Rare earth high-entropy alloys(RE-HEAs)exhibit great potential to be applied as refrigerants due to their good comprehensive magnetocaloric properties.In this work,octary GdTbDyHoErTmCoAl and GdTbDyHoErTmCoNi RE-HEAs ...Rare earth high-entropy alloys(RE-HEAs)exhibit great potential to be applied as refrigerants due to their good comprehensive magnetocaloric properties.In this work,octary GdTbDyHoErTmCoAl and GdTbDyHoErTmCoNi RE-HEAs with amorphous/nanocrystalline structure exhibiting comparable magnetocaloric effect were synthesized.Both RE-HEAs show a second-order magnetic phase transition in the temperature range of hydrogen liquefaction.Due to the complex magnetic interactions,a spin glasslike behavior at low temperatures is observed in the RE-HEAs.A superior magnetocaloric effect is obtained in the nanocrystalline GdTbDyHoErTmCoNi high-entropy alloy that is multiphase attributed to a stronger magnetic exchange interaction when compared with the other that exhibits single amorphous structure.Despite heterogeneous microstructure,homogeneous chemical distributions are observed in the partially crystallized high-entropy alloy.In addition,the magnetocaloric effect and magnetic transition behavior of rare earth medium-and high-entropy alloys,including the RE-HEAs in this study,are summarized and discussed.The results in this work provide a helpful guide for the design of RE-HEAs for hydrogen liquefaction applications with excellent magnetocaloric effects.展开更多
Soft magnetic composites(SMCs)play a pivotal role in the development of high-frequency,miniaturization and complex forming of modern electronics.However,they usually suffer from a trade-off between high magnetization ...Soft magnetic composites(SMCs)play a pivotal role in the development of high-frequency,miniaturization and complex forming of modern electronics.However,they usually suffer from a trade-off between high magnetization and good magnetic softness(high permeability and low core loss).In this work,utilizing the order modulation strategy,a critical state in a FeSiBCCr amorphous soft magnetic composite(ASMC),consisting of massive crystal-like orders(CLOs,∼1 nm in size)with the feature ofα-Fe,is designed.This critical-state structure endows the amorphous powder with the enhanced ferromagnetic exchange interactions and the optimized magnetic domains with uniform orientation and fewer micro-vortex dots.Superior comprehensive soft magnetic properties at high frequency emerge in the ASMC,such as a high saturation magnetization(Ms)of 170 emu g^(-1)and effective permeability(µ_(e))of 65 combined with a core loss(Pcv)as low as 70 mW cm^(-3)(0.01 T,1 MHz).This study provides a new strategy for the development of high-frequency ASMCs,possessing suitable comprehensive soft magnetic performance to match the requirements of the modern magnetic devices used in the third-generation semiconductors and new energy fields.展开更多
Comprehending the pressure-/temperature-induced structural transition in glasses,as one of the most fascinating issues in material science,is far from being well understood.Here,we report novel polyamorphic transition...Comprehending the pressure-/temperature-induced structural transition in glasses,as one of the most fascinating issues in material science,is far from being well understood.Here,we report novel polyamorphic transitions in a Cu-based metallic glass(MG)with apparent nanoscale structural heterogeneity relating to proper Y addition.The low-density MG compresses continuously with increasing pressure,and then a compression plateau appears after∼8.1 GPa,evolving into an intermediate state with an ultrahigh bulk modulus of∼467 GPa.It then transforms to a high-density MG with significantly decreased structural heterogeneity above∼14.1 GPa.Three-dimensional atom probe tomography reveals concentration waves of Cu/Zr elements with an average wavelength of∼5-6 nm,which promote the formation of interconnected ringlike networks composed of Cu-rich and Zr-rich dual-glass domains at nanometer scale.Our experimental and simulation results indicate that steplike polyamorphism may stem from synergic effects of the abnormal compression of the Zr-Zr bond length at the atomic scale and the interplay between the applied pressure and incipient concentration waves(Cu and Zr)at several nanometer scales.The present work provides new insights into polyamorphism in glasses and contributes to the development of high-performance amorphous materials by high-pressure nanostructure engineering.展开更多
Liquid dynamics plays an essential role in glass formation.Here we observed a distinct change of liquid dynamics in Gd_(55)Co_(20)Al_(25)metallic glass induced by microalloying Si element.In the equilibrium melt,minor...Liquid dynamics plays an essential role in glass formation.Here we observed a distinct change of liquid dynamics in Gd_(55)Co_(20)Al_(25)metallic glass induced by microalloying Si element.In the equilibrium melt,minor Si(0.5 at.%)addition leads to a more fragile liquid behavior and a smaller strength of liquid-liquid transition with the transition strength(F)decreasing from 0.76 to 0.35.However,in the supercooled liquid,Si-doped liquid exhibits a remarkable enhanced fragile-to-strong transition(FST),and the value of FST factor f increases sharply from 1.63 to 3.84,resulting in a stronger liquid behavior and more sluggish crystallization kinetics for Gd_(55)Co_(20)Al_(24.5)Si_(0.5)metallic glass.Moreover,minor Si addition promotes the formation of a crystal-like structure with a size of 1-2 nm.The interactions between the crystal-like structures and other local favored clusters frustrate the further growth of crystal-like phases,thus stabilizes the amorphous structure.As a result,the glass-forming ability(GFA)was largely improved.The critical diameter of Gd_(55)Co_(20)Al_(25)metallic glass increased from 2 to 7 mm with 0.5 at.%Si addition without deterioration of the magnetocaloric effect.This study provides valuable insight for understanding the distinct effect of microalloying on GFA of metallic glasses from the aspect of the evolution of the liquid.展开更多
Developing novel magnetocaloric materials is of great significance for the applications of magnetic refrigeration.In this study,we designed a heterogeneous rare-earth-based high-entropy alloy(HEA)comprising amorphous ...Developing novel magnetocaloric materials is of great significance for the applications of magnetic refrigeration.In this study,we designed a heterogeneous rare-earth-based high-entropy alloy(HEA)comprising amorphous matrix,local crystal-like cluster and nanocrystalline dihydride with average size of 7.5 nm through isothermal hydrogenation.This heterogeneous structure can significantly tune the magnetocaloric effect of alloy.After hydrogenation,the predominant exchange interaction transforms from ferromagnetic to antiferromagnetic with the disappearance of spin-glass-like behavior,and a complete second-order magnetic transition is obtained.Compared with the Gd_(20)Tb_(18)Dy_(18)Co_(20)Al_(24) high-entropy metallic glass with a small number of nanocrystals,the maximum magnetic entropy change of the hydrogen-containing HEA is increased from 8.8 to 13.6 J kg^(-1)K^(-1) under applied magnetic field change of 5 T accompanying unobvious hysteresis and decreased magnetic transition temperature from 59 to 8 K,which is more promising as magnetic refrigerant at cryogenic temperature.This work provides a novel concept of designing heterogeneous structure in terms of special cluster and preferential nanocrystalline to modulate the properties of metallic glasses.展开更多
基金Project supported by the National Natural Science Foundation of China(52101193,51975183)China Postdoctoral Science Foundation(2022M711002)+2 种基金Fundamental Research Funds for the Central Universities(B220202036)the Natural Science Foundation of Jiangsu Province(BK20201316)Jiangsu Planned Projects for Postdoctoral Research Funds(2021K646C)。
文摘Rare earth high-entropy alloys(RE-HEAs)exhibit great potential to be applied as refrigerants due to their good comprehensive magnetocaloric properties.In this work,octary GdTbDyHoErTmCoAl and GdTbDyHoErTmCoNi RE-HEAs with amorphous/nanocrystalline structure exhibiting comparable magnetocaloric effect were synthesized.Both RE-HEAs show a second-order magnetic phase transition in the temperature range of hydrogen liquefaction.Due to the complex magnetic interactions,a spin glasslike behavior at low temperatures is observed in the RE-HEAs.A superior magnetocaloric effect is obtained in the nanocrystalline GdTbDyHoErTmCoNi high-entropy alloy that is multiphase attributed to a stronger magnetic exchange interaction when compared with the other that exhibits single amorphous structure.Despite heterogeneous microstructure,homogeneous chemical distributions are observed in the partially crystallized high-entropy alloy.In addition,the magnetocaloric effect and magnetic transition behavior of rare earth medium-and high-entropy alloys,including the RE-HEAs in this study,are summarized and discussed.The results in this work provide a helpful guide for the design of RE-HEAs for hydrogen liquefaction applications with excellent magnetocaloric effects.
基金Guangdong Major Project of Basic and Applied Basic Research,China(Grant No.2019B030302010)the National Natural Science Foundation of China(Grant Nos.52301212,52071222,52101191,52001219)+1 种基金the National Key Research and Development Program of China(Grant No.2021YFA0716302)Guangdong Basic and Applied Basic Research,China(Grant Nos.2022A1515010347,2020B1515130007).
文摘Soft magnetic composites(SMCs)play a pivotal role in the development of high-frequency,miniaturization and complex forming of modern electronics.However,they usually suffer from a trade-off between high magnetization and good magnetic softness(high permeability and low core loss).In this work,utilizing the order modulation strategy,a critical state in a FeSiBCCr amorphous soft magnetic composite(ASMC),consisting of massive crystal-like orders(CLOs,∼1 nm in size)with the feature ofα-Fe,is designed.This critical-state structure endows the amorphous powder with the enhanced ferromagnetic exchange interactions and the optimized magnetic domains with uniform orientation and fewer micro-vortex dots.Superior comprehensive soft magnetic properties at high frequency emerge in the ASMC,such as a high saturation magnetization(Ms)of 170 emu g^(-1)and effective permeability(µ_(e))of 65 combined with a core loss(Pcv)as low as 70 mW cm^(-3)(0.01 T,1 MHz).This study provides a new strategy for the development of high-frequency ASMCs,possessing suitable comprehensive soft magnetic performance to match the requirements of the modern magnetic devices used in the third-generation semiconductors and new energy fields.
基金supported by the National Natural Science Foundation of China(Grant Nos.51971061,52231005,and 52031016)the Fundamental Research Funds for the Central Universities(Grant No.2242020R10003).
文摘Comprehending the pressure-/temperature-induced structural transition in glasses,as one of the most fascinating issues in material science,is far from being well understood.Here,we report novel polyamorphic transitions in a Cu-based metallic glass(MG)with apparent nanoscale structural heterogeneity relating to proper Y addition.The low-density MG compresses continuously with increasing pressure,and then a compression plateau appears after∼8.1 GPa,evolving into an intermediate state with an ultrahigh bulk modulus of∼467 GPa.It then transforms to a high-density MG with significantly decreased structural heterogeneity above∼14.1 GPa.Three-dimensional atom probe tomography reveals concentration waves of Cu/Zr elements with an average wavelength of∼5-6 nm,which promote the formation of interconnected ringlike networks composed of Cu-rich and Zr-rich dual-glass domains at nanometer scale.Our experimental and simulation results indicate that steplike polyamorphism may stem from synergic effects of the abnormal compression of the Zr-Zr bond length at the atomic scale and the interplay between the applied pressure and incipient concentration waves(Cu and Zr)at several nanometer scales.The present work provides new insights into polyamorphism in glasses and contributes to the development of high-performance amorphous materials by high-pressure nanostructure engineering.
基金the National Natural Science Foundation of China(Nos.51631003,51571131,51971061 and 51471050)the National Key Research Program of China(No.2016YFB0300500)。
文摘Liquid dynamics plays an essential role in glass formation.Here we observed a distinct change of liquid dynamics in Gd_(55)Co_(20)Al_(25)metallic glass induced by microalloying Si element.In the equilibrium melt,minor Si(0.5 at.%)addition leads to a more fragile liquid behavior and a smaller strength of liquid-liquid transition with the transition strength(F)decreasing from 0.76 to 0.35.However,in the supercooled liquid,Si-doped liquid exhibits a remarkable enhanced fragile-to-strong transition(FST),and the value of FST factor f increases sharply from 1.63 to 3.84,resulting in a stronger liquid behavior and more sluggish crystallization kinetics for Gd_(55)Co_(20)Al_(24.5)Si_(0.5)metallic glass.Moreover,minor Si addition promotes the formation of a crystal-like structure with a size of 1-2 nm.The interactions between the crystal-like structures and other local favored clusters frustrate the further growth of crystal-like phases,thus stabilizes the amorphous structure.As a result,the glass-forming ability(GFA)was largely improved.The critical diameter of Gd_(55)Co_(20)Al_(25)metallic glass increased from 2 to 7 mm with 0.5 at.%Si addition without deterioration of the magnetocaloric effect.This study provides valuable insight for understanding the distinct effect of microalloying on GFA of metallic glasses from the aspect of the evolution of the liquid.
基金supported by the National Natural Science Foundation of China(Grant Nos.51631003,51971061 and 11674052)。
文摘Developing novel magnetocaloric materials is of great significance for the applications of magnetic refrigeration.In this study,we designed a heterogeneous rare-earth-based high-entropy alloy(HEA)comprising amorphous matrix,local crystal-like cluster and nanocrystalline dihydride with average size of 7.5 nm through isothermal hydrogenation.This heterogeneous structure can significantly tune the magnetocaloric effect of alloy.After hydrogenation,the predominant exchange interaction transforms from ferromagnetic to antiferromagnetic with the disappearance of spin-glass-like behavior,and a complete second-order magnetic transition is obtained.Compared with the Gd_(20)Tb_(18)Dy_(18)Co_(20)Al_(24) high-entropy metallic glass with a small number of nanocrystals,the maximum magnetic entropy change of the hydrogen-containing HEA is increased from 8.8 to 13.6 J kg^(-1)K^(-1) under applied magnetic field change of 5 T accompanying unobvious hysteresis and decreased magnetic transition temperature from 59 to 8 K,which is more promising as magnetic refrigerant at cryogenic temperature.This work provides a novel concept of designing heterogeneous structure in terms of special cluster and preferential nanocrystalline to modulate the properties of metallic glasses.
基金financially supported by Guangdong Major Project of Basic and Applied Basic Research,China (Grant No.2019B030302010)the National Natural Science Foundation of China (No.52301212,52071157,52071222)+1 种基金the National Key Research and Development Program of China (Grant No.2021YFA0716302)the open research fund of Songshan Lake Materials Laboratory (No.2022SLABFN11)。