Using a titration setup to accurately control the reaction conditions and in situ monitor the reaction,we showed that fluoride exhibited negligible effects on the ion association process of calcium and phosphate and t...Using a titration setup to accurately control the reaction conditions and in situ monitor the reaction,we showed that fluoride exhibited negligible effects on the ion association process of calcium and phosphate and the formation of ACP nanospheres in a buffer solution with constant ionic strength.However,the stability of ACP increased with increasing fluoride concentration,which was ascribed to the inhibitory effect of fluoride on the aggregation of ACP nanospheres and the nucleation of nanocrystals on the surface of ACP nanospheres.Furthermore,fluoride could inhibit the lateral growth of HAP nanosheets and promote the formation of rod-like crystals.These results further improve our understanding of the crystallization pathway of HAP crystals and the regulatory effects of fluoride.展开更多
Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries.Herein,we report a unique silicon-carbon composite fabricated by unifor...Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries.Herein,we report a unique silicon-carbon composite fabricated by uniformly dis-persing amorphous Si nanodots(SiNDs)in carbon nanospheres(SiNDs/C)that are welded on the wall of the macroporous carbon framework(MPCF)by vertical graphene(VG),labeled as MPCF@VG@SiNDs/C.The high dispersity and amor-phous features of ultrasmall SiNDs(~0.7 nm),the flexible and directed electron/Li+transport channels of VG,and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites,rapid Li+transport path,and unique low-strain property during Li+storage.Consequently,the MPCF@VG@SiNDs/C exhibits high cycle stability(1301.4 mAh g^(-1) at 1 A g^(-1) after 1000 cycles without apparent decay)and high rate capacity(910.3 mAh g^(-1),20 A g^(-1))in half cells based on industrial electrode standards.The assembled pouch full cell delivers a high energy density(1694.0 Wh L^(-1);602.8 Wh kg^(-1))and an excellent fast-charging capability(498.5 Wh kg^(-1),charging for 16.8 min at 3 C).This study opens new possibilities for preparing advanced silicon-carbon com-posite anodes for practical applications.展开更多
Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problem...Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problems like difficulty in preparation and poor cycling stability need to be solved.At present,Mg-based amorphous alloys applied in wastewater degradation are available in powder and ribbon.The amorphous alloy powder fabricated by ball milling has a high specific surface area,and its reactivity is thousands of times better than that of gas atomized alloy powder.But the development is limited due to the high energy consumption,difficult and costly process of powder recycling.The single roller melt-spinning method is a new manufacturing process of amorphous alloy ribbon.Compared to amorphous powder,the specific surface area of amorphous ribbon is relatively lower,therefore,it is necessary to carry out surface modification to enhance it.Dealloying is a way that can form a pore structure on the surface of the amorphous alloys,increasing the specific surface area and providing more reactive sites,which all contribute to the catalytic performance.Exploring the optimal conditions for Mg-based amorphous alloys in wastewater degradation by adjusting amorphous alloy composition,choosing suitable method to preparation and surface modification,reducing cost,expanding the pH range will advance the steps to put Mg-based amorphous alloys in industrial environments into practice.展开更多
Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are...Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.展开更多
Herein,ionomer-free amorphous iridium oxide(IrO_(x))thin electrodes are first developed as highly active anodes for proton exchange membrane electrolyzer cells(PEMECs)via low-cost,environmentally friendly,and easily s...Herein,ionomer-free amorphous iridium oxide(IrO_(x))thin electrodes are first developed as highly active anodes for proton exchange membrane electrolyzer cells(PEMECs)via low-cost,environmentally friendly,and easily scalable electrodeposition at room temperature.Combined with a Nafion 117 membrane,the IrO_(x)-integrated electrode with an ultralow loading of 0.075 mg cm^(-2)delivers a high cell efficiency of about 90%,achieving more than 96%catalyst savings and 42-fold higher catalyst utilization compared to commercial catalyst-coated membrane(2 mg cm^(-2)).Additionally,the IrO_(x)electrode demonstrates superior performance,higher catalyst utilization and significantly simplified fabrication with easy scalability compared with the most previously reported anodes.Notably,the remarkable performance could be mainly due to the amorphous phase property,sufficient Ir^(3+)content,and rich surface hydroxide groups in catalysts.Overall,due to the high activity,high cell efficiency,an economical,greatly simplified and easily scalable fabrication process,and ultrahigh material utilization,the IrO_(x)electrode shows great potential to be applied in industry and accelerates the commercialization of PEMECs and renewable energy evolution.展开更多
Electrocatalytic converting CO_(2) into chemical products has emerged as a promising approach to achieving carbon neutrality.Herein,we report a bismuth-based catalyst with high curvature terminal and amorphous layer w...Electrocatalytic converting CO_(2) into chemical products has emerged as a promising approach to achieving carbon neutrality.Herein,we report a bismuth-based catalyst with high curvature terminal and amorphous layer which fabricated via two-step electrodeposition achieves stable formate output in a wide voltage window of 600 mV.The Faraday efficiency(FE) of formate reached up to 99.4% at-0.8 V vs.RHE and it remained constant for more than 92 h at-15 mA cm^(-2).More intriguingly,FE formate of95.4% can be realized at a current density of industrial grade(-667.7 mA cm^(-2)) in flow cell.The special structure promoted CO_(2) adsorption and reduced its activation energy and enhanced the electric-thermal field and K^(+) enrichment which accelerated the reaction kinetics.In situ spectroscopy and theoretical calculation further confirmed that the introduction of amorphous structure is beneficial to adsorpting CO_(2)and stabling*OCHO intermediate.This work provides special insights to fabricate efficient electrocatalysts by means of structural and crystal engineering and makes efforts to realize the industrialization of bismuth-based catalysts.展开更多
Anelasticity, as an intrinsic property of amorphous solids, plays a significant role in understanding their relaxation and deformation mechanism. However, due to the lack of long-range order in amorphous solids, the s...Anelasticity, as an intrinsic property of amorphous solids, plays a significant role in understanding their relaxation and deformation mechanism. However, due to the lack of long-range order in amorphous solids, the structural origin of anelasticity and its distinction from plasticity remain elusive. In this work, using frozen matrix method, we study the transition from anelasticity to plasticity in a two-dimensional model glass. Three distinct mechanical behaviors, namely,elasticity, anelasticity, and plasticity, are identified with control parameters in the amorphous solid. Through the study of finite size effects on these mechanical behaviors, it is revealed that anelasticity can be distinguished from plasticity.Anelasticity serves as an intrinsic bridge connecting the elasticity and plasticity of amorphous solids. Additionally, it is observed that anelastic events are localized, while plastic events are subextensive. The transition from anelasticity to plasticity is found to resemble the entanglement of long-range interactions between element excitations. This study sheds light on the fundamental nature of anelasticity as a key property of element excitations in amorphous solids.展开更多
The atomic structure of amorphous alloys plays a crucial role in determining both their glass-forming ability and magnetic properties. In this study, we investigate the influence of adding the Y element on the glass-f...The atomic structure of amorphous alloys plays a crucial role in determining both their glass-forming ability and magnetic properties. In this study, we investigate the influence of adding the Y element on the glass-forming ability and magnetic properties of Fe_(86-x)Y_xB_7C_7(x = 0, 5, 10 at.%) amorphous alloys via both experiments and ab initio molecular dynamics simulations. Furthermore, we explore the correlation between local atomic structures and properties. Our results demonstrate that an increased Y content in the alloys leads to a higher proportion of icosahedral clusters, which can potentially enhance both glass-forming ability and thermal stability. These findings have been experimentally validated. The analysis of the electron energy density and magnetic moment of the alloy reveals that the addition of Y leads to hybridization between Y-4d and Fe-3d orbitals, resulting in a reduction in ferromagnetic coupling between Fe atoms. This subsequently reduces the magnetic moment of Fe atoms as well as the total magnetic moment of the system, which is consistent with experimental results. The results could help understand the relationship between atomic structure and magnetic property,and providing valuable insights for enhancing the performance of metallic glasses in industrial applications.展开更多
This work investigated the effect of Cr and Si on the mechanical properties and oxidation resistance of press hardened steel.Results indicated that the microstructure of the Cr-Si micro-alloyed press hardened steel co...This work investigated the effect of Cr and Si on the mechanical properties and oxidation resistance of press hardened steel.Results indicated that the microstructure of the Cr-Si micro-alloyed press hardened steel consisted of lath martensite,M_(23)C_(6)carbides,and retained austenite.The retained austenite and carbides are responsible for the increase in elongation of the micro-alloyed steel.In addition,after oxidation at 930℃for 5 min,the thickness of the oxide scales on the Cr-Si micro-alloyed press hardened steel is less than 5μm,much thinner than 45.50μm-thick oxide scales on 22MnB5.The oxide scales of the Cr-Si micro-alloyed steel are composed of Fe_(2)O_(3),Fe_(3)O_(4),mixed spinel oxide(FeCr_(2)O_(4)and Fe_(2)SiO_(4)),and amorphous SiO_(2).Adding Cr and Si significantly reduces the thickness of the oxide scales and prevents the generation of the FeO phase.Due to the increase of spinel FeCr_(2)O_(4)and Fe_(2)SiO_(4)phase in the inner oxide scale and the amorphous SiO_(2)close to the substrate,the oxidation resistance of the Cr-Si micro-alloyed press hardened steel is improved.展开更多
To date,there is still a lack of a comprehensive explanation for caged dynamics which is regarded as one of the intricate dynamic behaviors in amorphous alloys.This study focuses on Pd_(82)Si_(18)as the research objec...To date,there is still a lack of a comprehensive explanation for caged dynamics which is regarded as one of the intricate dynamic behaviors in amorphous alloys.This study focuses on Pd_(82)Si_(18)as the research object to further elucidate the underlying mechanism of caged dynamics from multiple perspectives,including the cage's lifetime,atomic local environment,and atomic potential energy.The results reveal that Si atoms exhibit a pronounced cage effect due to the hindrance of Pd atoms,resulting in an anomalous peak in the non-Gaussian parameters.An in-depth investigation was conducted on the caged dynamics differences between fast and slow Si atoms.In comparison to fast Si atoms,slow Si atoms were surrounded by more Pd atoms and occupied lower potential energy states,resulting in smaller diffusion displacements for the slow Si atoms.Concurrently,slow Si atoms tend to be in the centers of smaller clusters with coordination numbers of 9 and 10.During the isothermal relaxation process,clusters with coordination numbers 9 and 10 have longer lifetimes,suggesting that the escape of slow Si atoms from their cages is more challenging.The findings mentioned above hold significant implications for understanding the caged dynamics.展开更多
An a-C/a-C:N junction,which used palmyra sugar as the carbon source and ammonium hydroxide(NH4OH)as the dopant source,was successfully deposited on the ITO glass substrate using the nano-spraying method.The current-vo...An a-C/a-C:N junction,which used palmyra sugar as the carbon source and ammonium hydroxide(NH4OH)as the dopant source,was successfully deposited on the ITO glass substrate using the nano-spraying method.The current-voltage relationship of the junction was found to be a Schottky-like contact,and therefore the junction shows the characteristic rectifiers.This means the a-C and a-C:N are semiconductors with different types of conduction.Moreover,the samples showed an increase in current and voltage value when exposed to visible light(bright state)compared to the dark condition,thereby,indicating the creation of electron-hole pairs during the exposure.It was also discovered that the relationship between current and voltage for the a-C/a-C:N junction sample formed a curve that satisfies the rule of the photovoltaic effect when exposed to visible light from a light bulb.The exposure of this sample to direct sunlight at AM 1.5 conditions produced a curve that meets the rules for the emergence of the photovoltaic effect with higher characteristics for the current-voltage relationship.Thus,the a-C/a-C:N junction sample is a solar cell successfully fabricated using a sample method and has a maximum efficiency of 0.0013%.展开更多
The as-cast amorphous Ti_(48)Zr_(27)Cu_(6)Nb_(5)Be_(14)composites,comprising in situ formedβ-Ti ductile crystalline precipitates,were prepared by water cooled copper mold suction casting.Then,the semi-solid composite...The as-cast amorphous Ti_(48)Zr_(27)Cu_(6)Nb_(5)Be_(14)composites,comprising in situ formedβ-Ti ductile crystalline precipitates,were prepared by water cooled copper mold suction casting.Then,the semi-solid composites were obtained after the as-cast composites were treated by semi-solid isothermal treatment.The microstructure evolution and kinetics of the composites were examined.Results show that the microstructures of both the as-cast and semi-solid composites comprise ofβ-Ti crystal phases and amorphous matrix phases.Before and after treatment,the crystals evolve from fine granular or fine dendritic crystals to coarse crystals.As the treatment temperature increasing or the time prolonging,the average crystal size gradually increases and the surface morphology of the crystals gradually becomes regular.By studying the microstructural evolution and dynamics during the isothermal treatment process,it is found that the final morphology ofβ-Ti crystals is influenced by the isothermal treatment temperature and time(t),and theβ-Ti evolution rate increases with an increase in treatment temperature.In addition,a linear relationship was observed between the size of cubicβ-Ti crystals(D^(3))and t;the growth kinetics factor K is 3.8μm^(3)·s^(-1).As the K value closes to 4μm^(3)·s^(-1),it is inferred the morphology evolution ofβ-Ti crystals is a coarsening behavior controlled by the diffusion of solute elements.展开更多
Amorphous solid dispersion(ASD)is one of the most effective approaches for delivering poorly soluble drugs.In ASDs,polymeric materials serve as the carriers in which the drugs are dispersed at the molecular level.To p...Amorphous solid dispersion(ASD)is one of the most effective approaches for delivering poorly soluble drugs.In ASDs,polymeric materials serve as the carriers in which the drugs are dispersed at the molecular level.To prepare the solid dispersions,there are many polymers with various physicochemical and thermochemical characteristics available for use in ASD formulations.Polymer selection is of great importance because it influences the stability,solubility and dissolution rates,manufacturing process,and bioavailability of the ASD.This review article provides a comprehensive overview of ASDs from the perspectives of physicochemical characteristics of polymers,formulation designs and preparation methods.Furthermore,considerations of safety and regulatory requirements along with the studies recommended for characterizing and evaluating polymeric carriers are briefly discussed.展开更多
Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge pot...Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge potential.However,growing binder-free Si NW anodes with adequate mass loading and stable capacity is severely limited by the low surface area of planar current collectors(CCs),and is particularly challenging to achieve on standard pure-Cu substrates due to the ubiquitous formation of Li+inactive silicide phases.Here,the growth of densely-interwoven In-seeded Si NWs is facilitated by a thin-film of copper-silicide(CS)network in situ grown on a Cu-foil,allowing for a thin active NW layer(<10μm thick)and high areal loading(≈1.04 mg/cm^(2))binder-free electrode architecture.The electrode exhibits an average Coulombic efficiency(CE)of>99.6%and stable performance for>900 cycles with≈88.7%capacity retention.More significantly,it delivers a volumetric capacity of≈1086.1 m A h/cm^(3)at 5C.The full-cell versus lithium manganese oxide(LMO)cathode delivers a capacity of≈1177.1 m A h/g at 1C with a stable rate capability.This electrode architecture represents significant advances toward the development of binder-free Si NW electrodes for LIB application.展开更多
This manuscript explores the influences of the Foucault current on bracket vibration. Noise measurements are obtained in conditions that the coils are enclosed by the bracket, and exposed to the air for confirming the...This manuscript explores the influences of the Foucault current on bracket vibration. Noise measurements are obtained in conditions that the coils are enclosed by the bracket, and exposed to the air for confirming the impact of Foucault current on bracket vibration. The outcomes illustrate that the bracket increases the primary noise to 21 d B. Throughout investigational modal computation, ordinary frequencies of the coils stay afar from the exciting frequency of 100 Hz but the ordinary frequency 72.924 Hz of the bracket stands near to 100 Hz, which similarly explicates the upsurge of the noise level. To do the computations on bracket vibrations instigated by the Foucault current, a finite-element method(FEM) has been utilized for evaluating the eddy current density, electromagnetic forces(EMF), coupled with bracket response in frequency domain. The calculations displayed a proper approval by mean of theoretic investigations, and the simulations analyzed effectively the bracket vibration produced by Eddy current, and the electromagnetic force(EMF). Referring to the simulation, the primary vibration characteristics, and noise level, the method by applying weights(stress) on the top bracket of transformer is proposed to lessen the vibration amplitude, and noise level. To indorse the utility, and application of the suggested technique, the experiment results are obtained, analyzed, and compared with those of simulations, primary vibration characteristics, and noise level.展开更多
The work is dedicated to revealing the structural features of coals with different ranks,such as anthracites,metaanthracite and graphite,that determine their ability to crush and form fine dust.For this purpose,a comb...The work is dedicated to revealing the structural features of coals with different ranks,such as anthracites,metaanthracite and graphite,that determine their ability to crush and form fine dust.For this purpose,a combination of various nanoin-dentation techniques and Raman spectroscopy was used.The mechanical behavior of the selected coals was investigated by cyclic nanoindentation with increasing peak load and quasi-static loading.The alteration of the mechanical properties was studied by analysis of elastic moduli and damage indices Rw.Three groups of coals were identified based on their propensity to crushing during cyclic nanoindentation.Coals assigned to the first and second groups are characterized by local destruction in the contact zone with the indenter and the formation of a core of crushed material.Coals assigned to the third group are characterized by bulk destruction(outside the zone of contact with the indenter).In general,the ability of coals to fracture under mechanical loading decreases in the series of metamorphism due to microscale compaction of vitrinite matter.In the series of anthracite,metaanthracite and graphite,it is established that the coal matter compaction takes place for the anthracite and metaanthracite,whereas graphite reveals rather different behavior due to abrupt change of its structure.The ratios between the amorphous and crystalline phases of carbon(S)were determined by deconvolution of coals Raman spectra.The propensity of coals to crushing(a damage index Rw)increases with growth of the proportion of amorphous carbon in the coal matter.For the considered coals and metaanthracite,it is established that the proneness to destruction outside the contact zone with the indenter is determined by the ratio of amorphous and crystalline carbon of 1 and higher.When S parameter is lower than 1,the coals are being crushed only in the zone of contact with the indenter.展开更多
The rapid cooling of a metallic liquid(ML)results in short-range order(SRO)among the atomic arrangements and a disordered structure in the resulting metallic glass(MG).These phenomena cause various possible features i...The rapid cooling of a metallic liquid(ML)results in short-range order(SRO)among the atomic arrangements and a disordered structure in the resulting metallic glass(MG).These phenomena cause various possible features in the microscopic structure of the MG,presenting a puzzle about the nature of the MGs’microscopic structure beyond SRO.In this study,the nanoscale density gradient(NDG)originating from a sequential arrangement of clusters with different atomic packing densities(APDs),representing the medium-range structural heterogeneity in Zr_(60)Cu_(30)Al_(10)MG,was characterized using electron tomography(ET)combined with image simulations based on structure modeling.The coarse polyhedrons with distinct facets identified in the three-dimensional images coincide with icosahedron-like clusters and represent the spatial positions of clusters with high APDs.Rearrangements of the different clusters according to descending APD order in the glass-forming process are responsible for the NDG that stabilizes both the supercooled ML and the amorphous states and acts as a hidden rule in the transition from ML to MG.展开更多
Development of an electrocatalyst that is cheap and has good properties to replace conventional noble metals is important for H_(2) applications.In this study,dealloying of an amorphous Ti_(37)Cu_(60)Ru_(3) alloy was ...Development of an electrocatalyst that is cheap and has good properties to replace conventional noble metals is important for H_(2) applications.In this study,dealloying of an amorphous Ti_(37)Cu_(60)Ru_(3) alloy was performed to prepare a freestanding nanostructured hydrogen evolution reaction(HER)catalyst.The effect of dealloying and addition of Ru to TiCu alloys on the microstructure and HER properties under alkaline conditions was investigated.3 at.%Ru addition in Ti_(40)Cu_(60) decreases the overpotential to reach a current density of 10mA cm^(-2) and Tafel slope of the dealloyed samples to 35 and 34mV dec−1.The improvement of electrocatalytic properties was attributed to the formation of a nanostructure and the modification of the electronic structure of the catalyst.First-principles calculations based on density function theory indicate that Ru decreases the Gibbs free energy of water dissociation.This work presents a method to prepare an efficient electrocatalyst via dealloying of amorphous alloys.展开更多
Amorphous oxide semiconductors(AOS)have unique advantages in transparent and flexible thin film transistors(TFTs)applications,compared to low-temperature polycrystalline-Si(LTPS).However,intrinsic AOS TFTs are difficu...Amorphous oxide semiconductors(AOS)have unique advantages in transparent and flexible thin film transistors(TFTs)applications,compared to low-temperature polycrystalline-Si(LTPS).However,intrinsic AOS TFTs are difficult to obtain field-effect mobility(μFE)higher than LTPS(100 cm^(2)/(V·s)).Here,we design ZnAlSnO(ZATO)homojunction structure TFTs to obtainμFE=113.8 cm^(2)/(V·s).The device demonstrates optimized comprehensive electrical properties with an off-current of about1.5×10^(-11)A,a threshold voltage of–1.71 V,and a subthreshold swing of 0.372 V/dec.There are two kinds of gradient coupled in the homojunction active layer,which are micro-crystallization and carrier suppressor concentration gradient distribution so that the device can reduce off-current and shift the threshold voltage positively while maintaining high field-effect mobility.Our research in the homojunction active layer points to a promising direction for obtaining excellent-performance AOS TFTs.展开更多
基金Funded by the National Natural Science Foundation of China(No.52172287)the National Key Research and Development Program of China(No.2021YFA0715700)。
文摘Using a titration setup to accurately control the reaction conditions and in situ monitor the reaction,we showed that fluoride exhibited negligible effects on the ion association process of calcium and phosphate and the formation of ACP nanospheres in a buffer solution with constant ionic strength.However,the stability of ACP increased with increasing fluoride concentration,which was ascribed to the inhibitory effect of fluoride on the aggregation of ACP nanospheres and the nucleation of nanocrystals on the surface of ACP nanospheres.Furthermore,fluoride could inhibit the lateral growth of HAP nanosheets and promote the formation of rod-like crystals.These results further improve our understanding of the crystallization pathway of HAP crystals and the regulatory effects of fluoride.
基金All authors acknowledge fund support from Guangdong Basic and Applied Basic Research Foundation(2020A1515110762)National Natural Science Foundation of China(52172084).
文摘Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries.Herein,we report a unique silicon-carbon composite fabricated by uniformly dis-persing amorphous Si nanodots(SiNDs)in carbon nanospheres(SiNDs/C)that are welded on the wall of the macroporous carbon framework(MPCF)by vertical graphene(VG),labeled as MPCF@VG@SiNDs/C.The high dispersity and amor-phous features of ultrasmall SiNDs(~0.7 nm),the flexible and directed electron/Li+transport channels of VG,and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites,rapid Li+transport path,and unique low-strain property during Li+storage.Consequently,the MPCF@VG@SiNDs/C exhibits high cycle stability(1301.4 mAh g^(-1) at 1 A g^(-1) after 1000 cycles without apparent decay)and high rate capacity(910.3 mAh g^(-1),20 A g^(-1))in half cells based on industrial electrode standards.The assembled pouch full cell delivers a high energy density(1694.0 Wh L^(-1);602.8 Wh kg^(-1))and an excellent fast-charging capability(498.5 Wh kg^(-1),charging for 16.8 min at 3 C).This study opens new possibilities for preparing advanced silicon-carbon com-posite anodes for practical applications.
基金supported by the National Natural Science Foundation of China(Grant No.52071276)the Natural Science Foundation of Chongqing,China(Grant No.CSTB2022NSCQ-MSX0440)the Fundamental Research Funds for the Central Universities(Grant No.SWUXDJH202313,SWU-KQ22083).
文摘Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problems like difficulty in preparation and poor cycling stability need to be solved.At present,Mg-based amorphous alloys applied in wastewater degradation are available in powder and ribbon.The amorphous alloy powder fabricated by ball milling has a high specific surface area,and its reactivity is thousands of times better than that of gas atomized alloy powder.But the development is limited due to the high energy consumption,difficult and costly process of powder recycling.The single roller melt-spinning method is a new manufacturing process of amorphous alloy ribbon.Compared to amorphous powder,the specific surface area of amorphous ribbon is relatively lower,therefore,it is necessary to carry out surface modification to enhance it.Dealloying is a way that can form a pore structure on the surface of the amorphous alloys,increasing the specific surface area and providing more reactive sites,which all contribute to the catalytic performance.Exploring the optimal conditions for Mg-based amorphous alloys in wastewater degradation by adjusting amorphous alloy composition,choosing suitable method to preparation and surface modification,reducing cost,expanding the pH range will advance the steps to put Mg-based amorphous alloys in industrial environments into practice.
基金supported by National Natural Science Foundation of China(52373221,U1910208,52250119)the National Key R&D Program of China(2020YFA0710403)the Scientific Research Fund of Hunan Provincial Education Department(NO.23B0114).
文摘Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and selectivity.However,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts.In this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet arrays.Based on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution reaction.The hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C catalysts.This work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.
基金the support from the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Hydrogen and Fuel Cell Technologies Office Awards DE-EE0008426 and DE-EE0008423National Energy Technology Laboratory under Award DEFE0011585.
文摘Herein,ionomer-free amorphous iridium oxide(IrO_(x))thin electrodes are first developed as highly active anodes for proton exchange membrane electrolyzer cells(PEMECs)via low-cost,environmentally friendly,and easily scalable electrodeposition at room temperature.Combined with a Nafion 117 membrane,the IrO_(x)-integrated electrode with an ultralow loading of 0.075 mg cm^(-2)delivers a high cell efficiency of about 90%,achieving more than 96%catalyst savings and 42-fold higher catalyst utilization compared to commercial catalyst-coated membrane(2 mg cm^(-2)).Additionally,the IrO_(x)electrode demonstrates superior performance,higher catalyst utilization and significantly simplified fabrication with easy scalability compared with the most previously reported anodes.Notably,the remarkable performance could be mainly due to the amorphous phase property,sufficient Ir^(3+)content,and rich surface hydroxide groups in catalysts.Overall,due to the high activity,high cell efficiency,an economical,greatly simplified and easily scalable fabrication process,and ultrahigh material utilization,the IrO_(x)electrode shows great potential to be applied in industry and accelerates the commercialization of PEMECs and renewable energy evolution.
基金financial support from the Zhejiang Provincial Natural Science Foundation of China(LQ22B060007)the National Natural Science Foundation of China(22206042)+2 种基金the Scientific Research Start-up of Hangzhou Normal University(2021GDL014)the Hebei Natural Science Foundation(E2021203047)the Hebei Provincial Foundation for Returness(C20200369)。
文摘Electrocatalytic converting CO_(2) into chemical products has emerged as a promising approach to achieving carbon neutrality.Herein,we report a bismuth-based catalyst with high curvature terminal and amorphous layer which fabricated via two-step electrodeposition achieves stable formate output in a wide voltage window of 600 mV.The Faraday efficiency(FE) of formate reached up to 99.4% at-0.8 V vs.RHE and it remained constant for more than 92 h at-15 mA cm^(-2).More intriguingly,FE formate of95.4% can be realized at a current density of industrial grade(-667.7 mA cm^(-2)) in flow cell.The special structure promoted CO_(2) adsorption and reduced its activation energy and enhanced the electric-thermal field and K^(+) enrichment which accelerated the reaction kinetics.In situ spectroscopy and theoretical calculation further confirmed that the introduction of amorphous structure is beneficial to adsorpting CO_(2)and stabling*OCHO intermediate.This work provides special insights to fabricate efficient electrocatalysts by means of structural and crystal engineering and makes efforts to realize the industrialization of bismuth-based catalysts.
基金Project supported by Guangdong Major Project of Basic and Applied Basic Research,China (Grant No.2019B030302010)the National Natural Science Foundation of China (Grant No.52130108)+1 种基金Guangdong Basic and Applied Basic Research,China (Grant No.2021B1515140005)Pearl River Talent Recruitment Program (Grant No.2021QN02C04)。
文摘Anelasticity, as an intrinsic property of amorphous solids, plays a significant role in understanding their relaxation and deformation mechanism. However, due to the lack of long-range order in amorphous solids, the structural origin of anelasticity and its distinction from plasticity remain elusive. In this work, using frozen matrix method, we study the transition from anelasticity to plasticity in a two-dimensional model glass. Three distinct mechanical behaviors, namely,elasticity, anelasticity, and plasticity, are identified with control parameters in the amorphous solid. Through the study of finite size effects on these mechanical behaviors, it is revealed that anelasticity can be distinguished from plasticity.Anelasticity serves as an intrinsic bridge connecting the elasticity and plasticity of amorphous solids. Additionally, it is observed that anelastic events are localized, while plastic events are subextensive. The transition from anelasticity to plasticity is found to resemble the entanglement of long-range interactions between element excitations. This study sheds light on the fundamental nature of anelasticity as a key property of element excitations in amorphous solids.
基金Project supported by the National Key Research and Development Program of China(Grant No.2021YFB2401703)the National Natural Science Foundation of China(Grant Nos.52177005 and 51871234)the China Postdoctoral Science Foundation(Grant No.2022T150691)。
文摘The atomic structure of amorphous alloys plays a crucial role in determining both their glass-forming ability and magnetic properties. In this study, we investigate the influence of adding the Y element on the glass-forming ability and magnetic properties of Fe_(86-x)Y_xB_7C_7(x = 0, 5, 10 at.%) amorphous alloys via both experiments and ab initio molecular dynamics simulations. Furthermore, we explore the correlation between local atomic structures and properties. Our results demonstrate that an increased Y content in the alloys leads to a higher proportion of icosahedral clusters, which can potentially enhance both glass-forming ability and thermal stability. These findings have been experimentally validated. The analysis of the electron energy density and magnetic moment of the alloy reveals that the addition of Y leads to hybridization between Y-4d and Fe-3d orbitals, resulting in a reduction in ferromagnetic coupling between Fe atoms. This subsequently reduces the magnetic moment of Fe atoms as well as the total magnetic moment of the system, which is consistent with experimental results. The results could help understand the relationship between atomic structure and magnetic property,and providing valuable insights for enhancing the performance of metallic glasses in industrial applications.
基金The authors gratefully acknowledge the financial support from the National Natural Science Foundation of China(Nos.52274372 and 52201101)the National Key R&D Program of China(No.2021YFB3702404)the Fundamental Research Funds for the Central Universities(No.FRF-TP-22-013A1).
文摘This work investigated the effect of Cr and Si on the mechanical properties and oxidation resistance of press hardened steel.Results indicated that the microstructure of the Cr-Si micro-alloyed press hardened steel consisted of lath martensite,M_(23)C_(6)carbides,and retained austenite.The retained austenite and carbides are responsible for the increase in elongation of the micro-alloyed steel.In addition,after oxidation at 930℃for 5 min,the thickness of the oxide scales on the Cr-Si micro-alloyed press hardened steel is less than 5μm,much thinner than 45.50μm-thick oxide scales on 22MnB5.The oxide scales of the Cr-Si micro-alloyed steel are composed of Fe_(2)O_(3),Fe_(3)O_(4),mixed spinel oxide(FeCr_(2)O_(4)and Fe_(2)SiO_(4)),and amorphous SiO_(2).Adding Cr and Si significantly reduces the thickness of the oxide scales and prevents the generation of the FeO phase.Due to the increase of spinel FeCr_(2)O_(4)and Fe_(2)SiO_(4)phase in the inner oxide scale and the amorphous SiO_(2)close to the substrate,the oxidation resistance of the Cr-Si micro-alloyed press hardened steel is improved.
基金Project supported by the National Natural Science Foundation of China (Grant No.51701071)the Natural Science Foundation of Hunan Province,China (Grant Nos.2022JJ50115 and 2021JJ30179)the Research Foundation of the Education Bureau of Hunan Province,China (Grant No.22A0522)。
文摘To date,there is still a lack of a comprehensive explanation for caged dynamics which is regarded as one of the intricate dynamic behaviors in amorphous alloys.This study focuses on Pd_(82)Si_(18)as the research object to further elucidate the underlying mechanism of caged dynamics from multiple perspectives,including the cage's lifetime,atomic local environment,and atomic potential energy.The results reveal that Si atoms exhibit a pronounced cage effect due to the hindrance of Pd atoms,resulting in an anomalous peak in the non-Gaussian parameters.An in-depth investigation was conducted on the caged dynamics differences between fast and slow Si atoms.In comparison to fast Si atoms,slow Si atoms were surrounded by more Pd atoms and occupied lower potential energy states,resulting in smaller diffusion displacements for the slow Si atoms.Concurrently,slow Si atoms tend to be in the centers of smaller clusters with coordination numbers of 9 and 10.During the isothermal relaxation process,clusters with coordination numbers 9 and 10 have longer lifetimes,suggesting that the escape of slow Si atoms from their cages is more challenging.The findings mentioned above hold significant implications for understanding the caged dynamics.
基金funded by the University of Muhammadiyah Malang through a doctoral scientific work development program and also by theMinistry of Finance of Indonesia through the LPDP BUDI-DN scholarship(BP),and National Competitive Fundamental Research Grant(Hibah Penelitian Dasar),Kemendikbudristek,2021–2022(D).
文摘An a-C/a-C:N junction,which used palmyra sugar as the carbon source and ammonium hydroxide(NH4OH)as the dopant source,was successfully deposited on the ITO glass substrate using the nano-spraying method.The current-voltage relationship of the junction was found to be a Schottky-like contact,and therefore the junction shows the characteristic rectifiers.This means the a-C and a-C:N are semiconductors with different types of conduction.Moreover,the samples showed an increase in current and voltage value when exposed to visible light(bright state)compared to the dark condition,thereby,indicating the creation of electron-hole pairs during the exposure.It was also discovered that the relationship between current and voltage for the a-C/a-C:N junction sample formed a curve that satisfies the rule of the photovoltaic effect when exposed to visible light from a light bulb.The exposure of this sample to direct sunlight at AM 1.5 conditions produced a curve that meets the rules for the emergence of the photovoltaic effect with higher characteristics for the current-voltage relationship.Thus,the a-C/a-C:N junction sample is a solar cell successfully fabricated using a sample method and has a maximum efficiency of 0.0013%.
基金supported by the Natural Science Foundation of Hunan Province(No.2023JJ50453)the Science Research Excellent Youth Project of Hunan Educational Department(No.22B0777)+1 种基金the Key Scientific Research Project of Hunan Educational Department(No.22A0551)the Key Scientific Research Projects of Huaihua University(No.HHUY2022-13).
文摘The as-cast amorphous Ti_(48)Zr_(27)Cu_(6)Nb_(5)Be_(14)composites,comprising in situ formedβ-Ti ductile crystalline precipitates,were prepared by water cooled copper mold suction casting.Then,the semi-solid composites were obtained after the as-cast composites were treated by semi-solid isothermal treatment.The microstructure evolution and kinetics of the composites were examined.Results show that the microstructures of both the as-cast and semi-solid composites comprise ofβ-Ti crystal phases and amorphous matrix phases.Before and after treatment,the crystals evolve from fine granular or fine dendritic crystals to coarse crystals.As the treatment temperature increasing or the time prolonging,the average crystal size gradually increases and the surface morphology of the crystals gradually becomes regular.By studying the microstructural evolution and dynamics during the isothermal treatment process,it is found that the final morphology ofβ-Ti crystals is influenced by the isothermal treatment temperature and time(t),and theβ-Ti evolution rate increases with an increase in treatment temperature.In addition,a linear relationship was observed between the size of cubicβ-Ti crystals(D^(3))and t;the growth kinetics factor K is 3.8μm^(3)·s^(-1).As the K value closes to 4μm^(3)·s^(-1),it is inferred the morphology evolution ofβ-Ti crystals is a coarsening behavior controlled by the diffusion of solute elements.
基金the National Natural Science Foundation of China(No.81872813,22108313,82273880)Natural Science Foundation of Jiangsu Province(No.BK 20200573,BK 20200576)+1 种基金Fundamental Research Funds for the Central Universities(No 2632022ZD16)the Scientific Research Fund of Hunan Provincial Education Department(No.22B0820).
文摘Amorphous solid dispersion(ASD)is one of the most effective approaches for delivering poorly soluble drugs.In ASDs,polymeric materials serve as the carriers in which the drugs are dispersed at the molecular level.To prepare the solid dispersions,there are many polymers with various physicochemical and thermochemical characteristics available for use in ASD formulations.Polymer selection is of great importance because it influences the stability,solubility and dissolution rates,manufacturing process,and bioavailability of the ASD.This review article provides a comprehensive overview of ASDs from the perspectives of physicochemical characteristics of polymers,formulation designs and preparation methods.Furthermore,considerations of safety and regulatory requirements along with the studies recommended for characterizing and evaluating polymeric carriers are briefly discussed.
基金funded by the Science Foundation Ireland (SFI)under the Principal Investigator Program under contract No.11PI-1148,16/IA/4629 and SFI 16/M-ERA/3419funding under the European Union’s Horizon 2020 Research and Innovation Program+7 种基金grant agreement No.814464 (Si-DRIVE project)IRCLA/2017/285 and SFI Research Centres AMBER,Ma REI and CONFIRM 12/RC/2302_P2,12/RC/2278_P2,and 16/RC/3918SFI for SIRG grant No.18/SIRG/5484support from the Sustainable Energy Authority of Ireland through the Research Development and Demonstration Funding Program (Grant No.19/RDD/548)Enterprise Ireland through the Innovation Partnership Program (Grant No.IP 20190910)support from the SFI Research Centre Ma REI (award reference No.12/RC/2302_P2)support from the SFI Industry RD&I Fellowship Program (21/IRDIF/9876)the EU Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Individual Fellowship Grant (843621)。
文摘Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge potential.However,growing binder-free Si NW anodes with adequate mass loading and stable capacity is severely limited by the low surface area of planar current collectors(CCs),and is particularly challenging to achieve on standard pure-Cu substrates due to the ubiquitous formation of Li+inactive silicide phases.Here,the growth of densely-interwoven In-seeded Si NWs is facilitated by a thin-film of copper-silicide(CS)network in situ grown on a Cu-foil,allowing for a thin active NW layer(<10μm thick)and high areal loading(≈1.04 mg/cm^(2))binder-free electrode architecture.The electrode exhibits an average Coulombic efficiency(CE)of>99.6%and stable performance for>900 cycles with≈88.7%capacity retention.More significantly,it delivers a volumetric capacity of≈1086.1 m A h/cm^(3)at 5C.The full-cell versus lithium manganese oxide(LMO)cathode delivers a capacity of≈1177.1 m A h/g at 1C with a stable rate capability.This electrode architecture represents significant advances toward the development of binder-free Si NW electrodes for LIB application.
基金supported by the national science foundation of China (51767008)Jiangxi natural science foundation of China (20192ACBL20016)。
文摘This manuscript explores the influences of the Foucault current on bracket vibration. Noise measurements are obtained in conditions that the coils are enclosed by the bracket, and exposed to the air for confirming the impact of Foucault current on bracket vibration. The outcomes illustrate that the bracket increases the primary noise to 21 d B. Throughout investigational modal computation, ordinary frequencies of the coils stay afar from the exciting frequency of 100 Hz but the ordinary frequency 72.924 Hz of the bracket stands near to 100 Hz, which similarly explicates the upsurge of the noise level. To do the computations on bracket vibrations instigated by the Foucault current, a finite-element method(FEM) has been utilized for evaluating the eddy current density, electromagnetic forces(EMF), coupled with bracket response in frequency domain. The calculations displayed a proper approval by mean of theoretic investigations, and the simulations analyzed effectively the bracket vibration produced by Eddy current, and the electromagnetic force(EMF). Referring to the simulation, the primary vibration characteristics, and noise level, the method by applying weights(stress) on the top bracket of transformer is proposed to lessen the vibration amplitude, and noise level. To indorse the utility, and application of the suggested technique, the experiment results are obtained, analyzed, and compared with those of simulations, primary vibration characteristics, and noise level.
基金funded by the Russian Science Foundation grant (#18-77-10052).
文摘The work is dedicated to revealing the structural features of coals with different ranks,such as anthracites,metaanthracite and graphite,that determine their ability to crush and form fine dust.For this purpose,a combination of various nanoin-dentation techniques and Raman spectroscopy was used.The mechanical behavior of the selected coals was investigated by cyclic nanoindentation with increasing peak load and quasi-static loading.The alteration of the mechanical properties was studied by analysis of elastic moduli and damage indices Rw.Three groups of coals were identified based on their propensity to crushing during cyclic nanoindentation.Coals assigned to the first and second groups are characterized by local destruction in the contact zone with the indenter and the formation of a core of crushed material.Coals assigned to the third group are characterized by bulk destruction(outside the zone of contact with the indenter).In general,the ability of coals to fracture under mechanical loading decreases in the series of metamorphism due to microscale compaction of vitrinite matter.In the series of anthracite,metaanthracite and graphite,it is established that the coal matter compaction takes place for the anthracite and metaanthracite,whereas graphite reveals rather different behavior due to abrupt change of its structure.The ratios between the amorphous and crystalline phases of carbon(S)were determined by deconvolution of coals Raman spectra.The propensity of coals to crushing(a damage index Rw)increases with growth of the proportion of amorphous carbon in the coal matter.For the considered coals and metaanthracite,it is established that the proneness to destruction outside the contact zone with the indenter is determined by the ratio of amorphous and crystalline carbon of 1 and higher.When S parameter is lower than 1,the coals are being crushed only in the zone of contact with the indenter.
基金supported by the National Natural Science Foundation of China(51971093,52192603,and 51501043)。
文摘The rapid cooling of a metallic liquid(ML)results in short-range order(SRO)among the atomic arrangements and a disordered structure in the resulting metallic glass(MG).These phenomena cause various possible features in the microscopic structure of the MG,presenting a puzzle about the nature of the MGs’microscopic structure beyond SRO.In this study,the nanoscale density gradient(NDG)originating from a sequential arrangement of clusters with different atomic packing densities(APDs),representing the medium-range structural heterogeneity in Zr_(60)Cu_(30)Al_(10)MG,was characterized using electron tomography(ET)combined with image simulations based on structure modeling.The coarse polyhedrons with distinct facets identified in the three-dimensional images coincide with icosahedron-like clusters and represent the spatial positions of clusters with high APDs.Rearrangements of the different clusters according to descending APD order in the glass-forming process are responsible for the NDG that stabilizes both the supercooled ML and the amorphous states and acts as a hidden rule in the transition from ML to MG.
基金National Natural Science Foundation of China,Grant/Award Number:52071217。
文摘Development of an electrocatalyst that is cheap and has good properties to replace conventional noble metals is important for H_(2) applications.In this study,dealloying of an amorphous Ti_(37)Cu_(60)Ru_(3) alloy was performed to prepare a freestanding nanostructured hydrogen evolution reaction(HER)catalyst.The effect of dealloying and addition of Ru to TiCu alloys on the microstructure and HER properties under alkaline conditions was investigated.3 at.%Ru addition in Ti_(40)Cu_(60) decreases the overpotential to reach a current density of 10mA cm^(-2) and Tafel slope of the dealloyed samples to 35 and 34mV dec−1.The improvement of electrocatalytic properties was attributed to the formation of a nanostructure and the modification of the electronic structure of the catalyst.First-principles calculations based on density function theory indicate that Ru decreases the Gibbs free energy of water dissociation.This work presents a method to prepare an efficient electrocatalyst via dealloying of amorphous alloys.
基金supported by National Natural Science Foundation of China(No.U20A20209)Zhejiang Provincial Natural Science Foundation of China(LD19E020001)+1 种基金Zhejiang Provincial Key Research and Development Program(2021C01030)"Pioneer"and"Leading Goose"R&D Program of Zhejiang Province(2021C01SA301612)。
文摘Amorphous oxide semiconductors(AOS)have unique advantages in transparent and flexible thin film transistors(TFTs)applications,compared to low-temperature polycrystalline-Si(LTPS).However,intrinsic AOS TFTs are difficult to obtain field-effect mobility(μFE)higher than LTPS(100 cm^(2)/(V·s)).Here,we design ZnAlSnO(ZATO)homojunction structure TFTs to obtainμFE=113.8 cm^(2)/(V·s).The device demonstrates optimized comprehensive electrical properties with an off-current of about1.5×10^(-11)A,a threshold voltage of–1.71 V,and a subthreshold swing of 0.372 V/dec.There are two kinds of gradient coupled in the homojunction active layer,which are micro-crystallization and carrier suppressor concentration gradient distribution so that the device can reduce off-current and shift the threshold voltage positively while maintaining high field-effect mobility.Our research in the homojunction active layer points to a promising direction for obtaining excellent-performance AOS TFTs.