Fe‐based amorphous alloys,despite their intrinsically low magnetocrystalline anisotropy,suffer from quasi‐dislocation dipoles and localized stress fields that impede domain‐wall motion and increase coercivity.Here,...Fe‐based amorphous alloys,despite their intrinsically low magnetocrystalline anisotropy,suffer from quasi‐dislocation dipoles and localized stress fields that impede domain‐wall motion and increase coercivity.Here,we introduce pulse current training(PCT)as an energy‐efficient technique to overcome these limitations in a Fe76Si9B10P5ribbon.As quenched ribbons exhibit a coercivity Hc~10.6 A m−1and the optimized infrared annealing reduced Hc~2 A m−1with a saturation magnetization Ms~162 emu g−1.By applying controlled square‐wave current pulses(J=7000 A cm−2,Tw:Tp=1:2,Tp=0.06 s)over 18-50 cycles,PCT further reduces Hc to below 1 A m−1and increases Ms to 179 emu g−1.Within a moderate‐cycle window,the ribbons maintain sufficient bendability for a practical core.Ultra‐rapid thermal annealing performed as a control reduces Hc to~2.5 A m−1but does not reach the level achieved by PCT,indicating that rapid heating alone cannot account for the superior magnetic softening.Finite‐element simulations and structural characterization show that PCT produces rapid and nearly uniform Joule heating,enabling efficient structural relaxation and enhanced medium‐range order while retaining an overall amorphous structure.Compared with conventional annealing,PCT implements a distinct,pulse energy injection pathway on the potential energy landscape,enabling more controllable tuning of amorphous configurations.This work establishes PCT as a versatile approach for tailoring both magnetic and mechanical properties in amorphous soft magnetic materials,paving the way for their optimized application in advanced electromagnetic devices.展开更多
The direct one-step separation of polymer-grade C2H4 from complex light hydrocarbon mixtures has high industrial significance but is very challenging.Herein,an ethylene-adsorption-weakening strategy is applied f...The direct one-step separation of polymer-grade C2H4 from complex light hydrocarbon mixtures has high industrial significance but is very challenging.Herein,an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks(MOFs)with pillar-layered structures,dubbed TYUT-10/11/12/13.Based on its pore geometry design and functional group regulation,TYUT-12 exhibits exceptional selective adsorption selectivity toward C3H8,C3H6,C2H6,C2H2,and CO2 over C2H4;its C2H6/C2H4 adsorption selectivity reaches 4.56,surpassing the record value of 4.4 by Fe2(O2)(dobdc)(dobdc4-=2,5-dioxido-1,4-benzenedicarboxylate).The weak p–p stacking binding affinity toward C2H4 in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations.Breakthrough experiments demonstrate that C2H4 can be directly obtained from binary,ternary,quaternary,and six-component light hydrocarbon mixtures with over 99.95%purity.展开更多
Engineering multiscale structural hierarchies in glassy alloys enable a broad spectrum of potential applications.Metallic glasses were born in hierarchical structures from atomic-to-nanometer scales.However,the frozen...Engineering multiscale structural hierarchies in glassy alloys enable a broad spectrum of potential applications.Metallic glasses were born in hierarchical structures from atomic-to-nanometer scales.However,the frozen-in structures in traditional metallic glasses prepared by rapid quenching techniques are challenging to tailor.Here,we show that a PdNiPbulk nanostructured glass of polyamorphous interfacial structures was prepared by inert-gas condensation with a laser evaporation source,and its multiscale structures could be engineered.In-situ scattering experiment results reveal polyamorphous phase transitions occurred in the interfacial regions,which are accompanied by the evolution of medium-range order and the nanoscale heterogeneous structures during the condensation process of glassy nanoparticles under high pressure and the following heating process.Moreover,changes in the cluster connectivity resulting from repacking of the local ordering induced by pressure and temperature could be observed.The thermophysical and mechanical properties,including boson peaks,hardness,and elasticity modulus,could be changed as a function of heat-treatment parameters.Our findings would shed light on the synthesis of bulk nanostructured glassy alloys with tailorable thermodynamic and dynamical behavior as well as mechanical properties based on the understanding of metastability for polyamorphous interfacial phases.展开更多
Fe-based metallic glasses are promising functional materials for advanced magnetism and sensor fields.Tailoring magnetic performance in amorphous materials requires a thorough knowledge of the correlation between stru...Fe-based metallic glasses are promising functional materials for advanced magnetism and sensor fields.Tailoring magnetic performance in amorphous materials requires a thorough knowledge of the correlation between structural disorder and magnetic order,which remains ambiguous.Two practical difficulties remain:the first is directly observing subtle magnetic structural changes on multiple scales,and the second is precisely regulating the various amorphous states.Here we propose a novel approach to tailor the amorphous structure through the liquid-liquid phase transition.In-situ synchrotron diffraction has unraveled a medium-range ordering process dominated by edge-sharing cluster connectivity during the liquid-liquid phase transition.Moreover,nanodomains with topological order have been found to exist in composition with liquid-liquid phase transition,manifesting as hexagonal patterns in small-angle neutron scattering profiles.The liquid-liquid phase transition can induce the nanodomains to be more locally ordered,generating stronger exchange interactions due to the reduced Fe–Fe bond length and the enhanced structural order,leading to the increment of saturation magnetization.Furthermore,the increased local heterogeneity at the medium-range scale enhances the magnetic anisotropy,promoting the permeability response under applied stress and leading to a better stress-impedance effect.These experimental results pave the way to tailor the magnetic structure and performance through the liquid-liquid phase transition.展开更多
Amorphous materials are ubiquitous and widely used in human society, yet their structures are far from being fully understood. Metallic glasses, a new class of amorphous materials, have attracted a great deal of inter...Amorphous materials are ubiquitous and widely used in human society, yet their structures are far from being fully understood. Metallic glasses, a new class of amorphous materials, have attracted a great deal of interests due to their exceptional properties. In recent years, our understanding of metallic glasses increases dramatically, thanks to the development of advanced instrumentation, such as in situ x-ray and neutron scattering. In this article, we provide a brief review of recent progress in study of the structure of metallic glasses. In particular, we will emphasize, from the scattering perspective, the multiscale structures of metallic glasses, i.e., short-to-medium range atomic packing, and phase transitions in the supercooled liquid region, e.g., crystallization and liquid-to-liquid phase transition. We will also discuss, based on the understanding of their structures and phase stability, the mechanical and magnetic properties of metallic glasses.展开更多
Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reve...Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reveal the response of critical structure units during deformation.Here,we report the experimental results of an in-situ synchrotron high-energy X-ray study of a Zr-based BMG under uniaxial tension after preprocessing by canning compression of the three-dimensional compressive stress state.It is revealed that the canning-compressed BMG(CC-BMG)sample has better tensile ductility and higher ultimate strength than the as-cast sample,which possesses heterogeneous and loosely packed local struc-tures on medium-range scales.The experimental results revealed two stages of plastic deformation in the CC-BMGs compared with one stage of plastic deformation in the as-cast BMG.Moreover,the shift in the first sharp diffraction peak along the tension direction for the canning-compressed sample is substan-tially more pronounced than that of the as-cast sample.Furthermore,the real-space analysis illustrates a competition mechanism between the 2-atom and 3-atom connection modes on medium-range order during the plastic deformation of the CC-BMG.Additionally,the ordering on the medium-range scale de-creases in the first plastic deformation stage but increases in the second plastic deformation stage.There-fore,a structural crossover phenomenon occurs in the CC-BMG during plastic deformation.Our results demonstrate a structure-property correlation for the CC-BMGs of heterogeneous medium-range ordered structures,which may be beneficial for endowing BMGs with ductility based on medium-range order engineering techniques.展开更多
Bulk metallic glasses(BMGs)are thermodynamically metastable.As such,crystallization occurs when a BMG is thermally annealed at a temperature above the glass transition temperature.While extensive studies have been per...Bulk metallic glasses(BMGs)are thermodynamically metastable.As such,crystallization occurs when a BMG is thermally annealed at a temperature above the glass transition temperature.While extensive studies have been performed on the crystallization kinetics of BMGs,most of them have focused on the amorphous-to-crystalline structural ordering,and little attention has been paid to chemical distribution and its relationship with the structural ordering during the crystallization process.In this paper,a new approach,with simultaneous differential scanning calorimetry(DSC)and small angle neutron scatter-ing(SANS)measurements,was applied to study in situ the crystallization of a Zr45.5Cu45.5Al9BMG upon isothermal annealing at a temperature in the supercooled liquid region.Quantitative analysis of the DSC and SANS data showed that the structural evolution during isothermal annealing could be classified into three stages:(Ⅰ)incubation;(Ⅱ)amorphous-to-crystalline structural ordering;(Ⅲ)continuous chemical redistribution.This finding was validated by composition analysis with atom probe tomography(APT),which further identified a transition region formed by expelling Al into the matrix.The transition re-gion,with a composition of(Cu,Al)50Zr50,served as an intermediate step facilitating the formation of a thermodynamically stable crystalline phase with a composition of(Cu,Al)10Zr7.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.52471180,52192601,52192602,and 52571196)Guangdong Basic and Applied Basic Research,China(Grant Nos.2024A1515140156 and 2024B1515120012)+3 种基金the GIMRT Program of the Institute for Materials Research,Tohoku University(Proposal No.202503‐CRKEQ‐0512)Guangdong Provincial Quantum Science Strategic Initiative(Grant No.GDZX2301001)Guangdong Talent Program(Grant Nos.2024TQ08C641 and 2024TQ08C536)SLAB Young Scientists Program,Guangdong Major Project of Basic and Applied Basic Research,China(Grant No.2019B030302010).
摘要Fe‐based amorphous alloys,despite their intrinsically low magnetocrystalline anisotropy,suffer from quasi‐dislocation dipoles and localized stress fields that impede domain‐wall motion and increase coercivity.Here,we introduce pulse current training(PCT)as an energy‐efficient technique to overcome these limitations in a Fe76Si9B10P5ribbon.As quenched ribbons exhibit a coercivity Hc~10.6 A m−1and the optimized infrared annealing reduced Hc~2 A m−1with a saturation magnetization Ms~162 emu g−1.By applying controlled square‐wave current pulses(J=7000 A cm−2,Tw:Tp=1:2,Tp=0.06 s)over 18-50 cycles,PCT further reduces Hc to below 1 A m−1and increases Ms to 179 emu g−1.Within a moderate‐cycle window,the ribbons maintain sufficient bendability for a practical core.Ultra‐rapid thermal annealing performed as a control reduces Hc to~2.5 A m−1but does not reach the level achieved by PCT,indicating that rapid heating alone cannot account for the superior magnetic softening.Finite‐element simulations and structural characterization show that PCT produces rapid and nearly uniform Joule heating,enabling efficient structural relaxation and enhanced medium‐range order while retaining an overall amorphous structure.Compared with conventional annealing,PCT implements a distinct,pulse energy injection pathway on the potential energy landscape,enabling more controllable tuning of amorphous configurations.This work establishes PCT as a versatile approach for tailoring both magnetic and mechanical properties in amorphous soft magnetic materials,paving the way for their optimized application in advanced electromagnetic devices.
基金supported by National Key Research and Development Program of China(2022YFB3806800)National Natural Science Foundation of China(22278288 and 22090062).
摘要The direct one-step separation of polymer-grade C2H4 from complex light hydrocarbon mixtures has high industrial significance but is very challenging.Herein,an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks(MOFs)with pillar-layered structures,dubbed TYUT-10/11/12/13.Based on its pore geometry design and functional group regulation,TYUT-12 exhibits exceptional selective adsorption selectivity toward C3H8,C3H6,C2H6,C2H2,and CO2 over C2H4;its C2H6/C2H4 adsorption selectivity reaches 4.56,surpassing the record value of 4.4 by Fe2(O2)(dobdc)(dobdc4-=2,5-dioxido-1,4-benzenedicarboxylate).The weak p–p stacking binding affinity toward C2H4 in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations.Breakthrough experiments demonstrate that C2H4 can be directly obtained from binary,ternary,quaternary,and six-component light hydrocarbon mixtures with over 99.95%purity.
基金financially supported by the National Key R&D Program of China(No.2021YFB3802800)the National Natural Science Foundation of China(No.51871120)+8 种基金the Natural Science Foundation of Jiangsu Province(No.BK20200019)the Fundamental Research Funds for the Central Universities(Nos.309190111073092001000430919011404)supports by Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technology and Shenzhen Science and Technology Innovation Commission(No.JCYJ202000109105618137)support from Qing Lan project and the distinguished professor project of Jiangsu provincesupport by the Shenzhen Science and Technology Innovation Committee(No.JCYJ20170413140446951)the Ministry of Science and Technology of China(No.2016YFA0401501)supported by the US DOE Office of Science,Office of Basic Energy Sciences。
摘要Engineering multiscale structural hierarchies in glassy alloys enable a broad spectrum of potential applications.Metallic glasses were born in hierarchical structures from atomic-to-nanometer scales.However,the frozen-in structures in traditional metallic glasses prepared by rapid quenching techniques are challenging to tailor.Here,we show that a PdNiPbulk nanostructured glass of polyamorphous interfacial structures was prepared by inert-gas condensation with a laser evaporation source,and its multiscale structures could be engineered.In-situ scattering experiment results reveal polyamorphous phase transitions occurred in the interfacial regions,which are accompanied by the evolution of medium-range order and the nanoscale heterogeneous structures during the condensation process of glassy nanoparticles under high pressure and the following heating process.Moreover,changes in the cluster connectivity resulting from repacking of the local ordering induced by pressure and temperature could be observed.The thermophysical and mechanical properties,including boson peaks,hardness,and elasticity modulus,could be changed as a function of heat-treatment parameters.Our findings would shed light on the synthesis of bulk nanostructured glassy alloys with tailorable thermodynamic and dynamical behavior as well as mechanical properties based on the understanding of metastability for polyamorphous interfacial phases.
基金financially supported by the National Key R&D Program of China(No.2021YFB3802800)the Natural Science Foundation of Jiangsu Province(No.BK20200019)+6 种基金the National Natural Science Foundation of China(Nos.52222104,12261160364,51871120,and 51520105001)support from the Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technologysupport of the Shenzhen Science and Technology Innovation Committee(No.JCYJ20170413140446951)partial support by the Research Grants Council of the Hong Kong Special Administrative Region,Project N_CityU173/22support of the National Natural Science Foundation of China(No.12275154)the Guangdong Basic and Applied Basic Research Foundation(No.2021B1515140028)supported by the US DOE Office of Science,Office of Basic Energy Sciences.
摘要Fe-based metallic glasses are promising functional materials for advanced magnetism and sensor fields.Tailoring magnetic performance in amorphous materials requires a thorough knowledge of the correlation between structural disorder and magnetic order,which remains ambiguous.Two practical difficulties remain:the first is directly observing subtle magnetic structural changes on multiple scales,and the second is precisely regulating the various amorphous states.Here we propose a novel approach to tailor the amorphous structure through the liquid-liquid phase transition.In-situ synchrotron diffraction has unraveled a medium-range ordering process dominated by edge-sharing cluster connectivity during the liquid-liquid phase transition.Moreover,nanodomains with topological order have been found to exist in composition with liquid-liquid phase transition,manifesting as hexagonal patterns in small-angle neutron scattering profiles.The liquid-liquid phase transition can induce the nanodomains to be more locally ordered,generating stronger exchange interactions due to the reduced Fe–Fe bond length and the enhanced structural order,leading to the increment of saturation magnetization.Furthermore,the increased local heterogeneity at the medium-range scale enhances the magnetic anisotropy,promoting the permeability response under applied stress and leading to a better stress-impedance effect.These experimental results pave the way to tailor the magnetic structure and performance through the liquid-liquid phase transition.
基金supported by Shenzhen Science and Technology Innovation Commission of China(Grant No.R-IND8701)the Croucher Foundation(Project No.City U 9500020)+2 种基金partially supported by the Fundamental Research Funds for the Central Universities of China(Grant No.30915015103)the National Natural Science Foundation of China(Grant No.51501090)partially supported by the National Natural Science Foundation of China(Grant No.51571170)
摘要Amorphous materials are ubiquitous and widely used in human society, yet their structures are far from being fully understood. Metallic glasses, a new class of amorphous materials, have attracted a great deal of interests due to their exceptional properties. In recent years, our understanding of metallic glasses increases dramatically, thanks to the development of advanced instrumentation, such as in situ x-ray and neutron scattering. In this article, we provide a brief review of recent progress in study of the structure of metallic glasses. In particular, we will emphasize, from the scattering perspective, the multiscale structures of metallic glasses, i.e., short-to-medium range atomic packing, and phase transitions in the supercooled liquid region, e.g., crystallization and liquid-to-liquid phase transition. We will also discuss, based on the understanding of their structures and phase stability, the mechanical and magnetic properties of metallic glasses.
基金the National Key R&D Program of China(No.2021YFB3802800)the National Natural Sci-ence Foundation of China(Nos.52222104,12261160364,51871120 and 51520105001)+3 种基金the Natural Science Foundation of Jiangsu Province(No.BK20200019)Si Lan acknowledges the support by Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scat-tering Science and Technology and Shenzhen Science and Technol-ogy Innovation Commission(No.JCYJ20200109105618137)the resources of the China Spallation Neutron Source located in Dongguan,China,and the Advanced Photon Source,a US Department of Energy(DOE)Office of Science User Facility op-erated for the DOE Office of Science by Argonne National Labora-tory under Contract No.DE-AC02-06CH11357the US DOE Office of Science,Office of Basic Energy Sciences.The neutron scattering experiments carried out at the Spallation Neutron Source were sponsored by the Scientific User Facilities Di-vision,Office of Basic Energy Sciences,U.S.Department of Energy,under Contract No.DE-AC05-00OR22725 with Oak Ridge National Laboratory.
摘要Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reveal the response of critical structure units during deformation.Here,we report the experimental results of an in-situ synchrotron high-energy X-ray study of a Zr-based BMG under uniaxial tension after preprocessing by canning compression of the three-dimensional compressive stress state.It is revealed that the canning-compressed BMG(CC-BMG)sample has better tensile ductility and higher ultimate strength than the as-cast sample,which possesses heterogeneous and loosely packed local struc-tures on medium-range scales.The experimental results revealed two stages of plastic deformation in the CC-BMGs compared with one stage of plastic deformation in the as-cast BMG.Moreover,the shift in the first sharp diffraction peak along the tension direction for the canning-compressed sample is substan-tially more pronounced than that of the as-cast sample.Furthermore,the real-space analysis illustrates a competition mechanism between the 2-atom and 3-atom connection modes on medium-range order during the plastic deformation of the CC-BMG.Additionally,the ordering on the medium-range scale de-creases in the first plastic deformation stage but increases in the second plastic deformation stage.There-fore,a structural crossover phenomenon occurs in the CC-BMG during plastic deformation.Our results demonstrate a structure-property correlation for the CC-BMGs of heterogeneous medium-range ordered structures,which may be beneficial for endowing BMGs with ductility based on medium-range order engineering techniques.
基金financially supported by the Croucher Foundation(Project No.City U 9500034)the Research Grants Council of Hong Kong Special Administrative Region(No.JLFS/P102/18)+5 种基金the National Natural Science Foundation of China(Nos.51871120,51520105001,5157117051571170,and 51501090)the Shenzhen Science and Technology Innovation Committee(No.JCYJ20170413140446951)support from the Ministry of Science and Technology of the People’s Republic of China(No.2016YFA0401501)support of the Fundamental Research Funds for the Central Universities(Nos.30919011107,30919011404)the Natural Science Foundation of Jiangsu Province(No.BK20171425)support from Guangdong Basic and Applied Basic Research Foundation(No.2020B1515120077)。
摘要Bulk metallic glasses(BMGs)are thermodynamically metastable.As such,crystallization occurs when a BMG is thermally annealed at a temperature above the glass transition temperature.While extensive studies have been performed on the crystallization kinetics of BMGs,most of them have focused on the amorphous-to-crystalline structural ordering,and little attention has been paid to chemical distribution and its relationship with the structural ordering during the crystallization process.In this paper,a new approach,with simultaneous differential scanning calorimetry(DSC)and small angle neutron scatter-ing(SANS)measurements,was applied to study in situ the crystallization of a Zr45.5Cu45.5Al9BMG upon isothermal annealing at a temperature in the supercooled liquid region.Quantitative analysis of the DSC and SANS data showed that the structural evolution during isothermal annealing could be classified into three stages:(Ⅰ)incubation;(Ⅱ)amorphous-to-crystalline structural ordering;(Ⅲ)continuous chemical redistribution.This finding was validated by composition analysis with atom probe tomography(APT),which further identified a transition region formed by expelling Al into the matrix.The transition re-gion,with a composition of(Cu,Al)50Zr50,served as an intermediate step facilitating the formation of a thermodynamically stable crystalline phase with a composition of(Cu,Al)10Zr7.