular,benefiting from the accelerated kinetics by high-entropy alloy nanocrystallites and synergistic adsorption by nitrogen-doped carbon,the cathode exhibits high reversible capacity of 1079.5 mAh g_(-cathode)^(-1)(high utilization of 89.4%)with the whole cathode as active material,instead of sulfur element.Moreover,under both lean electrolyte(3μmg^(-1))and ultrahigh sulfur loading(27.0 mg cm^(-2))condition,the high discharge capacity of 868.2 mAh g_(-cathode)^(-1)can be still achieved for the sulfur cathode.This strategy opens up a new path to explore catalytic host materials for enhancing the utilization of sulfur in the whole cathode for lithium-sulfur batteries.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.52006074,52101255)Natural Science Foundation of Guangdong Province,China(Grant No.2021A1515010886)+2 种基金Youth science and technology innovation talent of Guangdong TeZhi planChina(Grant No.2019TQ05N068)the Fundamental Research Funds for the Central Universities,HUST:2021GCRC046
文摘The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added chemicals.Yet their complex molecular structures often require multiple active sites synergy for effective activation and achieving high chemoselectivity.Herein,it is reported that a high-entropy alloy(HEA)on high-entropy oxide(HEO)hetero-structured catalyst for highly active,chemoselective,and robust vanillin hydrodeoxygenation.The heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs(NiZnCuFeAlZrO_(x)),where exsolvable metals(e.g.,Ni,Zn,Cu)in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO matrix.This catalyst exhibits excellent catalytic performance:100%conversion of vanillin and 95%selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120℃,which were attributed to the synergistic effect among HEO matrix(with abundant oxygen vacancies),anchored HEA nanoparticles(having excellent hydrogenolysis capability),and their intimate hetero-interfaces(showing strong electron transferring effect).Therefore,our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion,which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.
基金the National Key R&D Program of China(No.2021YFB3701404)the National Natural Science Fund for Distinguished Young Scholars(No.52025041)+1 种基金the National Natural Science Foundation of China(Nos.52250091,51904021,and 52174294)the Fundamental Research Funds for the Central Universities(Nos.FRF-TP-20-02C2 and FRF-BD-22-05).
文摘Thermal insulation materials play an increasingly important role in protecting mechanical parts functioning at high temperatures.In this study,a new porous high-entropy(La_(1/6)Ce_(1/6)Pr_(1/6)Sm_(1/6)Eu_(1/6)Gd_(1/6))PO_(4)(HE(6RE_(1/6))PO_(4))ceramics was prepared by combining the high-entropy method with the pore-forming agent method and the effect of different starch contents(0–60vol%)on this ceramic properties was systematically investigated.The results show that the porous HE(6RE_(1/6))PO_(4)ceramics with 60vol%starch exhibit the lowest thermal conductivity of 0.061 W·m^(-1)·K^(-1)at room temperature and good pore structure stability with a linear shrinkage of approximately1.67%.Moreover,the effect of large regular spherical pores(>10μm)on its thermal insulation performance was discussed,and an optimal thermal conductivity prediction model was screened.The superior properties of the prepared porous HE(6RE_(1/6))PO_(4)ceramics allow them to be promising insulation materials in the future.
基金supported by the National Natural Science Foundation of China(No.52273280)the Creative Research Groups of China(No.51921001).
文摘High-entropy alloys(HEAs),which were introduced as a pioneering concept in 2004,have captured the keen interest of nu-merous researchers.Entropy,in this context,can be perceived as representing disorder and randomness.By contrast,elemental composi-tions within alloy systems occupy specific structural sites in space,a concept referred to as structure.In accordance with Shannon entropy,structure is analogous to information.Generally,the arrangement of atoms within a material,termed its structure,plays a pivotal role in dictating its properties.In addition to expanding the array of options for alloy composites,HEAs afford ample opportunities for diverse structural designs.The profound influence of distinct structural features on the exceptional behaviors of alloys is underscored by numer-ous examples.These features include remarkably high fracture strength with excellent ductility,antiballistic capability,exceptional radi-ation resistance,and corrosion resistance.In this paper,we delve into various unique material structures and properties while elucidating the intricate relationship between structure and performance.
基金the Swedish Foundation for International Cooperation in Research and Higher Education(STINT,Nos.IB2020-8781 and IB20229228)for the collaboration between KTH<U(Sweden),HYU(Korea),and NEU(China)VINNOVA(No.2022-01216),the SSF Strategic Mobility Grant(No.SM22-0039),the?Forsk(No.23-540),and the Swedish Steel Producers’Association(Jernkontoret),in particular,Axel Ax:-son Johnsons forskningsfond,Prytziska fondennr 2,Gerhard von Hofstens Stiftelse f?r Metallurgisk forskning,and Stiftelsen?veringenj?ren Gustaf Janssons Jernkontorsfond for the financial support.Key Lab of EPM(NEU)is acknowledged for supporting the partial FactSage calculation+2 种基金the Key Laboratory for Ferrous Metallurgy and Resources Utilization of the Min-istry of Education and Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steelmaking(No.FMRUlab-22-1)for supporting this researchThe Natural Science Foundation of Liaoning Province,China(No.2023MSBA-135)the Fundamental Research Funds for the Central Universities(No.N2409006)are also acknowledged。
文摘Specific grades of high-entropy alloys(HEAs)can provide opportunities for optimizing properties toward high-temperature applications.In this work,the Co-based HEA with a chemical composition of Co_(47.5)Cr_(30)Fe_(7.5)Mn_(7.5)Ni_(7.5)(at%)was chosen.The refractory metallic elements hafnium(Hf)and molybdenum(Mo)were added in small amounts(1.5at%)because of their well-known positive effects on high-temperature properties.Inclusion characteristics were comprehensively explored by using a two-dimensional cross-sectional method and extracted by using a three-dimensional electrolytic extraction method.The results revealed that the addition of Hf can reduce Al_(2)O_(3)inclusions and lead to the formation of more stable Hf-rich inclusions as the main phase.Mo addition cannot influence the inclusion type but could influence the inclusion characteristics by affecting the physical parameters of the HEA melt.The calculated coagulation coefficient and collision rate of Al_(2)O_(3)inclusions were higher than those of HfO_(2)inclusions,but the inclusion amount played a larger role in the agglomeration behavior of HfO_(2)and Al_(2)O_(3)inclusions.The impurity level and active elements in HEAs were the crucial factors affecting inclusion formation.
基金Project supported by the National Natural Science Foundation of China (Grant No.12272118)the National Key Research and Development Program of China (Grant No.2022YFE03030003)。
文摘The tension and compression of face-centered-cubic high-entropy alloy(HEA) nanowires are significantly asymmetric, but the tension–compression asymmetry in nanoscale body-centered-cubic(BCC) HEAs is still unclear. In this study,the tension–compression asymmetry of the BCC Al Cr Fe Co Ni HEA nanowire is investigated using molecular dynamics simulations. The results show a significant asymmetry in both the yield and flow stresses, with BCC HEA nanowire stronger under compression than under tension. The strength asymmetry originates from the completely different deformation mechanisms in tension and compression. In compression, atomic amorphization dominates plastic deformation and contributes to the strengthening, while in tension, deformation twinning prevails and weakens the HEA nanowire.The tension–compression asymmetry exhibits a clear trend of increasing with the increasing nanowire cross-sectional edge length and decreasing temperature. In particular, the compressive strengths along the [001] and [111] crystallographic orientations are stronger than the tensile counterparts, while the [110] crystallographic orientation shows the exactly opposite trend. The dependences of tension–compression asymmetry on the cross-sectional edge length, crystallographic orientation,and temperature are explained in terms of the deformation behavior of HEA nanowire as well as its variations caused by the change in these influential factors. These findings may deepen our understanding of the tension–compression asymmetry of the BCC HEA nanowires.
基金supported in part by the National Science Foundation(NSF)award#CMMI-1944040。
文摘We describe a novel mechanism for the synthesis of a stable high-entropy alloy powder from an otherwise immiscible Mg-Ti rich metallic mixture by employing high-energy mechanical milling.The presented methodology expedites the synthesis of amorphous alloy powder by strategically injecting entropic disorder through the inclusion of multi-principal elements in the alloy composition.Predictions from first principles and materials theory corroborate the results from microscopic characterizations that reveal a transition of the amorphous phase from a precursor intermetallic structure.This transformation,characterized by the emergence of antisite disorder,lattice expansion,and the presence of nanograin boundaries,signifies a departure from the precursor intermetallic structure.Additionally,this phase transformation is accelerated by the presence of multiple principal elements that induce severe lattice distortion and a higher configurational entropy.The atomic size mismatch of the dissimilar elements present in the alloy produces a stable amorphous phase that resists reverting to an ordered lattice even on annealing.
基金supported by Stability Supports Research Project of Treasury Department(No.197801)Talent Fund of CIAE(No.219213)。
文摘Experimental scratch tests and first-principles calculations were used to investigate the adhesion property of AlCrNbSiTi high-entropy alloy(HEA)coatings on zirconium substrates.AlCrNbSiTi HEA and Cr coatings were deposited on Zr alloy substrates using multi-arc ion plating technology,and scratch tests were subsequently conducted to estimate the adhesion property of the coatings.The results indicated that Cr coatings had better adhesion strength than HEA coatings,and the HEA coatings showed brittleness.The special quasi-random structure approach was used to build HEA models,and Cr/Zr and HEA/Zr interface models were employed to investigate the cohesion between the coatings and Zr substrate using first-principles calculations.The calculated interface energies showed that the cohesion between the Cr coating and the Zr substrate was stronger than that of the HEA coating with Zr.In contrary to Al or Si in the HEA coating,Cr,Nb,and Ti atoms binded strongly with Zr substrate.Based on the calculated elastic constants,it was found that low Cr and high Al content decreased the mechanical performances of HEA coatings.Finally,this study demonstrated the utilization of a combined approach involving first-principles calculations and experimental studies for future HEA coating development.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.52371203 and 52271192)the Ministry of Science and Technology of China(Grant No.2021YFB3501201)。
文摘Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass exhibited excellent magnetic refrigeration material with a wide temperature range and high refrigeration capacity(RC)was reported.Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass was observed with typical spin glass behavior around 15.5 K.In addition,we find that the magnetic entropy change(-△S_(M))originates from the sample undergoing a ferromagnetic(FM)to paramagnetic(PM)transition around 20 K.Under a field change from 0 T to 7 T,the value of maximum magnetic entropy change(-△S_(M)^(max))reaches 12.5 J/kg·K,and the corresponding value of RC reaches 487.7 J/kg in the temperature range from 6 K to 60 K.The large RC and wide temperature range make the Er_(20)Ho_(20)Dy_(20)Cu_(20)Ni_(20)high-entropy metallic glass be a promising material for application in magnetic refrigerators.
基金supported by the Office of Scientific Research of Shandong Vocational and Technical University of International Studies.
文摘This review focuses on thermodynamic and physical parameters,synthesis methods,and reported phases of Magnesium(Mg)containing high-entropy alloys(HEAs).Statistical data of publications concerning Mg-containing HEAs were collected and analyzed.Data on the chemical elements included in Mg-containing HEAs,their theoretical end experimental densities,thermodynamic parameters,physical parameters,fabricated techniques and reported phases were also collected and discussed.On the basis of this information,a new classification for HEAs was proposed.It is also shown that the existing thermodynamic parameters cannot accurately predict the formation of a single phase solid solution for Mg-containing HEAs.The physical parameters of Mg-containing HEAs are within a wide range,and most of the synthesized Mg-containing HEAs have a complex multiphase structure.
基金supported by the China Postdoctoral Science Foundation Project(2018M633650XB)Gansu Province Young Doctoral Fund Project(2021QB-043)the CNNC Operations Management Limited R&D Project(QS4FY-22003224)。
文摘AlCrCuFeMnx(x=0,0.5,1,1.5,and 2)high-entropy alloys were prepared using the vacuum arc melting technology.The microstructure and mechanical properties of AlCrCuFeMnxwere analyzed and tested by XRD,SEM,TEM,nanoindentation,and electronic universal testing.The results indicate that the AlCrCuFeMnxhigh-entropy alloy exhibits a dendritic structure,consisting of dendrites with a BCC structure,interdendrite regions with an FCC structure,and precipitates with an ordered BCC structure that form within the dendrite.Manganese(Mn)has a strong affinity for dendritic,interdendritic,and precipitate structures,allowing it to easily enter these areas.With an increase in Mn content,the size of the precipitated nanoparticles in the dendritic region initially increases and then decreases.Similarly,the area fraction initially decreases and then increases.Additionally,the alloy’s strength and wear resistance decrease,while its plasticity increases.The Al Cr Cu Fe Mn1.5alloy boasts excellent mechanical properties,including a hardness of 360 HV and a wear rate of 2.4×10^(-5)mm^(3)·N^(-1)·mm^(-1).It also exhibits impressive yield strength,compressive strength,and deformation rates of 960 MPa,1,700 MPa,and 27.5%,respectively.
基金support provided by the National Natural Science Foundation of China(Grant Nos.51972048,U23A20605)support provided by the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(Grant No.22567627H)the additional data in the revised manuscriptsupported by the National Key Research and Development Program of China(No.2022YFB3706300).
文摘High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.
基金Project support provided by the National Natural Science Foundation of China(Grant No.12075200)the National Key Research and Development Program of China(Grant No.2022YFB3706004)。
文摘A series of high-entropy alloys(HEAs) containing nanoprecipitates of varying sizes is successfully prepared by a non-consuming vacuum arc melting method.In order to study the irradiation evolution of helium bubbles in the FeCoNiCrbased HE As with γ' precipitates,these samples are irradiated by 100-keV helium ions with a fluence of 5 × 10^(20) ions/m^(2) at 293 K and 673 K,respectively.And the samples irradiated at room temperature are annealed at different temperatures to examine the diffusion behavior of helium bubbles.Transmission electron microscope(TEM) is employed to characterize the structural morphology of precipitated nanoparticles and the evolution of helium bubbles.Experimental results reveal that nanosized,spherical,dispersed,coherent,and ordered L1_(2)-type Ni_(3)Ti γ' precipitations are introduced into FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs by means of ageing treatments at temperatures between 1073 K and 1123 K.Under the ageing treatment conditions adopted in this work,γ' nanoparticles are precipitated in FeCoNiCr(Ni_(3)Ti)_(0.1) HE As,with average diameters of 15.80 nm,37.09 nm,and 62.50 nm,respectively.The average sizes of helium bubbles observed in samples after 673-K irradiation are 1.46 nm,1.65 nm,and 1.58 nm,respectively.The improvement in the irradiation resistance of FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs is evidenced by the diminution in bubbles size.Furthermore,the FeCoNiCr(Ni_(3)Ti)_(0.1) HEAs containing γ' precipitates of 15.8 nm exhibits the minimum size and density of helium bubbles,which can be ascribed to the considerable helium trapping effects of heterogeneous coherent phase boundaries.Subsequently,annealing experiments conducted after 293-K irradiation indicate that HEAs containing precipitated phases exhibits smaller apparent activation energy(E_(a)) for helium bubbles,resulting in larger helium bubble size.This study provides guidance for improving the irradiation resistance of L1_(2)-strengthened high-entropy alloy.
基金supported by the Yunnan Science and Technology Leading Talent Project(No.202305AB350005)National Science Foundation for Young Scientists of China(No.51404118).
文摘The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral resources.However,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to date.In addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation technology.In this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral surface.The homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain balance.The flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption decreases.According to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency and stability of the flotation reagents improves refractory mineral flotation.
基金supported by the Natural Science Foundation of China(61901142)the Key Research and Development Project of Hainan Province(ZDYF2022SHFZ093).
文摘Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prospects of high-entropy materials with high structural disorder and strong component controllability in the field of electrochemical energy storage,herein,a novel high-entropy garnet-type oxide solid electrolyte,Li_(5.75)Ga_(0.25)La_(3)Zr_(0.5)Ti_(0.5)Sn_(0.5)Nb_(0.5)O_(12)(LGLZTSNO)was constructed by partially replacing the Li and Zr sites in Li_(7)La_(3)Zr_(2)O_(12)with Ga and Ti/Sn/Nb elements,respectively.The experimental and density functional theory(DFT)calculation results show that the high-entropy LGLZTSNO electrolyte has preferable room temperature ion conductivity,air stability,interface contact performance with lithium anode,and the ability to suppress lithium dendrites.Thanks to the improvement of electrolyte performance,the critical current density of Li/Ag@LGLZTSNO/Li symmetric cell was increased from 0.42 to 1.57 mA cm^(−2),and the interface area specific impedance(IASR)was reduced from 765.2 to 42.3Ωcm^(2).Meanwhile,the Li/Ag@LGLZTSNO/LFP full cell also exhibits excellent rate performance and cycling performance(148 mA h g^(−1)at 0.1 C and 124 mA h g^(−1)at 0.5 C,capacity retention up to 84.8%after 100 cycles at 0.1 C),showing the application prospects of high-entropy LGLZTSNO solid electrolyte in high-performance all solid state lithium batteries.
基金the National Natural Science Foundation of China(Nos.51977185,51972277)the financial supported from Southwest Jiaotong University Science and Technology Rising Star Program(No.2682021CG021)
文摘lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance.Here we demonstrate the low-enthalpy and high-entropy(LEHE)electrolytes can intrinsically generate remarkably free ions and high mobility,enabling them to efficiently drive lithium-ion storage.The LEHE electrolytes are constructed on the basis of introducing CsPbl_(3)perovskite quantum dots(PQDs)to strengthen PEO@LiTFSI complexes.An extremely stable cycling>1000 h at 0.3 mA cm^(-2)can be delivered by LEHE electrolytes.Also,the as-developed Li|LEHE|LiFePO_(4)cell retains 92.3%of the initial capacity(160.7 mAh g^(-1))after 200 cycles.This cycling stability is ascribed to the suppressed charge concentration gradient leading to free lithium dendrites.It is realized by a dramatic increment in lithium-ion transference number(0.57 vs 0.19)and a significant decline in ion-transfer activation energy(0.14 eV vs 0.22 eV)for LEHE electrolytes comparing with PEO@LiTFSI counterpart.The CsPbl_(3)PQDs promote highly structural disorder by inhibiting crystallization and hence endow polymer electrolytes with low melting enthalpy and high structural entropy,which in turn facilitate long-term cycling stability and excellent rate-capability of lithium-metal batteries.
基金Project supported by the Natural Science Foundation of Jiangsu Province of China(Grant Nos.BK20220407 and BK20220428)。
文摘Since the superior mechanical,chemical and physical properties of high-entropy alloys(HEAs)were discovered,they have gradually become new emerging candidates for renewable energy applications.This review presents the novel applications of HEAs in thermoelectric energy conversion.Firstly,the basic concepts and structural properties of HEAs are introduced.Then,we discuss a number of promising thermoelectric materials based on HEAs.Finally,the conclusion and outlook are presented.This article presents an advanced understanding of the thermoelectric properties of HEAs,which provides new opportunities for promoting their applications in renewable energy.
基金financially supported by the National Key Research and Development Program of China (2022YFA1505700,2019YFA0210403)the National Natural Science Foundation of China (52102216)+1 种基金the Natural Science Foundation of Fujian Province (2022J01625,2022-S-002)the Innovation Training Program for College Students (202310394020,cxxl-2023097,cxxl-2024131,cxxl-2024136)。
文摘Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is realized by doping V^(3+)site with Ga^(3+)/Cr^(3+)/Al^(3+)/Fe^(3+)/In^(3+)simultaneously(i.e.Na_(3)V_(2-x)(GaCrAlFeIn)_x(PO_(4))_(3);x=0,0.04,0.06,and 0.08)to stimulate the V^(5+)■V^(2+)reversible multi-electron redox.Such configuration high-entropy can effectively suppress the structural collapse,enhance the redox reversibility in high working voltage(4.0 V),and optimize the electronic induced effect.The in-situ X-ray powder diffraction and in-situ electrochemical impedance spectroscopy tests efficaciously confirm the robust structu ral recovery and far lower polarization throughout an entire charge-discharge cycle during 1.6-4.3 V,respectively.Moreover,the density functional theory calculations clarify the stronger metallicity of high-entropy electrode than the bare that is derived from the more mobile free electrons surrounding the vicinity of Fermi level.By grace of high-entropy design and multi-electron transfer reactions,the optimal Na_(3)V_(1.7)(GaCrAlFeIn)_(0.06)(PO_(4))_(3)can exhibit perfect cycling/rate performances(90.97%@5000 cycles@30 C;112 mA h g^(-1)@10 C and 109 mA h g^(-1)@30 C,2.0-4.3 V).Furthermore,it can supply ultra-high185 mA h g^(-1)capacity with fa ntastic energy density(522 W h kg^(-1))in half-cells(1.4-4.3 V),and competitive capacity(121 mA h g^(-1))as well as energy density(402 W h kg^(-1))in full-cells(1.6-4.1 V),demonstrating enormous application potential for sodium-ion batteries.
基金funded in part by the Advanced Research Projects Agency-Energy (ARPA-E), U.S. Department of Energy, under Award Number DE-AR0001428supported by the National Science Foundation under Award ECCS: 2025298the Nebraska Research Initiative。
文摘The concept of multi-principal component has created promising opportunities for the development of novel high-entropy ceramics for extreme environments encountered in advanced turbine engines, nuclear reactors, and hypersonic vehicles, as it expands the compositional space of ceramic materials with tailored properties within a single-phase solid solution. The unique physical properties of some high-entropy carbides and borides, such as higher hardness, high-temperature strength, lower thermal conductivity, and improved irradiation resistance than the constitute ceramics, have been observed. These promising properties may be attributed to the compositional complexity, atomic-level disorder, lattice distortion, and other fundamental processes related to defect formation and phonon scattering.This manuscript serves as a critical review of the recent progress in high-entropy carbides and borides, focusing on synthesis and evaluations of their performance in extreme high-temperature, irradiation, and gaseous environments.
基金supported by the National Natural Science Foundation of China(Grant Nos.21825102,22235002,52172181,and 22105017)Key R&D Plan of the Ministry of Science and Technology of China(Grant No.2022YFB3204000)。
文摘Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market.Here,an ultrahigh energy storage density of~13.8 J cm^(-3)and a large efficiency of~82.4%are achieved in high-entropy lead-free relaxor ferroelectrics by increasing configuration entropy,named high-entropy strategy,realizing nearly ten times growth of energy storage density compared with low-entropy material.Evolution of energy storage performance and domain structure with increasing configuration entropy is systematically revealed for the first time.The achievement of excellent energy storage properties should be attributed to the enhanced random field,decreased nanodomain size,strong multiple local distortions,and improved breakdown field.Furthermore,the excellent frequency and fatigue stability as well as charge/discharge properties with superior thermal stability are also realized.The significantly enhanced comprehensive energy storage performance by increasing configuration entropy demonstrates that high entropy is an effective but convenient strategy to design new high-performance dielectrics,promoting the development of advanced capacitors.
基金Financial support from National Natural Science Foundation of China(21935006)is gratefully acknowledged。
文摘Sulfur element possesses an ultrahigh theoretical specific capacity,while the utilization of sulfur in the whole cathode is lower obviously owing to the sluggish kinetics of sulfur and discharged products,limiting the enhancement on energy density of lithium-sulfur batteries.Herein,for the first time,Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy is introduced as the core catalytic host to activate the electrochemical performance of the sulfur cathode for lithium-sulfur batteries.It is manifested that Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy nanocrystallites distributed on nitrogen-doped carbon exhibit high electrocatalytic activity toward the conversion of solid sulfur to solid discharged products across soluble intermediate lithium polysulfides.In particular,benefiting from the accelerated kinetics by high-entropy alloy nanocrystallites and synergistic adsorption by nitrogen-doped carbon,the cathode exhibits high reversible capacity of 1079.5 mAh g_(-cathode)^(-1)(high utilization of 89.4%)with the whole cathode as active material,instead of sulfur element.Moreover,under both lean electrolyte(3μmg^(-1))and ultrahigh sulfur loading(27.0 mg cm^(-2))condition,the high discharge capacity of 868.2 mAh g_(-cathode)^(-1)can be still achieved for the sulfur cathode.This strategy opens up a new path to explore catalytic host materials for enhancing the utilization of sulfur in the whole cathode for lithium-sulfur batteries.