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
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
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
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
Separated preparation of prealloys and amorphous alloys results in severe solidification-remelting and beneficial element removal-readdition contradictions,which markedly increase energy consumption and emissions.This...Separated preparation of prealloys and amorphous alloys results in severe solidification-remelting and beneficial element removal-readdition contradictions,which markedly increase energy consumption and emissions.This study offered a novel strategy for the direct production of FePC amorphous soft magnetic alloys via smelting reduction of high-phosphorus iron ore(HPIO)and apatite.First,the thermodynamic conditions and equilibrium states of the carbothermal reduction reactions in HPIO were calculated,and the element content in reduced alloys was theoretically determined.The phase and structural evolutions,as well as element migration and enrichment behaviors during the smelting reduction of HPIO and Ca_(3)(PO_(4))_(2),were then experimentally verified.The addition of Ca_(3)(PO_(4))_(2)in HPIO contributes to the enrichment of the P element in reduced alloys and the subsequent development of Fe_(3)P and Fe_(2)P phases.The content of P and C elements in the range of 1.52 wt% -14.63 wt% and 0.62 wt% -2.47 wt%,respectively,can be well tailored by adding 0-50 g Ca_(3)(PO_(4))_(2)and controlling the C/O mole ratio of 0.8-1.1,which is highly consistent with the calculated results.These FePC alloys were then successfully formed into amorphous ribbons and rods.The energy consumption of the proposed strategy was estimated to be 2.00×10^(8) kJ/t,which is reduced by 30% when compared with the conventional production process.These results are critical for the comprehensive utilization of mineral resources and pave the way for the clean production of Fe-based amorphous soft magnetic alloys.展开更多
For electromagnetic wave-absorbing materials,maximizing absorption at a specific frequency has been constantly achieved,but enhancing the absorption properties in the entire band remains a challenge.In this work,a 3D ...For electromagnetic wave-absorbing materials,maximizing absorption at a specific frequency has been constantly achieved,but enhancing the absorption properties in the entire band remains a challenge.In this work,a 3D porous pyrolytic carbon(PyC)foam matrix was synthesized by a template method.Amorphous carbon nanotubes(CNTs)were then in-situ grown on the matrix surface to obtain ultralight CNTs/Py C foam.These in-situ grown amorphous CNTs were distributed uniformly and controlled by the catalytic growth time and can enhance the interface polarization and conduction loss of composites.When the electromagnetic wave enters the internal holes,the electromagnetic energy can be completely attenuated under the combined action of polarization,conductivity loss,and multiple reflections.The ultralight CNTs/Py C foam had a density of 22.0 mg·cm^(-3)and a reflection coefficient lower than-13.3 d B in the whole X-band(8.2-12.4 GHz),which is better than the conventional standard of effective absorption bandwidth(≤-10 dB).The results provide ideas for researching ultralight and strong electromagnetic wave absorbing materials in the X-band.展开更多
Developing advanced electrode materials is crucial for improving the electrochemical performances of proton batteries.Currently,the anodes are primarily crystalline materials which suffer from inferior cyclic stabilit...Developing advanced electrode materials is crucial for improving the electrochemical performances of proton batteries.Currently,the anodes are primarily crystalline materials which suffer from inferior cyclic stability and high electrode potential.Herein,we propose amorphous electrode materials for proton batteries by using a general ion-exchange protocol to introduce multivalent metal cations for activating the host material.Taking Al^(3+)as an example,theoretical and experimental analysis demonstrates electrostatic interaction between metal cations and lattice oxygen,which is the primary barrier for direct introduction of the multivalent cations,is effectively weakened through ion exchange between Al^(3+)and pre-intercalated K+.The as-prepared Al-MoOx anode therefore delivered a remarkable capacity and outstanding cycling stability that outperforms most of the state-of-the-art counterparts.The assembled full cell also achieved a high voltage of 1.37 V.This work opens up new opportunities for developing high-performance electrodes of proton batteries by introducing amorphous materials.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
Defining the structure characteristics of amorphous materials is one of the fundamental problems that need to be solved urgently in complex materials because of their complex structure and long-range disorder.In this ...Defining the structure characteristics of amorphous materials is one of the fundamental problems that need to be solved urgently in complex materials because of their complex structure and long-range disorder.In this study,we develop an interpretable deep learning model capable of accurately classifying amorphous configurations and characterizing their structural properties.The results demonstrate that the multi-dimensional hybrid convolutional neural network can classify the two-dimensional(2D)liquids and amorphous solids of molecular dynamics simulation.The classification process does not make a priori assumptions on the amorphous particle environment,and the accuracy is 92.75%,which is better than other convolutional neural networks.Moreover,our model utilizes the gradient-weighted activation-like mapping method,which generates activation-like heat maps that can precisely identify important structures in the amorphous configuration maps.We obtain an order parameter from the heatmap and conduct finite scale analysis of this parameter.Our findings demonstrate that the order parameter effectively captures the amorphous phase transition process across various systems.These results hold significant scientific implications for the study of amorphous structural characteristics via deep learning.展开更多
Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from...Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from the low intrinsic electronic conductivity,sluggish ions diffusion kinetics,and structural collapse,hindering their large-scale application.Herein,we successfully developed a latent amorphous Mn_(1.8)Fe_(1.2)O_(4) hollow nanocube(a-H-MnFeO) cathode material derived from Prussian blue analogue precursor.The amorphous nature endows the cathode with lower diffusion barrier and narrower band gap compared with crystalline counterpart,resulting in the superior Zn^(2+) ions and electrons transport kinetics.Hollow structure can furnish abundant surface sites and suppress the structural collapse during the repeated charge/discharge processes.By virtue of the multiple advantageous features,the a-H-MnFeO cathode exhibits exceptional electrochemical performance,in terms of high capacity,excellent rate capability,and prolonged cycle life.This strategy will pave the way for the structural design of emerging cathode materials.展开更多
As growing applications demand higher driving currents of oxide semiconductor thin-film transistors(TFTs),severe instabilities and even hard breakdown under high-current stress(HCS)become critical challenges.In this w...As growing applications demand higher driving currents of oxide semiconductor thin-film transistors(TFTs),severe instabilities and even hard breakdown under high-current stress(HCS)become critical challenges.In this work,the triggering voltage of HCS-induced self-heating(SH)degradation is defined in the output characteristics of amorphous indium-galliumzinc oxide(a-IGZO)TFTs,and used to quantitatively evaluate the thermal generation process of channel donor defects.The fluorinated a-IGZO(a-IGZO:F)was adopted to effectively retard the triggering of the self-heating(SH)effect,and was supposed to originate from the less population of initial deep-state defects and a slower rate of thermal defect transition in a-IGZO:F.The proposed scheme noticeably enhances the high-current applications of oxide TFTs.展开更多
Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive r...Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.展开更多
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 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financially supported by the National Natural Science Foundation of China(Nos.52174217 and 52304354)the China Postdoctoral Science Foundation(No.2020M682495)。
文摘Separated preparation of prealloys and amorphous alloys results in severe solidification-remelting and beneficial element removal-readdition contradictions,which markedly increase energy consumption and emissions.This study offered a novel strategy for the direct production of FePC amorphous soft magnetic alloys via smelting reduction of high-phosphorus iron ore(HPIO)and apatite.First,the thermodynamic conditions and equilibrium states of the carbothermal reduction reactions in HPIO were calculated,and the element content in reduced alloys was theoretically determined.The phase and structural evolutions,as well as element migration and enrichment behaviors during the smelting reduction of HPIO and Ca_(3)(PO_(4))_(2),were then experimentally verified.The addition of Ca_(3)(PO_(4))_(2)in HPIO contributes to the enrichment of the P element in reduced alloys and the subsequent development of Fe_(3)P and Fe_(2)P phases.The content of P and C elements in the range of 1.52 wt% -14.63 wt% and 0.62 wt% -2.47 wt%,respectively,can be well tailored by adding 0-50 g Ca_(3)(PO_(4))_(2)and controlling the C/O mole ratio of 0.8-1.1,which is highly consistent with the calculated results.These FePC alloys were then successfully formed into amorphous ribbons and rods.The energy consumption of the proposed strategy was estimated to be 2.00×10^(8) kJ/t,which is reduced by 30% when compared with the conventional production process.These results are critical for the comprehensive utilization of mineral resources and pave the way for the clean production of Fe-based amorphous soft magnetic alloys.
基金supported by the National Natural Science Foundation of China(No.51702197)Creative Research Foundation of the Science and Technology on Thermostructural Composite Materials Laboratory,the Natural Science Foundation of Shaanxi Province(No.2022JM248)the Doctoral Scientific Research Foundation of Shaanxi University of Science&Technology(No.BJ16-06)。
文摘For electromagnetic wave-absorbing materials,maximizing absorption at a specific frequency has been constantly achieved,but enhancing the absorption properties in the entire band remains a challenge.In this work,a 3D porous pyrolytic carbon(PyC)foam matrix was synthesized by a template method.Amorphous carbon nanotubes(CNTs)were then in-situ grown on the matrix surface to obtain ultralight CNTs/Py C foam.These in-situ grown amorphous CNTs were distributed uniformly and controlled by the catalytic growth time and can enhance the interface polarization and conduction loss of composites.When the electromagnetic wave enters the internal holes,the electromagnetic energy can be completely attenuated under the combined action of polarization,conductivity loss,and multiple reflections.The ultralight CNTs/Py C foam had a density of 22.0 mg·cm^(-3)and a reflection coefficient lower than-13.3 d B in the whole X-band(8.2-12.4 GHz),which is better than the conventional standard of effective absorption bandwidth(≤-10 dB).The results provide ideas for researching ultralight and strong electromagnetic wave absorbing materials in the X-band.
基金supported by the National Natural Science Foundation of China(51904059)Applied Basic Research Program of Liaoning(2022JH2/101300200)+1 种基金Fundamental Research Funds for the Central Universities(N2002005,N2125004,N2225044)Liao Ning Revitalization Talents Program(XLYC1807123).
文摘Developing advanced electrode materials is crucial for improving the electrochemical performances of proton batteries.Currently,the anodes are primarily crystalline materials which suffer from inferior cyclic stability and high electrode potential.Herein,we propose amorphous electrode materials for proton batteries by using a general ion-exchange protocol to introduce multivalent metal cations for activating the host material.Taking Al^(3+)as an example,theoretical and experimental analysis demonstrates electrostatic interaction between metal cations and lattice oxygen,which is the primary barrier for direct introduction of the multivalent cations,is effectively weakened through ion exchange between Al^(3+)and pre-intercalated K+.The as-prepared Al-MoOx anode therefore delivered a remarkable capacity and outstanding cycling stability that outperforms most of the state-of-the-art counterparts.The assembled full cell also achieved a high voltage of 1.37 V.This work opens up new opportunities for developing high-performance electrodes of proton batteries by introducing amorphous materials.
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.
基金National Natural Science Foundation of China(Grant No.11702289)the Key Core Technology and Generic Technology Research and Development Project of Shanxi Province,China(Grant No.2020XXX013)the National Key Research and Development Project of China。
文摘Defining the structure characteristics of amorphous materials is one of the fundamental problems that need to be solved urgently in complex materials because of their complex structure and long-range disorder.In this study,we develop an interpretable deep learning model capable of accurately classifying amorphous configurations and characterizing their structural properties.The results demonstrate that the multi-dimensional hybrid convolutional neural network can classify the two-dimensional(2D)liquids and amorphous solids of molecular dynamics simulation.The classification process does not make a priori assumptions on the amorphous particle environment,and the accuracy is 92.75%,which is better than other convolutional neural networks.Moreover,our model utilizes the gradient-weighted activation-like mapping method,which generates activation-like heat maps that can precisely identify important structures in the amorphous configuration maps.We obtain an order parameter from the heatmap and conduct finite scale analysis of this parameter.Our findings demonstrate that the order parameter effectively captures the amorphous phase transition process across various systems.These results hold significant scientific implications for the study of amorphous structural characteristics via deep learning.
基金funding supported by the National Natural Science Foundation of China (52101246)the Fundamental Research Funds for the Central Universities+1 种基金the Natural Science Foundation of Heilongjiang Province, China (YQ2022B006)the funding supported by the Natural Science Foundation of Anhui Province (2208085MB21)。
文摘Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from the low intrinsic electronic conductivity,sluggish ions diffusion kinetics,and structural collapse,hindering their large-scale application.Herein,we successfully developed a latent amorphous Mn_(1.8)Fe_(1.2)O_(4) hollow nanocube(a-H-MnFeO) cathode material derived from Prussian blue analogue precursor.The amorphous nature endows the cathode with lower diffusion barrier and narrower band gap compared with crystalline counterpart,resulting in the superior Zn^(2+) ions and electrons transport kinetics.Hollow structure can furnish abundant surface sites and suppress the structural collapse during the repeated charge/discharge processes.By virtue of the multiple advantageous features,the a-H-MnFeO cathode exhibits exceptional electrochemical performance,in terms of high capacity,excellent rate capability,and prolonged cycle life.This strategy will pave the way for the structural design of emerging cathode materials.
基金supported by National Key Research and Development Program under Grant No.2022YFB3607100Shenzhen Research Programs under Grant Nos.JCYJ20200109140601691,JCYJ20190808154803565,SGDX20201103095607022,SGDX20211123145404006,and GXWD20201231165807007-20200807025846001。
文摘As growing applications demand higher driving currents of oxide semiconductor thin-film transistors(TFTs),severe instabilities and even hard breakdown under high-current stress(HCS)become critical challenges.In this work,the triggering voltage of HCS-induced self-heating(SH)degradation is defined in the output characteristics of amorphous indium-galliumzinc oxide(a-IGZO)TFTs,and used to quantitatively evaluate the thermal generation process of channel donor defects.The fluorinated a-IGZO(a-IGZO:F)was adopted to effectively retard the triggering of the self-heating(SH)effect,and was supposed to originate from the less population of initial deep-state defects and a slower rate of thermal defect transition in a-IGZO:F.The proposed scheme noticeably enhances the high-current applications of oxide TFTs.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government,Ministry of Science and ICT(MSIT)(NRF-2020M3D1A2102837)the Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(20214000000500,training program of CCUS for the green growth)。
文摘Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.
