FeNi-based MGs exhibit the most excellent room-temperature mechanical properties among different Fe-based metallic glasses(MGs)systems.However,the glass-forming ability(GFA)of FeNi-based MGs is much lower than that of...FeNi-based MGs exhibit the most excellent room-temperature mechanical properties among different Fe-based metallic glasses(MGs)systems.However,the glass-forming ability(GFA)of FeNi-based MGs is much lower than that of their counterparts.Thus,uncovering the solidification and anomalous nano-crystallization behavior of FeNi-based MGs is crucial to the development of FeNibased bulk metallic glasses with larger plasticity and critical size concurrently.Regarding this,a combination of complementary in situ synchrotron radiation high-energy X-ray diffraction,small-angle neutron scattering(SANS),and 3-dimentional atom probe tomography(3-D APT)is used to study solidification and nano-crystallization behavior of Fe_(48)Ni_(30)Mo_(3)B_(19)liquid and MG.The time–temperature–transformation diagram was successfully depicted via melting spun,in situ solidification,and isothermal annealing methods.We found that the Fe_(48)Ni_(30)Mo_(3)B_(19)MG can only be prepared via the meltspinning method to obtain amorphous ribbons,which could contribute to the low activation energy for the nano-crystallization growth E_(p).Moreover,during isothermal annealing,the anomalous slow growth behavior in kinetic of theγ-FeNi phase embedded in the amorphous matrix is caused by the Fe and Ni partitioning,and the Mo-enriched region around the nanosizedγ-FeNi phase,which is revealed by 3-D APT.These results exhibit a new perspective for understanding the relationship between GFA and nano-crystallization behavior and provide feasible guidance for the development of newγ-FeNi-containing Fe-based BMG composites with desired mechanical properties and GFA.展开更多
Ms-T curves and hysteresis loops were investigated for amorphous Fe78Si9B13, (FeNi)78(CrSiB)22, their lap-wound-cores, and their composite ribbons made by two-chamber-crucible technique. The properties of the lap-woun...Ms-T curves and hysteresis loops were investigated for amorphous Fe78Si9B13, (FeNi)78(CrSiB)22, their lap-wound-cores, and their composite ribbons made by two-chamber-crucible technique. The properties of the lap-wound cores of the two kinds of ribbons are similar. For the composite ribbons, the intrinsic properties are the average of the two alloys. Their technological properties, i.e., hysteresis loops, however, are no longer the average of the two alloys. Instead, they show some dramatic changes compared to the lap-wound-cores. Especially, the shape of the hysteresis loop of the composite ribbon cores is largely different from that of lap-wound-cores. The reason for the difference is supposed to be internal stress induced from cooling after annealing.展开更多
The magnetic properties and anisotropy of amor- phous(Fe_(80)Ni_(20))_(78)Si_xB_(22-x).alloys have been investigated systematically.The maximum permeability,coercive force and remanence have been determined for as-pre...The magnetic properties and anisotropy of amor- phous(Fe_(80)Ni_(20))_(78)Si_xB_(22-x).alloys have been investigated systematically.The maximum permeability,coercive force and remanence have been determined for as-prepared and annealed samples,The results on the technical magnetic properties of this alloy system have been discussed and compared with Masumoto's.展开更多
L1_(0)-FeNi hard magnetic alloy with coercivity reaching 861 Oe was synthesized through annealing Fe_(42)Ni_(41.3)Si_8 B_(4)P_(4)Cu_(0.7)amorphous alloy,and the L1_(0)-FeNi formation mechanism has been studied.It is f...L1_(0)-FeNi hard magnetic alloy with coercivity reaching 861 Oe was synthesized through annealing Fe_(42)Ni_(41.3)Si_8 B_(4)P_(4)Cu_(0.7)amorphous alloy,and the L1_(0)-FeNi formation mechanism has been studied.It is found the L1_(0)-FeNi in annealed samples at 400℃mainly originated from the residual amorphous phase during the second stage of crystallization which could take place over 600 C lower than the measured onset temperature of the second stage with a50 C/min heating rate.Annealing at 4000 C after fully crystallization still caused a slight increase of coercivity,which was probably contributed by the limited transformation from other high temperature crystalline phases towards L1_(0)phase,or the removal of B from L1_(0)lattice and improvement of the ordering quality of L1_(0)phase due to the reduced temperature from520℃to 400℃.The first stage of crystallization has hardly direct contribution to L1_(0)-FeNi formation.Ab initio simulations show that the addition of Si or Co in L1_(0)-FeNi has the effect of enhancing the thermal stability of L1_(0)phase without seriously deteriorating its magnetic hardness.The non-monotonic feature of direction dependent coercivity in ribbon segments resulted from the combination of domain wall pinning and demagnetization effects.The approaches of synthesizing L1_(0)-FeNi magnets by adding Si or Co and decreasing the onset crystallization temperature have been discussed in detail.展开更多
The morbidity rate of primary cardiac tumors(PCTs)is only 0.0138%.[1]Calcified amorphous tumors(CATs)are a particularly rare entity with only a few cases reported in the literature,and account for only 2.47%of PCTs.[2...The morbidity rate of primary cardiac tumors(PCTs)is only 0.0138%.[1]Calcified amorphous tumors(CATs)are a particularly rare entity with only a few cases reported in the literature,and account for only 2.47%of PCTs.[2]CATs can occur at any age and have been identified at various intracardiac locations.The clinical manifestations of patients are related to the location and size of the lesion.展开更多
Photoelectrochemical seawater splitting is promising for renewable hydrogen,yet severe chloride corrosion remains a roadblock.Although amorphous catalysts improve hematite(α-Fe_(2)O_(3))photoanode activity,their defe...Photoelectrochemical seawater splitting is promising for renewable hydrogen,yet severe chloride corrosion remains a roadblock.Although amorphous catalysts improve hematite(α-Fe_(2)O_(3))photoanode activity,their defect-enabled functionality inherently accelerates structural degradation,exacerbating chloride-induced corrosion.Here,a synergistic dual-functional nano-armor is designed by anchoring phosphate(PO_(4)^(3-))to active sites on amorphous NiMoO_(4)(a-NiMoO_(4)@PO_(4)^(3-)),achieving dual activitystability enhancement.Detailed physicochemical characterization and density functional theory(DFT)calculations show that the successful and stable anchoring of phosphate is highly dependent on the amorphous structural properties of a-NiMoO_(4).Its rich disordered coordination environment provides sufficient highly reactive sites,allowing PO_(4)^(3-)to be firmly bound through strong coordination bonds,which is the key for the dual role of PO_(4)^(3-)coordination.As a dynamic Cl-shield,PO_(4)^(3-)coordinates unsaturated Ni sites,forming an anionic layer that resists Cl-via steric-electrostatic blocking.As an electronic modulator,PO_(4)^(3-)triggers metal-to-ligand charge transfer at Ni sites,depleting electron density to optimize the intermediate adsorption of oxygen evolution reaction(OER)and reduce kinetic barriers.Simultaneously,this charge redistribution induces a built-in electric field that accelerates holeselective transport.Benefiting from these dual effects,the Fe_(2)O_(3)/a-NiMoO_(4)@PO_(4)^(3-)achieves 4 mA cm^(-2)at 1.23 V_(RHE) with exceptional stability in seawater.This work leverages the unique coordination flexibility of amorphous structures to construct a phosphate-coordinated bifunctional nano-armor on hematite photoanodes,which simultaneously enables efficient chloride exclusion and electronic structure optimization.The synergistic mechanism,rooted in strong phosphate anchoring on amorphous carriers,establishes a new design paradigm for photoelectrochemical systems that integrate high activity with extreme environmental stability,providing an efficient pathway toward corrosion-resistant seawater splitting.展开更多
High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environm...High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.展开更多
Recent advances in geoscience have underscored the critical role of abiogenic processes in petroleum formation,especially the formation and polymerization of methane.However,whether a direct carbon-H_(2) reaction can ...Recent advances in geoscience have underscored the critical role of abiogenic processes in petroleum formation,especially the formation and polymerization of methane.However,whether a direct carbon-H_(2) reaction can produce C_(2+)hydrocarbons(e.g.,ethane and propane)beyond methane remains an open question.Here,we demonstrate the direct synthesis of ethane and propane via reactions between amorphous carbon and H_(2) under upper mantle conditions(2-10 GPa and 800-1200℃).A systematic investigation reveals that increasing structural disorder in carbon precursors,from graphite to glassy carbon-Ⅱ and carbon black,enhances the production of C_(2)-C_(3) hydrocarbons.Through integrated X-ray diffraction and reverse Monte Carlo simulations,we establish that the continuous random atomic network structures in amorphous carbon enable one-step synthesis of heavy hydrocarbons with H_(2).These models establish a direct link between atomic-scale carbon structures and the one-step synthesis of C_(2+) hydrocarbons under H_(2)-rich,high-pressure,and high-temperature conditions—potentially revealing an efficient mechanism for the abiotic production of C_(2+) hydrocarbons in the upper mantle.展开更多
Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)e...Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)encapsulated in nitrogen-doped carbon shells(A-Ni@NC)via pulsed laser ablation in liquid(PLAL).The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm^(-2)in 1.0 m KOH.Furthermore,the bifunctional catalyst achieved a current density of 10 mA cm^(-2)at 1.63 V and retained 98.9%of its initial performance after 100 h of operation.The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport.Density functional theory(DFT)calculations revealed that N-doping optimized intermediate adsorption energies,while the amorphous Ni core facilitated efficient electron transfer.This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.展开更多
Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior perf...Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior performance of amorphous CuNi alloys for CO_(2)electrochemical reduction.By integrating machine learning forcefields for efficient structure generation and density functional theory for subsequent structural refinement and property calculations,we reveal the potential of these disordered systems to outperform their crystalline counterparts.Machine learning forcefields can generate a bulk structure containing a mixture of Cu and Ni atoms,resulting in enhanced catalytic performance.Effective screening of the amorphous surfaces is used to identify undercoordinated Cu and Ni sites in the amorphous structure to synergistically promote selective CO production and favor ethanol formation over ethylene via the stabilization of the*COCHO intermediate,resulting in significantly lower Gibbs free energy changes compared to the crystalline counterpart.The varying atomic coordination environments on amorphous surfaces promote both C–C bond formation and subsequent proton-electron transfer,leading to ethanol formation.These findings demonstrate the superior catalytic performance of amorphous CuNi,highlighting its potential for efficient and selective electroreduction of CO_(2).展开更多
Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy ...Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.展开更多
The introduction of two-dimensional(2D)perovskite layers on top of three-dimensional(3D)perovskite films enhances the performance and stability of perovskite solar cells(PSCs).However,the electronic effect of the spac...The introduction of two-dimensional(2D)perovskite layers on top of three-dimensional(3D)perovskite films enhances the performance and stability of perovskite solar cells(PSCs).However,the electronic effect of the spacer cation and the quality of the 2D capping layer are critical factors in achieving the required results.In this study,we compared two fluorinated salts:4-(trifluoromethyl)benzamidine hydrochloride(4TF-BA·HCl)and 4-fluorobenzamidine hydrochloride(4F-BA·HCl)to engineer the 3D/2D perovskite films.Surprisingly,4F-BA formed a high-performance 3D/2D heterojunction,while4TF-BA produced an amorphous layer on the perovskite films.Our findings indicate that the balanced intramolecular charge polarization,which leads to effective hydrogen bonding,is more favorable in 4F-BA than in 4TF-BA,promoting the formation of a crystalline 2D perovskite.Nevertheless,4TF-BA managed to improve efficiency to 24%,surpassing the control device,primarily due to the natural passivation capabilities of benzamidine.Interestingly,the devices based on 4F-BA demonstrated an efficiency exceeding 25%with greater longevity under various storage conditions compared to 4TF-BA-based and the control devices.展开更多
In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strat...In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strategy utilizing high-electronegativity N(χ=3.04)to modulate local electronic domains and stabilize amorphous Mo–Se coordination(N/Mo-Se).Through self-polymerization and tunable selenization,N-doped carbon(NC)nanospheres encapsulating N-stabilized amorphous Mo-Se clusters(N/Mo-Se@NC)are successfully constructed.Theoretical and experimental analyses reveal that N-optimization effectively reconstructs the electronic distribution of Mo–Se coordination via strong covalent Mo–N bonds.This significantly enhances the covalency of Mo-Se clusters and induces localized electronic domains,thereby substantially suppressing polyselenide dissolution/shuttle during cycling.Concurrently,the amorphous N/Mo-Se clusters provide isotropic ion diffusion pathways,and together with the threedimensional(3D)conductive networks of the NC,they jointly optimize charge transfer kinetics.The N/Mo-Se@NC anode exhibits a high reversible capacity of 328.7 mAh g^(-1)after 5000 cycles,even at 10.0 A g^(-1),with a remarkable capacity retention of 110%.The assembled N/Mo-Se@NC//AC SIHCs achieve high energy/power densities(236.1 Wh kg^(-1)/9990 W kg^(-1)),demonstrating superior comprehensive performance compared to most previously reported anodes.This study,through high-electronegativity atom modulation and amorphization engineering,opens new avenues for designing highly stable and high-rate Na^(+) storage materials.展开更多
Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphou...Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).展开更多
Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improv...Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improved mass transfer and stability.Herein,self-supported crystalline/amorphous NiO/Ni(OH)_(2)nanosheet arrays on nickel foam(NF)are fabricated via an in-situ dissolution-deposition hydrothermal growing of Ni(OH)_(2)nanosheets without additional metal sources assisted by a common Lewis base,EDTA,followed by a rapid calcination at 300℃in air.The as-prepared EDTA-NF-12 h exhibits high OER and HER performance under alkaline conditions,requiring 235 mV and 158 mV,respectively,to reach 10 mA cm^(-2),and the decent performance can be maintained for 24 h without obvious degradation.The dual interfaces,i.e.,the dense crystalline/amorphous interfaces within the NiO/Ni(OH)_(2)nanosheet arrays,as well as the intimate interfaces between nanoarrays and NF,both serve as reaction active sites,facilitate electron transfer,and endow the catalyst with high activity and stability.Furthermore,by applying EDTA-Ni^(2+)and other Lewis bases with varying basicities instead of EDTA,the interfaces with the NF substrate are found to promote the formation of crystalline/amorphous interfaces within the nanosheets.This study offers appealing opportunities for tailoring the electrocatalytic performance of self-supported electrodes via dual interface engineering.展开更多
Guided bone regeneration in the alveolar bone relies on the colonization and differentiation of immune cells within the defect area.The absence of osteoinductive and osteoimmune properties of currently available scaff...Guided bone regeneration in the alveolar bone relies on the colonization and differentiation of immune cells within the defect area.The absence of osteoinductive and osteoimmune properties of currently available scaffolds hinders to achieve optimal repair outcomes in clinical settings.Thus,we aimed to enhance the bone repair ability of polycaprolactone(PCL)scaffolds by incorporating osteoinductive amorphous calcium phosphate(ACP)with immune-regulating zinc ions(ACP(Zn),ACZP),to create a favorable immunomodulatory microenvironment.After one day of co-culture with PCL-ACZP,the spreading area of macrophage cells was significantly higher than that from the original PCL scaffold.Additionally,over 32.1%of macrophages exhibited M2 polarization within three days of co-culture.The PCLACZP/macrophage-conditioned medium significantly boosted osteogenic gene expression in MC3T3-E1 cells.After eight weeks of implantation in a rat femoral condyle defect,the BV/TV from the PCL-ACZP group reached 32.9%,1.4 times of that from the PCL group.Furthermore,the PCL-ACZP-GelMA biphasic module as prepared successfully achieved complete regeneration of three-walled alveolar bone defects in rabbits,resulting in arch-shaped alveolar bone repair and providing greater convenience in the clinical settings.This study showcased the effectiveness of PCL-ACZP-GelMA biphasic module as bioactive scaffolds in the morphological restoration of alveolar bone.展开更多
The unique high-entropy and sluggish diffusion effects of amorphous high-entropy alloys endow them with excellent thermal stability and plastic deformation.In this work,the near-equiatomic TaTiZr amorphous medium-entr...The unique high-entropy and sluggish diffusion effects of amorphous high-entropy alloys endow them with excellent thermal stability and plastic deformation.In this work,the near-equiatomic TaTiZr amorphous medium-entropy alloy(AMEA)was prepared via the magnetron sputtering to investigate the microstructural thermostability and nanoindentation creep behavior.Thermal annealing below the glass transition temperature gave rise to the microstructural heterogeneity due to the positive mixing enthalpy in TaTiZr AMEA,which became increasingly enhanced with raising the annealing temperature.Correspondingly,there appeared a monotonic increase in hardness as well as the elastic/shear modulus,yet a reduction in strain-rate sensitivity m or an increment in shear transformation zone volume with annealing temperature.Meanwhile,the indentation morphology measured by atomic force microscope exhibited a significant transformation from pile-up to sink-in,demonstrating the degradation of plastic deformability with enhancing the microstructural heterogeneity.Based on the relaxation time spectra for Maxwell-Voigt model,the microstructural heterogeneity can restrain the activation of internal defects associated with the operation of flow units during creeping,further triggering the strain-strengthening behavior and improved creep resistance in the annealed samples.This work provides significant guidance for the structural design of high-performance amorphous alloys.展开更多
Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain si...Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain size,microstructural stability,and hydrogen storage properties.Crystallization kinetics,along with in-situ high-energy XRD characterization,revealed a concentrated and synchronous crystallization of Mg_(2)Ni and RE-Mg-Ni ternary phases with the increase in La and Ni content.The attributed synchronous crystallization process was found to be a result of the close local affinity of Mg_(2)Ni and RE-Mg-Ni ternary phases,as assessed by the thermodynamic Miedema model.Significant secondary phase pinning effect,arising from the high likelihood of well-matching phase structures between Mg_(2)Ni,LaMg_(2)Ni,and LaMgNi_(4),was validated through both the edge-to-edge matching model prediction and experimental observation.Thefine and homogeneous microstructure was shown to be a consequence of fast crystallization kinetics and the secondary phase pinning effect.Improved activation performance and cycling stability were observed,stemming from grain refinement and excellent microstructural stability.Our study provides insights into mechanism of grain refinement of nanocrystalline microstructure tailored by phase constitution and crystallization kinetics in the amorphous-crystallization route.We also demonstrate the potential of material design guided by phase equilibria and crystallographic predictions to improve nanocrystalline with excellent microstructural stability.展开更多
Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling...Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling SLCO.However,due to the presence of cobalt oxide with a spinel phase on the surface of highly-degraded LCO,the strong electrostatic repulsion from the transition metal octahedron poses a high Li replenishment barrier,making the regeneration of highly-degraded LCO a challenge.Herein,we propose a structural transformation strategy for reconstructing Li replenishment channels to aid the direct regeneration of highly-degraded LCO.In this approach,ball milling is employed to disrupt the inherent structure of highly-degraded LCO,thereby releasing the internal stress and converting the surface spinel phase into a homogeneous amorphous structure,which promotes Li insertion and regeneration.The regenerated LCO(RLCO)exhibits an outstanding discharge capacity of 179.10 mAh·g^(−1) in the voltage range of 3.0–4.5 V at 0.5 C.The proposed strategy is an effective regeneration approach for highly-degraded LCO,thereby facilitating the efficient recycling of spent lithium-ion battery cathode materials.展开更多
In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment techni...In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.展开更多
基金financially supported by the National Key R&D Program of China(No.2022YFA1603801)the Open Fund of the Science and Technology on Metrology and Calibration Laboratory(No.JLKG2023001C004)+6 种基金the National Natural Science Foundation of China(Nos.52130108,52301213,52071024,52271003,and 52101188)Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515110805,2021B1515140028,and 2021CX02C087)the Open Fund of the China Spallation Neutron Source Songshan Lake Science City(No.KFKT2023B11)Construction of a Coordination Network for Science and Technology Assistance to Latin American Countries(Science and Technology Partnership Program,Ministry of Science and Technology of China,No.KY202401006)the Youth Innovation Promotion Association,CAS(No.2020010)the State Key Lab of Advanced Metals and Materials(No.2022-ZD01)the SSRF proposal(No.2024-SSRF-PT-506766)
文摘FeNi-based MGs exhibit the most excellent room-temperature mechanical properties among different Fe-based metallic glasses(MGs)systems.However,the glass-forming ability(GFA)of FeNi-based MGs is much lower than that of their counterparts.Thus,uncovering the solidification and anomalous nano-crystallization behavior of FeNi-based MGs is crucial to the development of FeNibased bulk metallic glasses with larger plasticity and critical size concurrently.Regarding this,a combination of complementary in situ synchrotron radiation high-energy X-ray diffraction,small-angle neutron scattering(SANS),and 3-dimentional atom probe tomography(3-D APT)is used to study solidification and nano-crystallization behavior of Fe_(48)Ni_(30)Mo_(3)B_(19)liquid and MG.The time–temperature–transformation diagram was successfully depicted via melting spun,in situ solidification,and isothermal annealing methods.We found that the Fe_(48)Ni_(30)Mo_(3)B_(19)MG can only be prepared via the meltspinning method to obtain amorphous ribbons,which could contribute to the low activation energy for the nano-crystallization growth E_(p).Moreover,during isothermal annealing,the anomalous slow growth behavior in kinetic of theγ-FeNi phase embedded in the amorphous matrix is caused by the Fe and Ni partitioning,and the Mo-enriched region around the nanosizedγ-FeNi phase,which is revealed by 3-D APT.These results exhibit a new perspective for understanding the relationship between GFA and nano-crystallization behavior and provide feasible guidance for the development of newγ-FeNi-containing Fe-based BMG composites with desired mechanical properties and GFA.
文摘Ms-T curves and hysteresis loops were investigated for amorphous Fe78Si9B13, (FeNi)78(CrSiB)22, their lap-wound-cores, and their composite ribbons made by two-chamber-crucible technique. The properties of the lap-wound cores of the two kinds of ribbons are similar. For the composite ribbons, the intrinsic properties are the average of the two alloys. Their technological properties, i.e., hysteresis loops, however, are no longer the average of the two alloys. Instead, they show some dramatic changes compared to the lap-wound-cores. Especially, the shape of the hysteresis loop of the composite ribbon cores is largely different from that of lap-wound-cores. The reason for the difference is supposed to be internal stress induced from cooling after annealing.
文摘The magnetic properties and anisotropy of amor- phous(Fe_(80)Ni_(20))_(78)Si_xB_(22-x).alloys have been investigated systematically.The maximum permeability,coercive force and remanence have been determined for as-prepared and annealed samples,The results on the technical magnetic properties of this alloy system have been discussed and compared with Masumoto's.
基金supported by the National Natural Science Foundation of China(Grant Nos.51971179 and 51971180)the Natural Science Foundation of Chongqing,China(Grant No.cstc2019jcyj-msxmX0328)+3 种基金Shaanxi Provincial Natural Science Foundation,China(Grant No.2020JM-112)Guangdong Provincial Science and Technology Program,China(Grant No.2019B090905009)the Fundamental Research Funds for the Central Universities of China(Grant No.D5000210731)Shaanxi Provincial Key R&D Program,China(Grant No.2021KWZ-13)。
文摘L1_(0)-FeNi hard magnetic alloy with coercivity reaching 861 Oe was synthesized through annealing Fe_(42)Ni_(41.3)Si_8 B_(4)P_(4)Cu_(0.7)amorphous alloy,and the L1_(0)-FeNi formation mechanism has been studied.It is found the L1_(0)-FeNi in annealed samples at 400℃mainly originated from the residual amorphous phase during the second stage of crystallization which could take place over 600 C lower than the measured onset temperature of the second stage with a50 C/min heating rate.Annealing at 4000 C after fully crystallization still caused a slight increase of coercivity,which was probably contributed by the limited transformation from other high temperature crystalline phases towards L1_(0)phase,or the removal of B from L1_(0)lattice and improvement of the ordering quality of L1_(0)phase due to the reduced temperature from520℃to 400℃.The first stage of crystallization has hardly direct contribution to L1_(0)-FeNi formation.Ab initio simulations show that the addition of Si or Co in L1_(0)-FeNi has the effect of enhancing the thermal stability of L1_(0)phase without seriously deteriorating its magnetic hardness.The non-monotonic feature of direction dependent coercivity in ribbon segments resulted from the combination of domain wall pinning and demagnetization effects.The approaches of synthesizing L1_(0)-FeNi magnets by adding Si or Co and decreasing the onset crystallization temperature have been discussed in detail.
文摘The morbidity rate of primary cardiac tumors(PCTs)is only 0.0138%.[1]Calcified amorphous tumors(CATs)are a particularly rare entity with only a few cases reported in the literature,and account for only 2.47%of PCTs.[2]CATs can occur at any age and have been identified at various intracardiac locations.The clinical manifestations of patients are related to the location and size of the lesion.
基金supported by the Shandong Provincial Natural Science Foundation(No.ZR2022ME052)the National Natural Science Foundation of China(No.22404153)+4 种基金the TaiShan Scholars of Shandong China(No.tsqn202306113 and tsqn202408081)the Excellent Youth Science Fund Project of Shandong China(No.2025HWYQ-032)the China Postdoctoral Science Foundation(No.2024M753044)the Postdoctoral Fellowship Program of CPSF(No.GZB20240693)the Natural Science Foundation of Qingdao(No.24-4-4-zrjj-9-jch)。
文摘Photoelectrochemical seawater splitting is promising for renewable hydrogen,yet severe chloride corrosion remains a roadblock.Although amorphous catalysts improve hematite(α-Fe_(2)O_(3))photoanode activity,their defect-enabled functionality inherently accelerates structural degradation,exacerbating chloride-induced corrosion.Here,a synergistic dual-functional nano-armor is designed by anchoring phosphate(PO_(4)^(3-))to active sites on amorphous NiMoO_(4)(a-NiMoO_(4)@PO_(4)^(3-)),achieving dual activitystability enhancement.Detailed physicochemical characterization and density functional theory(DFT)calculations show that the successful and stable anchoring of phosphate is highly dependent on the amorphous structural properties of a-NiMoO_(4).Its rich disordered coordination environment provides sufficient highly reactive sites,allowing PO_(4)^(3-)to be firmly bound through strong coordination bonds,which is the key for the dual role of PO_(4)^(3-)coordination.As a dynamic Cl-shield,PO_(4)^(3-)coordinates unsaturated Ni sites,forming an anionic layer that resists Cl-via steric-electrostatic blocking.As an electronic modulator,PO_(4)^(3-)triggers metal-to-ligand charge transfer at Ni sites,depleting electron density to optimize the intermediate adsorption of oxygen evolution reaction(OER)and reduce kinetic barriers.Simultaneously,this charge redistribution induces a built-in electric field that accelerates holeselective transport.Benefiting from these dual effects,the Fe_(2)O_(3)/a-NiMoO_(4)@PO_(4)^(3-)achieves 4 mA cm^(-2)at 1.23 V_(RHE) with exceptional stability in seawater.This work leverages the unique coordination flexibility of amorphous structures to construct a phosphate-coordinated bifunctional nano-armor on hematite photoanodes,which simultaneously enables efficient chloride exclusion and electronic structure optimization.The synergistic mechanism,rooted in strong phosphate anchoring on amorphous carriers,establishes a new design paradigm for photoelectrochemical systems that integrate high activity with extreme environmental stability,providing an efficient pathway toward corrosion-resistant seawater splitting.
基金supported by the Australian Research Council(ARC)Projects(DP220101139,DP220101142,and LP240100542).
文摘High‐entropy amorphous catalysts(HEACs)integrate multielement synergy with structural disorder,making them promising candidates for water splitting.Their distinctive features—including flexible coordination environments,tunable electronic structures,abundant unsaturated active sites,and dynamic structural reassembly—collectively enhance electrochemical activity and durability under operating conditions.This review summarizes recent advances in HEACs for hydrogen evolution,oxygen evolution,and overall water splitting,highlighting their disorder-driven advantages over crystalline counterparts.Catalytic performance benchmarks are presented,and mechanistic insights are discussed,focusing on how multimetallic synergy,amorphization effect,and in‐situ reconstruction cooperatively regulate reaction pathways.These insights provide guidance for the rational design of next‐generation amorphous high‐entropy electrocatalysts with improved efficiency and durability.
基金mainly supported by the Natural Science Foundation of China (Grant Nos. 52288102, 52090020, and 52372261)the Natural Science Foundation of Hebei Province (Grant No. E202403045)+1 种基金the S&T Program of Hebei (Grant No. 225A1102D)the Ministry of Education Chang Jiang Scholar Professor Program (Grant No. T2022241)
文摘Recent advances in geoscience have underscored the critical role of abiogenic processes in petroleum formation,especially the formation and polymerization of methane.However,whether a direct carbon-H_(2) reaction can produce C_(2+)hydrocarbons(e.g.,ethane and propane)beyond methane remains an open question.Here,we demonstrate the direct synthesis of ethane and propane via reactions between amorphous carbon and H_(2) under upper mantle conditions(2-10 GPa and 800-1200℃).A systematic investigation reveals that increasing structural disorder in carbon precursors,from graphite to glassy carbon-Ⅱ and carbon black,enhances the production of C_(2)-C_(3) hydrocarbons.Through integrated X-ray diffraction and reverse Monte Carlo simulations,we establish that the continuous random atomic network structures in amorphous carbon enable one-step synthesis of heavy hydrocarbons with H_(2).These models establish a direct link between atomic-scale carbon structures and the one-step synthesis of C_(2+) hydrocarbons under H_(2)-rich,high-pressure,and high-temperature conditions—potentially revealing an efficient mechanism for the abiotic production of C_(2+) hydrocarbons in the upper mantle.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(NRF-2023R1A2C1005419).
文摘Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites.Herein,we report a one-step,surfactant-free synthesis of amorphous nickel nanoparticles(NPs)encapsulated in nitrogen-doped carbon shells(A-Ni@NC)via pulsed laser ablation in liquid(PLAL).The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm^(-2)in 1.0 m KOH.Furthermore,the bifunctional catalyst achieved a current density of 10 mA cm^(-2)at 1.63 V and retained 98.9%of its initial performance after 100 h of operation.The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport.Density functional theory(DFT)calculations revealed that N-doping optimized intermediate adsorption energies,while the amorphous Ni core facilitated efficient electron transfer.This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.
基金partially funded by EPSRC (EP/T022213/1, EP/W032260/1 and EP/P020194/1) via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202)part of the “Advancing Solid Interface and Lubricants by First Principles Material Design (SLIDE)” project that has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant agreement No. 865633)
文摘Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior performance of amorphous CuNi alloys for CO_(2)electrochemical reduction.By integrating machine learning forcefields for efficient structure generation and density functional theory for subsequent structural refinement and property calculations,we reveal the potential of these disordered systems to outperform their crystalline counterparts.Machine learning forcefields can generate a bulk structure containing a mixture of Cu and Ni atoms,resulting in enhanced catalytic performance.Effective screening of the amorphous surfaces is used to identify undercoordinated Cu and Ni sites in the amorphous structure to synergistically promote selective CO production and favor ethanol formation over ethylene via the stabilization of the*COCHO intermediate,resulting in significantly lower Gibbs free energy changes compared to the crystalline counterpart.The varying atomic coordination environments on amorphous surfaces promote both C–C bond formation and subsequent proton-electron transfer,leading to ethanol formation.These findings demonstrate the superior catalytic performance of amorphous CuNi,highlighting its potential for efficient and selective electroreduction of CO_(2).
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(No.20242BAB25223,20232BCJ23025,20232BCJ25040,20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594).
文摘Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.
基金supported by the National Key Research and Development Programs-Intergovernmental International Cooperation in Science and Technology Innovation Project(Grant No.2022YFE0118400)the Natural Science Foundation of Hunan Province(2023JJ50132)+1 种基金Shenzhen Science and Technology Innovation Committee(Grants Nos.JCYJ20220818100211025,and KCXST20221021111616039)Shenzhen Science and Technology Program(No.20231128110928003)。
文摘The introduction of two-dimensional(2D)perovskite layers on top of three-dimensional(3D)perovskite films enhances the performance and stability of perovskite solar cells(PSCs).However,the electronic effect of the spacer cation and the quality of the 2D capping layer are critical factors in achieving the required results.In this study,we compared two fluorinated salts:4-(trifluoromethyl)benzamidine hydrochloride(4TF-BA·HCl)and 4-fluorobenzamidine hydrochloride(4F-BA·HCl)to engineer the 3D/2D perovskite films.Surprisingly,4F-BA formed a high-performance 3D/2D heterojunction,while4TF-BA produced an amorphous layer on the perovskite films.Our findings indicate that the balanced intramolecular charge polarization,which leads to effective hydrogen bonding,is more favorable in 4F-BA than in 4TF-BA,promoting the formation of a crystalline 2D perovskite.Nevertheless,4TF-BA managed to improve efficiency to 24%,surpassing the control device,primarily due to the natural passivation capabilities of benzamidine.Interestingly,the devices based on 4F-BA demonstrated an efficiency exceeding 25%with greater longevity under various storage conditions compared to 4TF-BA-based and the control devices.
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(Grant Nos.20242BAB25223,20232BCJ23025,20232BCJ25040,and 20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594)。
文摘In sodium-ion hybrid capacitors(SIHCs),the high-capacity metal selenide anodes are severely limited by structural instability and polyselenide dissolution/shuttle during cycling.This study proposes an innovative strategy utilizing high-electronegativity N(χ=3.04)to modulate local electronic domains and stabilize amorphous Mo–Se coordination(N/Mo-Se).Through self-polymerization and tunable selenization,N-doped carbon(NC)nanospheres encapsulating N-stabilized amorphous Mo-Se clusters(N/Mo-Se@NC)are successfully constructed.Theoretical and experimental analyses reveal that N-optimization effectively reconstructs the electronic distribution of Mo–Se coordination via strong covalent Mo–N bonds.This significantly enhances the covalency of Mo-Se clusters and induces localized electronic domains,thereby substantially suppressing polyselenide dissolution/shuttle during cycling.Concurrently,the amorphous N/Mo-Se clusters provide isotropic ion diffusion pathways,and together with the threedimensional(3D)conductive networks of the NC,they jointly optimize charge transfer kinetics.The N/Mo-Se@NC anode exhibits a high reversible capacity of 328.7 mAh g^(-1)after 5000 cycles,even at 10.0 A g^(-1),with a remarkable capacity retention of 110%.The assembled N/Mo-Se@NC//AC SIHCs achieve high energy/power densities(236.1 Wh kg^(-1)/9990 W kg^(-1)),demonstrating superior comprehensive performance compared to most previously reported anodes.This study,through high-electronegativity atom modulation and amorphization engineering,opens new avenues for designing highly stable and high-rate Na^(+) storage materials.
基金supported by the National Natural Science Foundation of China(22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009).
文摘Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).
基金the foundation of Guangdong Engineering Technology Research Center for Hydrogen Energy and Fuel Cells,the Guangdong Provincial Department of Education Innovation Project(No.2022KQNCX056)the Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515110354 and 2021A1515110582)。
文摘Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improved mass transfer and stability.Herein,self-supported crystalline/amorphous NiO/Ni(OH)_(2)nanosheet arrays on nickel foam(NF)are fabricated via an in-situ dissolution-deposition hydrothermal growing of Ni(OH)_(2)nanosheets without additional metal sources assisted by a common Lewis base,EDTA,followed by a rapid calcination at 300℃in air.The as-prepared EDTA-NF-12 h exhibits high OER and HER performance under alkaline conditions,requiring 235 mV and 158 mV,respectively,to reach 10 mA cm^(-2),and the decent performance can be maintained for 24 h without obvious degradation.The dual interfaces,i.e.,the dense crystalline/amorphous interfaces within the NiO/Ni(OH)_(2)nanosheet arrays,as well as the intimate interfaces between nanoarrays and NF,both serve as reaction active sites,facilitate electron transfer,and endow the catalyst with high activity and stability.Furthermore,by applying EDTA-Ni^(2+)and other Lewis bases with varying basicities instead of EDTA,the interfaces with the NF substrate are found to promote the formation of crystalline/amorphous interfaces within the nanosheets.This study offers appealing opportunities for tailoring the electrocatalytic performance of self-supported electrodes via dual interface engineering.
基金financially supported by the National Natural Science Foundation of China(Nos.82203680 and 52273278)the Natural Scientific Foundation of Liaoning Province(No.2021-MS-176)+1 种基金Shenyang Bureau of Science and Technology(No.RC230527)the Central Guidance Funding for Local Scientific and Techno-logical Development in Liaoning(No.2023JH6/100100029).
文摘Guided bone regeneration in the alveolar bone relies on the colonization and differentiation of immune cells within the defect area.The absence of osteoinductive and osteoimmune properties of currently available scaffolds hinders to achieve optimal repair outcomes in clinical settings.Thus,we aimed to enhance the bone repair ability of polycaprolactone(PCL)scaffolds by incorporating osteoinductive amorphous calcium phosphate(ACP)with immune-regulating zinc ions(ACP(Zn),ACZP),to create a favorable immunomodulatory microenvironment.After one day of co-culture with PCL-ACZP,the spreading area of macrophage cells was significantly higher than that from the original PCL scaffold.Additionally,over 32.1%of macrophages exhibited M2 polarization within three days of co-culture.The PCLACZP/macrophage-conditioned medium significantly boosted osteogenic gene expression in MC3T3-E1 cells.After eight weeks of implantation in a rat femoral condyle defect,the BV/TV from the PCL-ACZP group reached 32.9%,1.4 times of that from the PCL group.Furthermore,the PCL-ACZP-GelMA biphasic module as prepared successfully achieved complete regeneration of three-walled alveolar bone defects in rabbits,resulting in arch-shaped alveolar bone repair and providing greater convenience in the clinical settings.This study showcased the effectiveness of PCL-ACZP-GelMA biphasic module as bioactive scaffolds in the morphological restoration of alveolar bone.
基金financially supported by the National Natural Science Foundation of China(Nos.U2067219,52371118,92163201,U23A6013,92360301,and U2330203)Shaanxi Province Innovation Team Project(No.2024RS-CXTD-58)the Fundamental Research Funds for the Central Universities(Nos.xtr042024014 and xtr062024006).
文摘The unique high-entropy and sluggish diffusion effects of amorphous high-entropy alloys endow them with excellent thermal stability and plastic deformation.In this work,the near-equiatomic TaTiZr amorphous medium-entropy alloy(AMEA)was prepared via the magnetron sputtering to investigate the microstructural thermostability and nanoindentation creep behavior.Thermal annealing below the glass transition temperature gave rise to the microstructural heterogeneity due to the positive mixing enthalpy in TaTiZr AMEA,which became increasingly enhanced with raising the annealing temperature.Correspondingly,there appeared a monotonic increase in hardness as well as the elastic/shear modulus,yet a reduction in strain-rate sensitivity m or an increment in shear transformation zone volume with annealing temperature.Meanwhile,the indentation morphology measured by atomic force microscope exhibited a significant transformation from pile-up to sink-in,demonstrating the degradation of plastic deformability with enhancing the microstructural heterogeneity.Based on the relaxation time spectra for Maxwell-Voigt model,the microstructural heterogeneity can restrain the activation of internal defects associated with the operation of flow units during creeping,further triggering the strain-strengthening behavior and improved creep resistance in the annealed samples.This work provides significant guidance for the structural design of high-performance amorphous alloys.
基金supported by National Natural Science Foundation of China(51761034,51961032,51962028 and 52261041)Innovation Foundation of Inner Mongolia University of Science and Technology(2019YQL03)+2 种基金Major Science and Technology Project of Inner Mongolia(2021ZD0029)Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT23005,NJYT23007)Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region(NMGIRT2401).
文摘Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain size,microstructural stability,and hydrogen storage properties.Crystallization kinetics,along with in-situ high-energy XRD characterization,revealed a concentrated and synchronous crystallization of Mg_(2)Ni and RE-Mg-Ni ternary phases with the increase in La and Ni content.The attributed synchronous crystallization process was found to be a result of the close local affinity of Mg_(2)Ni and RE-Mg-Ni ternary phases,as assessed by the thermodynamic Miedema model.Significant secondary phase pinning effect,arising from the high likelihood of well-matching phase structures between Mg_(2)Ni,LaMg_(2)Ni,and LaMgNi_(4),was validated through both the edge-to-edge matching model prediction and experimental observation.Thefine and homogeneous microstructure was shown to be a consequence of fast crystallization kinetics and the secondary phase pinning effect.Improved activation performance and cycling stability were observed,stemming from grain refinement and excellent microstructural stability.Our study provides insights into mechanism of grain refinement of nanocrystalline microstructure tailored by phase constitution and crystallization kinetics in the amorphous-crystallization route.We also demonstrate the potential of material design guided by phase equilibria and crystallographic predictions to improve nanocrystalline with excellent microstructural stability.
基金supported by a project of the Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(Grant No.SZPR2023007)Natural Science Foundation of Sichuan Province(Grant No.2025ZNSFSC0449)Shenzhen Science and Technology Program(Grant No.RCBS20231211090637065).
文摘Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling SLCO.However,due to the presence of cobalt oxide with a spinel phase on the surface of highly-degraded LCO,the strong electrostatic repulsion from the transition metal octahedron poses a high Li replenishment barrier,making the regeneration of highly-degraded LCO a challenge.Herein,we propose a structural transformation strategy for reconstructing Li replenishment channels to aid the direct regeneration of highly-degraded LCO.In this approach,ball milling is employed to disrupt the inherent structure of highly-degraded LCO,thereby releasing the internal stress and converting the surface spinel phase into a homogeneous amorphous structure,which promotes Li insertion and regeneration.The regenerated LCO(RLCO)exhibits an outstanding discharge capacity of 179.10 mAh·g^(−1) in the voltage range of 3.0–4.5 V at 0.5 C.The proposed strategy is an effective regeneration approach for highly-degraded LCO,thereby facilitating the efficient recycling of spent lithium-ion battery cathode materials.
基金supported by the Major Science and Technology Project of Zhongshan City(No.2022AJ004)the Key Basic and Applied Research Program of Guangdong Province(Nos.2019B030302010 and 2022B1515120082)Guangdong Science and Technology Innovation Project(No.2021TX06C111).
文摘In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.