The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystalliz...The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystallized mixture is α Fe and Pr 2Fe 14 B, and the metastable Pr 2Fe 23 B 3 phase occurs during crystallization of Pr 8Fe 86 B 6 amorphous alloy, not during crystallization of Pr 8Fe 86- x Zr x B 6( x =1, 2) amorphous alloys. By analyzing the activation energy of crystallization, the formation of an α Fe/Pr 2Fe 14 B composite microstructure with a coarse grain size in annealed Pr 8Fe 86 B 6 alloy, is attributed to a difficult nucleation and an easy growth for both the α Fe and Pr 2Fe 14 B in the alloy. The addition of Zr can be used to change the crystallization behavior of the α Fe phase in Pr Fe B amorphous alloy, which is helpful to reduce the grain size for the α Fe phase.展开更多
Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate ...Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.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
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
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
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
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
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
The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were inves...The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were investigated.The DCT samples were obtained by subjecting the as-annealed samples to a thermal cycling process between the temperature of the supercooled liquid zone and the temperature of liquid nitrogen.Through flat plate bending testing,hardness measurements,and nanoindentation experiment,it is found that the bending toughness of the DCT samples is improved and the soft magnetic properties are also slightly enhanced.These are attributed to the rejuvenation behavior of the DCT samples,which demonstrate a higher enthalpy of relaxation.Therefore,DCT is an effective method to enhance the bending toughness of Fe-based amorphous nanocrystalline alloys without degrading the soft magnetic properties.展开更多
Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(...Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(NFM30-N)for the oxygen evolution reaction(OER)using a facile top-down approach that combines arc melting with dealloying-oxidation.Due to the dealloying-oxidation effect,the asderived porous amorphous M-O,M-OH,and M-OOH(M=Ni,Fe)nanocones cover the basic NiFeMn alloy.This integrated design enables NFM30-N to exhibit outstanding OER performance at high current densities,requiring low overpotentials of only 282 and 323 mV to achieve large current densities of 100 and 500 mA cm^(-2),respectively.It also displays a small Tafel slope of 44.1 mV dec^(-1) and remarkable stability for over 100 h at 100 and 500 mA cm^(-2).When used as an anode,a two-electrode electrolyzer cell with NFM30-N at 500 mA cm^(-2) only requires a cell voltage of 1.619 V and exhibits excellent stability,with almost no performance degradation after continuous chronopotentiometry test for each 100 h at 500 and 100 mA cm^(-2).This exceptional OER electrocatalytic performance is attributed to the integrated structure providing high electrical conductivity and stability,the presence of numerous active sites due to dealloying and the amorphous structure,and the promotion of the OER process by M-O,M-OH,and M-OOH species.This work offers a novel idea for fabricating integrated,industrially relevant electrocatalytic electrodes through traditional metallurgy combined with dealloying-oxidation.展开更多
Amorphous metallic coatings with a composition of Fe48Cr15Mo14C15B6Y2 were prepared by detonation gun spraying process. Microstructural studies show that the coatings present a densely layered structure typical of the...Amorphous metallic coatings with a composition of Fe48Cr15Mo14C15B6Y2 were prepared by detonation gun spraying process. Microstructural studies show that the coatings present a densely layered structure typical of thermally sprayed deposits with the porosity below 2%. Both crystallization and oxidation occurred obviously during spraying process, so that the amorphous fraction of the coatings decreased to 54% compared with fully amorphous alloy ribbons of the same component. Corrosion behavior of the amorphous coatings was investigated by electrochemical measurement. The results show that the coatings exhibit extremely wide passive region and low passive current density in 3.5% NaCl (mass fraction) and 1 mol/L HCl solutions, which illustrates excellent ability to resist localized corrosion.展开更多
In this study,a few Fe-based amorphous matrix composite coatings reinforced with various portions(4,8 and16 vol.%) of 31 6L stainless steel powders have been successfully produced through high velocity oxy-fuel(HVOF) ...In this study,a few Fe-based amorphous matrix composite coatings reinforced with various portions(4,8 and16 vol.%) of 31 6L stainless steel powders have been successfully produced through high velocity oxy-fuel(HVOF) spraying.The microstructure of the composite coatings was systematically characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM) and transmission electron microscopy(TEM).The main structure of composite coatings remained amorphous while 31 6L stainless steel splats were distributed homogeneously in the amorphous matrix and well connected with surrounding amorphous phase.Bonding strength of coatings to the substrate was determined by 'pull-off' tensile tests.The results revealed that the31 6L stainless steel phase effectively improved the bonding strength of amorphous coatings,which is mainly contributed by the strong metallurgical bonding between stainless steel and amorphous splats.The addition of31 6L stainless steel also enhanced the ductility and fracture resistance of the coatings due to the ductile stainless steel phases,which can arrest crack propagation and increase energy dissipation.展开更多
The core loss spectrum P(f) of Fe-B-Si amorphous soft magnetic alloy has been studied.It is found that P(f) has the fractal structure.The effect of heat treatment on the fractal dimension Df is discussed.
In this work,the electrochemical behaviors of SAM2X5 Fe-based amorphous alloy coating and hard chromium coating were comparatively studied in 3.5 wt% NaCl solution.In comparison with the hard chromium coating,the SAM2...In this work,the electrochemical behaviors of SAM2X5 Fe-based amorphous alloy coating and hard chromium coating were comparatively studied in 3.5 wt% NaCl solution.In comparison with the hard chromium coating,the SAM2X5 coating exhibited a wider and stable passive region with lower passive current density in the potentiodynamic polarization and showed a considerably lower current density at different anodic potentials in the potentiostatic polarization.In order to understand the passivation mechanism of the Fe-based amorphous coating,the components of the passive films formed at various polarization potentials were examined by X-ray photoelectron spectroscopy.The synergistic effect of Mo,W,Mn and Cr in the passive films was systemically analyzed.It has been revealed that Mo and W facilitate the formation of compact and stable Cr2O3 passive film at lower potentials,and the substantial enrichment of Mn in the passive film enhances the passivation ability at relatively higher potentials.The deep understanding of the passivation characteristics in multicomponent alloy systems could provide a guide for the design of corrosion-resistant amorphous alloy coatings for engineering applications.展开更多
A novel nanosized amorphous Ru-Fe-B/ZrO2 alloy catalyst for benzene selective hydrogenation to cyclohexene was investigated. The superior properties of this catalyst were attributed to the combination of the nanosize ...A novel nanosized amorphous Ru-Fe-B/ZrO2 alloy catalyst for benzene selective hydrogenation to cyclohexene was investigated. The superior properties of this catalyst were attributed to the combination of the nanosize and the amorphous character as well as to its textural character. In addition, the concentration of zinc ions, the content of ZrO2 in the slurry, and the pretreatment of the catalyst were found to be effective in improving the activity and the selectivity of the catalyst.展开更多
Tensile and fracture behaviors of sandwich-structured composites consisting of a Fe-based amorphous layer with a constant thickness and ultrafine-grained Ni layers with different thicknesses were investigated. The res...Tensile and fracture behaviors of sandwich-structured composites consisting of a Fe-based amorphous layer with a constant thickness and ultrafine-grained Ni layers with different thicknesses were investigated. The results indicate that the initiation and the stable propagation of the shear band in the amorphous layer was dominated by the Ni layers due to their strong constraint role. The catastrophic fracture of the amorphous layer was postponed in the sandwich composites through properly increasing the constrained Ni layer thickness, which effectively decreased the shear stress on the shear fracture planes of the amorphous layer, and thus led to stable propagation of the primary SB characterized by the increase in the smooth region size of the shear band.展开更多
Fe83（Cox,Niy）（B11Si2P3C1）1-x,y/17（x,y=1–3）amorphous alloys with high saturation magnetic flux density（Bs）and excellent soft-magnetic properties were developed and then the microalloying and clustering effects...Fe83（Cox,Niy）（B11Si2P3C1）1-x,y/17（x,y=1–3）amorphous alloys with high saturation magnetic flux density（Bs）and excellent soft-magnetic properties were developed and then the microalloying and clustering effects were explored.The microalloying of Co and Ni improves the Bsfrom 1.65 T to 1.67–1.72 T and 1.66–1.68 T,respectively.The Ni-doped alloys exhibit better soft-magnetic properties,containing a low coercivity（Hc） of about 5.0 A/m and a high Effective permeability（μe）of（8–10）×10^3,whereas the microalloying of Co leads to a deteriorative Hc of 5.0–13.0 A/m and a μeof（5–8）×10^3.Moreover,microalloying of Ni can increase the ductile-brittle transition（DBT）temperature of the ribbons,while a totally opposite effect is found in the Co-doped alloys.The formation of dense α-Fe（Co,Ni）clusters during annealing process is used to explain the distinct effects of Co and Ni microalloying on the magnetic properties and bending toughness.展开更多
The Fe-based amorphous coatings were produced by air plasma spraying. The as-sprayed coatings were heat-treated at the temperature of 573, 873, and 1 023 K, respectively. The crystallization and wear behavior of the h...The Fe-based amorphous coatings were produced by air plasma spraying. The as-sprayed coatings were heat-treated at the temperature of 573, 873, and 1 023 K, respectively. The crystallization and wear behavior of the heat-treated amorphous coatings were investigated. It was found that the amorphous- nanocrystalline transformation appeared when the as-sprayed coatings were treated at 853 K. The crystallization process had completed and a coating with microcrystallines was formed when the treatment temperature reached 1 023 K. The resultant amorphous and nanocrystalline composite coatings exhibited superior wear resistance compared to crystalline coating. It is attributed to fine grain strengthening of formed nanocrystallines.展开更多
In this paper, the synthetic effect ofCr, Mo and Y on corrosion resistance was explored, and the YCr/Mo value was employed to evaluate the corrosion resistance. The composition of amorphous alloy was designed by mixin...In this paper, the synthetic effect ofCr, Mo and Y on corrosion resistance was explored, and the YCr/Mo value was employed to evaluate the corrosion resistance. The composition of amorphous alloy was designed by mixing the Fe41Co7Cr15Mo14C15B6Y2 （BMG1） with good glass forming ability （GFA） and Fe50Cr22B23Ni5.4 with a high corrosion resistance at 9：1 ratio. At the same time, the contents of Y, Mo and Cr were fine-tuned. The electrochemical tests demonstrated that the passivation current density decreased with the increase of the yCr/Mo value. The passivation current density of Fe-based amorphous alloy was reduced by about half an order of magnitude. The fitting result showed that the logarithm ofpassivation current density （I） and the YCr/Mo value （X） were logarithmic relationship, and the fitting equation was I=-5.649＋4.904× 1015 e 17.52x. The X-ray photoelectron spectroscopy （XPS） results showed that the yC,/Mo value played a key role in stability of passive films. When the yCr/Mo value Was low, the Cr6＋ ion, Mo6＋ ion were enriched in the initial stage of passivation process, then leading to the increase passivation current density. However, when the YCr/Mo value was high, the low-valence Fe2-, Cr3＋, and Mo4＋ ion were enriched more easily, which result in small passivation current densities and more stable passive films.展开更多
文摘The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystallized mixture is α Fe and Pr 2Fe 14 B, and the metastable Pr 2Fe 23 B 3 phase occurs during crystallization of Pr 8Fe 86 B 6 amorphous alloy, not during crystallization of Pr 8Fe 86- x Zr x B 6( x =1, 2) amorphous alloys. By analyzing the activation energy of crystallization, the formation of an α Fe/Pr 2Fe 14 B composite microstructure with a coarse grain size in annealed Pr 8Fe 86 B 6 alloy, is attributed to a difficult nucleation and an easy growth for both the α Fe and Pr 2Fe 14 B in the alloy. The addition of Zr can be used to change the crystallization behavior of the α Fe phase in Pr Fe B amorphous alloy, which is helpful to reduce the grain size for the α Fe phase.
基金supported by the Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the National Natural Science Foundation of China(Key Program)(52131306,52122209,52403001)+1 种基金the Project on National Key R&D Program of China(2021YFB2400400)the Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University。
文摘Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.
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 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 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.
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(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supported by Liaoning Joint Fund of NSFC(No.U1908219)。
文摘The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were investigated.The DCT samples were obtained by subjecting the as-annealed samples to a thermal cycling process between the temperature of the supercooled liquid zone and the temperature of liquid nitrogen.Through flat plate bending testing,hardness measurements,and nanoindentation experiment,it is found that the bending toughness of the DCT samples is improved and the soft magnetic properties are also slightly enhanced.These are attributed to the rejuvenation behavior of the DCT samples,which demonstrate a higher enthalpy of relaxation.Therefore,DCT is an effective method to enhance the bending toughness of Fe-based amorphous nanocrystalline alloys without degrading the soft magnetic properties.
基金the National Natural Science Foundation of China(Nos.52174365,52004155,52334009 and 52130204)the National Key R&D Program of China(Nos.2023YFB3506701 and 2022YFB3706801)the Science and Technology Commission of Shanghai Municipality(No.21DZ1208900).
文摘Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(NFM30-N)for the oxygen evolution reaction(OER)using a facile top-down approach that combines arc melting with dealloying-oxidation.Due to the dealloying-oxidation effect,the asderived porous amorphous M-O,M-OH,and M-OOH(M=Ni,Fe)nanocones cover the basic NiFeMn alloy.This integrated design enables NFM30-N to exhibit outstanding OER performance at high current densities,requiring low overpotentials of only 282 and 323 mV to achieve large current densities of 100 and 500 mA cm^(-2),respectively.It also displays a small Tafel slope of 44.1 mV dec^(-1) and remarkable stability for over 100 h at 100 and 500 mA cm^(-2).When used as an anode,a two-electrode electrolyzer cell with NFM30-N at 500 mA cm^(-2) only requires a cell voltage of 1.619 V and exhibits excellent stability,with almost no performance degradation after continuous chronopotentiometry test for each 100 h at 500 and 100 mA cm^(-2).This exceptional OER electrocatalytic performance is attributed to the integrated structure providing high electrical conductivity and stability,the presence of numerous active sites due to dealloying and the amorphous structure,and the promotion of the OER process by M-O,M-OH,and M-OOH species.This work offers a novel idea for fabricating integrated,industrially relevant electrocatalytic electrodes through traditional metallurgy combined with dealloying-oxidation.
文摘Amorphous metallic coatings with a composition of Fe48Cr15Mo14C15B6Y2 were prepared by detonation gun spraying process. Microstructural studies show that the coatings present a densely layered structure typical of thermally sprayed deposits with the porosity below 2%. Both crystallization and oxidation occurred obviously during spraying process, so that the amorphous fraction of the coatings decreased to 54% compared with fully amorphous alloy ribbons of the same component. Corrosion behavior of the amorphous coatings was investigated by electrochemical measurement. The results show that the coatings exhibit extremely wide passive region and low passive current density in 3.5% NaCl (mass fraction) and 1 mol/L HCl solutions, which illustrates excellent ability to resist localized corrosion.
基金financially supported by the National Natural Science Foundation of China (Grant Nos. 51271081 and 51301072)partially supported by the Key Fundamental Research Project from Shenzhen Research Council (No. JC201105170745A)
文摘In this study,a few Fe-based amorphous matrix composite coatings reinforced with various portions(4,8 and16 vol.%) of 31 6L stainless steel powders have been successfully produced through high velocity oxy-fuel(HVOF) spraying.The microstructure of the composite coatings was systematically characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM) and transmission electron microscopy(TEM).The main structure of composite coatings remained amorphous while 31 6L stainless steel splats were distributed homogeneously in the amorphous matrix and well connected with surrounding amorphous phase.Bonding strength of coatings to the substrate was determined by 'pull-off' tensile tests.The results revealed that the31 6L stainless steel phase effectively improved the bonding strength of amorphous coatings,which is mainly contributed by the strong metallurgical bonding between stainless steel and amorphous splats.The addition of31 6L stainless steel also enhanced the ductility and fracture resistance of the coatings due to the ductile stainless steel phases,which can arrest crack propagation and increase energy dissipation.
文摘The core loss spectrum P(f) of Fe-B-Si amorphous soft magnetic alloy has been studied.It is found that P(f) has the fractal structure.The effect of heat treatment on the fractal dimension Df is discussed.
基金supported by the National Natural Science Foundation of China (Nos. 51471166, 51131006 and 51171119)the College Youth Scholar Fostering Program of Liaoning Province (No. LJQ2014015)
文摘In this work,the electrochemical behaviors of SAM2X5 Fe-based amorphous alloy coating and hard chromium coating were comparatively studied in 3.5 wt% NaCl solution.In comparison with the hard chromium coating,the SAM2X5 coating exhibited a wider and stable passive region with lower passive current density in the potentiodynamic polarization and showed a considerably lower current density at different anodic potentials in the potentiostatic polarization.In order to understand the passivation mechanism of the Fe-based amorphous coating,the components of the passive films formed at various polarization potentials were examined by X-ray photoelectron spectroscopy.The synergistic effect of Mo,W,Mn and Cr in the passive films was systemically analyzed.It has been revealed that Mo and W facilitate the formation of compact and stable Cr2O3 passive film at lower potentials,and the substantial enrichment of Mn in the passive film enhances the passivation ability at relatively higher potentials.The deep understanding of the passivation characteristics in multicomponent alloy systems could provide a guide for the design of corrosion-resistant amorphous alloy coatings for engineering applications.
文摘A novel nanosized amorphous Ru-Fe-B/ZrO2 alloy catalyst for benzene selective hydrogenation to cyclohexene was investigated. The superior properties of this catalyst were attributed to the combination of the nanosize and the amorphous character as well as to its textural character. In addition, the concentration of zinc ions, the content of ZrO2 in the slurry, and the pretreatment of the catalyst were found to be effective in improving the activity and the selectivity of the catalyst.
基金supported by the National Natural Science Foundation of China(NSFC,Grant Nos.51571199 and 51671050)supported by NSFC(Grant No.51601198)
文摘Tensile and fracture behaviors of sandwich-structured composites consisting of a Fe-based amorphous layer with a constant thickness and ultrafine-grained Ni layers with different thicknesses were investigated. The results indicate that the initiation and the stable propagation of the shear band in the amorphous layer was dominated by the Ni layers due to their strong constraint role. The catastrophic fracture of the amorphous layer was postponed in the sandwich composites through properly increasing the constrained Ni layer thickness, which effectively decreased the shear stress on the shear fracture planes of the amorphous layer, and thus led to stable propagation of the primary SB characterized by the increase in the smooth region size of the shear band.
基金mainly supported by the National Natural Science Foundation of China (Grant Nos.51601206,51671206)Ningbo International Cooperation Projects (Grant No.2015D10022)Ningbo Major Project for Science and Technology (Grant No.201401B1003003)
文摘Fe83（Cox,Niy）（B11Si2P3C1）1-x,y/17（x,y=1–3）amorphous alloys with high saturation magnetic flux density（Bs）and excellent soft-magnetic properties were developed and then the microalloying and clustering effects were explored.The microalloying of Co and Ni improves the Bsfrom 1.65 T to 1.67–1.72 T and 1.66–1.68 T,respectively.The Ni-doped alloys exhibit better soft-magnetic properties,containing a low coercivity（Hc） of about 5.0 A/m and a high Effective permeability（μe）of（8–10）×10^3,whereas the microalloying of Co leads to a deteriorative Hc of 5.0–13.0 A/m and a μeof（5–8）×10^3.Moreover,microalloying of Ni can increase the ductile-brittle transition（DBT）temperature of the ribbons,while a totally opposite effect is found in the Co-doped alloys.The formation of dense α-Fe（Co,Ni）clusters during annealing process is used to explain the distinct effects of Co and Ni microalloying on the magnetic properties and bending toughness.
基金Funded by the Basic Scientific Research of Central Colleges,Chang’an University (No. CHD2011JC126)
文摘The Fe-based amorphous coatings were produced by air plasma spraying. The as-sprayed coatings were heat-treated at the temperature of 573, 873, and 1 023 K, respectively. The crystallization and wear behavior of the heat-treated amorphous coatings were investigated. It was found that the amorphous- nanocrystalline transformation appeared when the as-sprayed coatings were treated at 853 K. The crystallization process had completed and a coating with microcrystallines was formed when the treatment temperature reached 1 023 K. The resultant amorphous and nanocrystalline composite coatings exhibited superior wear resistance compared to crystalline coating. It is attributed to fine grain strengthening of formed nanocrystallines.
基金Project supported by the National Natural Science Foundation of China(51261021)Science and Technology Landing Plan Project of Jiangxi Province(KJLD13056)
文摘In this paper, the synthetic effect ofCr, Mo and Y on corrosion resistance was explored, and the YCr/Mo value was employed to evaluate the corrosion resistance. The composition of amorphous alloy was designed by mixing the Fe41Co7Cr15Mo14C15B6Y2 （BMG1） with good glass forming ability （GFA） and Fe50Cr22B23Ni5.4 with a high corrosion resistance at 9：1 ratio. At the same time, the contents of Y, Mo and Cr were fine-tuned. The electrochemical tests demonstrated that the passivation current density decreased with the increase of the yCr/Mo value. The passivation current density of Fe-based amorphous alloy was reduced by about half an order of magnitude. The fitting result showed that the logarithm ofpassivation current density （I） and the YCr/Mo value （X） were logarithmic relationship, and the fitting equation was I=-5.649＋4.904× 1015 e 17.52x. The X-ray photoelectron spectroscopy （XPS） results showed that the yC,/Mo value played a key role in stability of passive films. When the yCr/Mo value Was low, the Cr6＋ ion, Mo6＋ ion were enriched in the initial stage of passivation process, then leading to the increase passivation current density. However, when the YCr/Mo value was high, the low-valence Fe2-, Cr3＋, and Mo4＋ ion were enriched more easily, which result in small passivation current densities and more stable passive films.
