Two novel diketopiperazines(1 and 5),along with ten known compounds(2−4,6−12)demonstrating significant skin inflammation inhibition,were isolated from a marine-derived fungus identified as Aspergillus sp.FAZW0001.The ...Two novel diketopiperazines(1 and 5),along with ten known compounds(2−4,6−12)demonstrating significant skin inflammation inhibition,were isolated from a marine-derived fungus identified as Aspergillus sp.FAZW0001.The structural elucidation and configurational reassessments of compounds 1−5 were established through comprehensive spectral analyses,with their absolute configurations determined via single crystal X-ray diffraction using Cu Kαradiation,Marfey’s method,and comparison between experimental and calculated electronic circular dichroism(ECD)spectra.Compounds 1,2,and 8 exhibited significant anti-inflammatory activities in Propionibacterium acnes(P.acnes)-induced human monocyte cell lines.Compound 8 demonstrated the ability to down-regulate interleukin-1β(IL-1β)expression by inhibiting Toll-like receptor 2(TLR2)expression and modulating the activation of myeloid differentiation factor 88(MyD88),mitogen-activated protein kinase(MAPK),and nuclear factorκB(NF-κB)signaling pathways,thus reducing the cellular inflammatory response induced by P.acnes.Additionally,compound 8 showed the capacity to suppress mitochondrial reactive oxygen species(ROS)production and nucleotide-binding oligomerization domain-like receptor protein 3(NLRP3)inflammasome activation,thereby reducing IL-1βmaturation and secretion.A three-dimensional quantitative structure-activity relationships(3D-QSAR)model was applied to compounds 5−12 to analyze their anti-inflammatory structure-activity relationships.展开更多
The promotion of energy efficiency(EE)helps address energy constraints and promote environmental sustainability.This study comprehensively explores the spatiotemporal variations,influencing factors,and configuration p...The promotion of energy efficiency(EE)helps address energy constraints and promote environmental sustainability.This study comprehensively explores the spatiotemporal variations,influencing factors,and configuration promotion paths of EE in 284 Chinese cities during 2003‒2019 using the global super-efficiency minimum distance to strong efficient frontier(G-S-MinDS),exploratory spatial data analysis(ESDA),multiscale geographically weighted regression(MGWR),and fuzzy set qualitative comparative analysis(fsQCA)methods.The findings are:①China’s cities have an annual average EE of 0.658 with a growth rate of 0.53%,showing considerable promotion potential.②Industrial structure optimization,population agglomeration,economic development,and increased green coverage contribute positively,while government intervention and openness hinder China’s urban EE.③Four configurational promotion paths for enhancing China’s urban EE are identified,where among those paths population density is a core condition,while government intervention is not.This study provides valuable insights into substantially improving urban EE,emphasizing the need for targeted policies to address energy and environmental crises in China.展开更多
Configurational information entropy(CIE)theory was employed to determine the neutron-skin thickness of neutron-rich calcium isotopes.The nuclear density distributions and fragment cross sections in 350 MeV/u ^(40-60)C...Configurational information entropy(CIE)theory was employed to determine the neutron-skin thickness of neutron-rich calcium isotopes.The nuclear density distributions and fragment cross sections in 350 MeV/u ^(40-60)Ca+^(9)Be projectile fragmentation reactions were calculated using a modified statistical abrasion-ablation model.CIE quantities were determined from the nuclear density,isotopic,mass,and charge distributions.The linear correlations between the CIE determined using the isotopic,mass,and charge distributions and the neutron-skin thickness of the projectile nucleus show that CIE provides new methods to extract the neutron-skin thickness of neutron-rich nuclei.展开更多
ABX_(2)(A=Ag,Na,Cu;B=Sb,Bi;X=S,Se,Te)(GroupsⅠ-Ⅴ-Ⅵ_(2))compounds,which are all characterized by the ultralow lattice thermal conductivity because of their strong lattice anharmonicity caused by lone-pair electrons,h...ABX_(2)(A=Ag,Na,Cu;B=Sb,Bi;X=S,Se,Te)(GroupsⅠ-Ⅴ-Ⅵ_(2))compounds,which are all characterized by the ultralow lattice thermal conductivity because of their strong lattice anharmonicity caused by lone-pair electrons,have aroused wide attention in thermoelectric community.The practical application of thermoelectric devices usually requires both the compatible n-type and p-type materials simultaneously.However,most ofⅠ-Ⅴ-Ⅵ_(2)compounds are intrinsic p-type semiconductors,lacking their n-type counterparts for thermoelectrics.Herein,in this work,we increase the configuration entropy of AgBiTe_(2)by alloying SnTe,in order to stabilize the cubic phase at room temperature.With further optimization of thermal and electrical performance,the thermoelectric performance could be improved simultaneously in both n-and p-type(AgBiTe_(2))_(1-x)(SnTe)_(x)(x=0.3,0.4)solid solutions.Finally,p-type compound with the nominal composition of(AgBi_(0.99)Cd_(0.01)Te_(2))_(0.6)(SnTe)_(0.4)and n-type of(AgBiTe_(2))_(0.7)(SnTe)_(0.3)~Br 6%show the maximum zT of~0.33 and~0.21,at 381 and 423 K,respectively.展开更多
Configurational information entropy(CIE)analysis has been shown to be applicable for determining the neutron skin thickness(δnp)of neutron-rich nuclei from fragment production in projectile fragmentation reactions.Th...Configurational information entropy(CIE)analysis has been shown to be applicable for determining the neutron skin thickness(δnp)of neutron-rich nuclei from fragment production in projectile fragmentation reactions.The BNN+FRACS machine learning model was adopted to predict the fragment mass cross-sections(σ_(A))of the projectile fragmentation reactions induced by calcium isotopes from ^(36)Ca to ^(56)Ca on a ^(9)Be target at 140MeV/u.The fast Fourier transform was adopted to decompose the possible information compositions inσA distributions and determine the quantity of CIE(S_(A)[f]).It was found that the range of fragments significantly influences the quantity of S_(A)[f],which results in different trends of S_(A)[f]~δnp correlation.The linear S_(A)[f]~δnp correlation in a previous study[Nucl.Sci.Tech.33,6(2022)]could be reproduced using fragments with relatively large mass fragments,which verifies that S_(A)[f]determined from fragmentσAis sensitive to the neutron skin thickness of neutron-rich isotopes.展开更多
The spinel-type LiMn_(2)O_(4) is a promising candidate as cathode material for rechargeable Li-ion batteries due to its good thermal stability and safety.Experimentally,it is observed that in this compound there occur...The spinel-type LiMn_(2)O_(4) is a promising candidate as cathode material for rechargeable Li-ion batteries due to its good thermal stability and safety.Experimentally,it is observed that in this compound there occur the structural phase transitions from cubic(Fd3m)to tetragonal(I4_(1)/amd)phase at slightly below room temperature.To understand the phase transition mechanism,we compare the Gibbs free energy between cubic phase and tetragonal phase by including the configurational entropy.Our results show that the configurational entropy contributes substantially to the stability of the cubic phase at room temperature due to the disordered Mn^(3+)/Mn^(4+)distribution as well as the orientation of the Jahn-Teller elongation of the Mn^(3+)O_(6) octahedron in the the spinel phase.Meanwhile,the phase transition temperature is predicted to be 267.8 K,which is comparable to the experimentally observed temperature.These results serve as a good complement to the experimental study,and are beneficial to the improving of the electrochemical performance of LiMn_(2)O_(4) cathode.展开更多
Metallic amorphous/crystalline(A/C)nanolaminates exhibit excellent ductility while retaining their high strength.However,the underlying physical mechanisms and the resultant structural changes during plastic deformati...Metallic amorphous/crystalline(A/C)nanolaminates exhibit excellent ductility while retaining their high strength.However,the underlying physical mechanisms and the resultant structural changes during plastic deformation still remain unclear.In the present work,the structure-property relationship of CuZr/Cu A/C nanolaminates is established through integrated high-throughput micro-compression tests and molecular dynamics simulations together with high-resolution transmission electron microcopy.The serrated flow of nanolaminates results from the formation of hexagonal-close-packed(HCP)-type stacking faults and twins inside the face-centered-cubic(FCC)Cu nano-grains,the body-centered-cubic(BCC)-type ordering at their grain boundaries,and the crystallization of the amorphous CuZr layers.The serration behavior of CuZr/Cu A/C nanolaminates is determined by several factors,including the formation of dense dislocation networks from the multiplication of initial dislocations that formed after yielding,weak-spots-related configurational-transitions and shear-transition-zone activities,and deformation-induced devitrification.The present work provides an insight into the heterogeneous deformation mechanism of A/C nanolaminates at the atomic scale,and mechanistic base for the microstructural design of self-toughening metallic-glass(MG)-based composites and A/C nanolaminates.展开更多
A full-relaxation optimization of molecule and the popular MM2 force field are employed to obtain the geometry parameters and the conformational energy surface of a meso or a racemic dyad of poly(methyl acrylate) (PMA...A full-relaxation optimization of molecule and the popular MM2 force field are employed to obtain the geometry parameters and the conformational energy surface of a meso or a racemic dyad of poly(methyl acrylate) (PMA) with a specified carbonyl-bond orientation in side-groups. It is found that the conformational energy maps calculated here considerably differ from those calculated with the rigid molecular model as reported in the earlier studies. The g(-) state cannot be omitted in the obtained contour maps. Two important conformers tg(-) and g(-t) with energy minima were newly detected for a racemic dyad. The analysis on the conformations with energy minima confirmed that the ester groups are not always perpendicular to the plane defined by the two adjacent skeletal bonds and may change their relative orientations to meet the requirement of lower energies during the conformational state transition. Instead of the early way of adjusting the interaction energy parameters to fit the experimental data, we attempt to predict unperturbed chain dimensions via the reliable force field and the configurational statistical mechanics. The proposed scheme with three rotational states identified from the contour maps allowed us to satisfactorily reproduce the experimental dimensions of random PMA chains.展开更多
This paper concerns the theme of the universal accessibility to urban spaces, proposing the contribution of configurational approach to their inclusive design. Born in the first Nineties on the roots of the efforts an...This paper concerns the theme of the universal accessibility to urban spaces, proposing the contribution of configurational approach to their inclusive design. Born in the first Nineties on the roots of the efforts and the studies for reducing material and architectural barriers for disabled people, such discipline extends its sphere and purposes so as to mitigate the effects of spatial exclusion of a wider and wider variety of human categories, up to virtually include any potential urban user. Several questions persuade that a merely functional approach, essentially based on the position of the located activities, cannot be said satisfying： only a configurational approach can account for the effects of the grid configuration on the actual accessibility of its spaces. Our research focuses on Italian urban settlements, which appear as ideal case studies, due to the typical consistency of their urban spaces, which, especially in the inner historical cores, are densely build, geometrically irregular and hence generally far from actually providing a universal material accessibility. Here the impedance of space is much more than a theoretical hypothesis and concrete interventions are generally requested to eliminate or reduce its barriers and to make space actually and safely usable. Rather than at indicating the technical solution of single urban problems, which of course are strongly different each other, the research aims at defining a method suitable for any local context. Such method, integrating into a reliable tool the configurational vision with the functional and interactional approach, will provide a hierarchy of urban spaces with reference to the necessity of their universal accessibility.展开更多
Molecular photoswitches hold an important position in chemical research,and it is of significance to develop novel structures and mechanisms.Herein we report a new type of E/Z photoswitches in tellurazole/tellurazoliu...Molecular photoswitches hold an important position in chemical research,and it is of significance to develop novel structures and mechanisms.Herein we report a new type of E/Z photoswitches in tellurazole/tellurazolium-based olefin scaffolds,wherein intramolecular through-space n→π^(*)orbital interaction plays a stabilizing role in the Z isomer approaching quantitative conversion.The manipulation of diverse noncovalent interactions,including intermolecular chalcogen bonding,further provided versatile handles for regulating molecular recognition and multiaddressable switching.Despite bidirectional E/Z photoisomerization with neutral tellurazole derivatives,protonation-induced cationic tellurazoliums allowed significant enhancement in the efficiency of Z→E switching(E up to 73%)while maintaining high percentage E→Z switching(Z up to 95%),as chalcogen bonding with counteranions contributes to the stabilization of electron-accepting tellurazoliums affording a larger wavelength difference between E/Z isomers.Furthermore,the n→π^(*)orbital interaction enables the preference of Z isomer in the ground state for N-methyl tellurazoliums.Bidirectional E/Z photoswitching with high conversion(Z up to 99%,E up to 81%)was attained,and E→Z isomerization can also be invoked by nucleophilic catalysis,making N-methyl tellurazoliums as T-type photoswitches.The results showcase the power of noncovalent interactions for controlling molecular photoswitches and should set the scene for vip recognition,dynamic assemblies,and responsive materials.展开更多
The prediction of configurational disorder properties,such as configurational entropy and orderdisorder phase transition temperature,of compound materials relies on efficient and accurate evaluations of configurationa...The prediction of configurational disorder properties,such as configurational entropy and orderdisorder phase transition temperature,of compound materials relies on efficient and accurate evaluations of configurational energies.Previous cluster expansion methods are not applicable to configurationally-complex material systems,including those with atomic distortions and long-range orders.In this work,we propose to leverage the versatile expressive capabilities of graph neural networks(GNNs)for efficient evaluations of configurational energies and present a workflow combining attention-based GNNs and Monte Carlo simulations to calculate the disorder properties.Using the dataset of face-centered tetragonal gold copper without and with local atomic distortions as an example,we demonstrate that the proposed data-driven framework enables the prediction of phase transition temperatures close to experimental values.We also elucidate that the variance of the energy deviations among configurations controls the prediction accuracy of disorder properties and can be used as the target loss function when training and selecting the GNN models.The work serves as a fundamental step toward a data-driven paradigm for the accelerated design of configurationallycomplex functional material systems.展开更多
The cluster expansion method(CEM)is a widely used lattice-based technique in the study of multicomponent alloys.Despite its prevalent use,a clear understanding of expansion terms is lacking.Wepresent amodern mathemati...The cluster expansion method(CEM)is a widely used lattice-based technique in the study of multicomponent alloys.Despite its prevalent use,a clear understanding of expansion terms is lacking.Wepresent amodern mathematical formalism of the CEM and introduce the cluster decomposition-a unique and basis-independent decomposition for functions of the atomic configuration in a crystal.展开更多
Dense cropping increases crop yield but intensifies resource competition,which reduces single plant yield and limits potential yield growth.Optimizing canopy spacing could enhance resource utilization,support crop mor...Dense cropping increases crop yield but intensifies resource competition,which reduces single plant yield and limits potential yield growth.Optimizing canopy spacing could enhance resource utilization,support crop morphological development and increase yield.Here,a three-year study was performed to verify the feasibility of adjusting row spacing to further enhance yield in densely planted soybeans.Of three row-spacing configurations(40-40,20-40,and 20-60 cm)and two planting densities(normal 180,000 plants ha 1 and high 270,000 plants ha 1).The differences in canopy structure,plant morphological development,photosynthetic capacity and their impact on yield were analyzed.Row spacing configurations have a significant effect on canopy transmittance(CT).The 20-60 cm row spacing configuration increased CT and creates a favorable canopy light environment,in which plant height is reduced,while branching is promoted.This approach reduces plant competition,optimizes the developments of leaf area per plant,specific leaf area,leaf area development rate,leaf area duration and photosynthetic physiological indices(F_(v)/F_(m),ETR,P_(n)).The significant increase of 11.9%-34.2%in canopy apparent photosynthesis(CAP)is attributed to the significant optimization of plant growth and photosynthetic physiology through CT,an important contributing factor to yield increases.The yield in the 20-60 cm treatment is 4.0%higher than in equidistant planting under normal planting density,but 5.9%under high density,primarily driven by CAP and pod number.These findings suggest that suitable row spacing configurations optimize the light environment for plants,promote source-sink transformation in soybeans,and further improve yield.In practice,a 20-60 cm row spacing configuration could be employed for high-density soybean planting to achieve a more substantial yield gain.展开更多
One sort of very important polyelectrolytes, polyacrylamide (PAA) and its copolymers with acrylic acid, on the one hand, have been widely applied as commercial products as flocculants and mobility control fluids in en...One sort of very important polyelectrolytes, polyacrylamide (PAA) and its copolymers with acrylic acid, on the one hand, have been widely applied as commercial products as flocculants and mobility control fluids in enhanced oil recovery. On the other hand, these polymers relate to the fundamental point of polymer physics, a configuration of very long chain molecules containing many hydrogen-bonding groups.展开更多
To obtain the Ti_(p)with different aspect ratios,the Ti_(p)/Mg-5Zn-0.3Ca composite prepared by semi-solid stir casting was subjected to extrusion at 220℃,180℃,and 140℃,respectively.Then,the effect of the Ti_(p)’s ...To obtain the Ti_(p)with different aspect ratios,the Ti_(p)/Mg-5Zn-0.3Ca composite prepared by semi-solid stir casting was subjected to extrusion at 220℃,180℃,and 140℃,respectively.Then,the effect of the Ti_(p)’s aspect ratio on the microstructure,mechanical properties,work hardening and softening behaviors of Ti_(p)/Mg-5Zn-0.3Ca composites was investigated.The results indicated that the Ti_(p)could be elongated obviously after low-temperature extrusion,and the aspect ratio of which would reach to 13.7:1 as the extrusion temperature deceased to 140℃.Then the“Ti/Mg”layer-like structure was formed in the Ti_(p)/Mg-5Zn-0.3Ca composite.Accompanied with the elongation of Ti_(p),the dynamic recrystallized grains and dynamic precipitates were both refined significantly,however,the dynamic recrystallization rate changed a little.The elongated Ti_(p)endowed the Ti_(p)/Mg-5Zn-0.3Ca composites with better matching of strength and toughness without the sacrifice of elongation and bending strain.Both the work hardening rate and softening rate of Ti_(p)/Mg-5Zn-0.3Ca composites increased with the increasing aspect ratio of Ti_(p).The formation of“Ti/Mg”layer-like structure contributed to the redistribution of strain from large aggregations to a network-like distribution,which effectively suppresses the initiation and propagation of micro-cracks,thus enhancing the plasticity of the Ti_(p)/Mg-5Zn-0.3Ca composites.展开更多
Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR pr...Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.展开更多
In the context of the“dual carbon”goals,to address issues such as high energy consumption,high costs,and low power quality in the rapid development of electrified railways,this study focused on the China Railways Hi...In the context of the“dual carbon”goals,to address issues such as high energy consumption,high costs,and low power quality in the rapid development of electrified railways,this study focused on the China Railways High-Speed 5 Electric Multiple Unit and proposed a mathematical model and capacity optimization method for an onboard energy storage system using lithium batteries and supercapacitors as storage media.Firstly,considering the electrical characteristics,weight,and volume of the storage media,a mathematical model of the energy storage system was established.Secondly,to tackle problems related to energy consumption and power quality,an energy management strategy was proposed that comprehensively considers peak shaving and valley filling and power quality by controlling the charge/discharge thresholds of the storage system.Thecapacity optimization adopted a bilevel programming model,with the series/parallel number of storage modules as variables,considering constraints imposed by the Direct Current to Direct Current converter,train load,and space.An improved Particle Swarm Optimization algorithm and linear programming solver were used to solve specific cases.The results show that the proposed onboard energy storage system can effectively achieve energy savings,reduce consumption,and improve power qualitywhile meeting the load and space limitations of the train.展开更多
Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)an...Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.展开更多
Filter capacitors play an important role in altern-ating current(AC)-line filtering for stabilizing voltage,sup-pressing harmonics,and improving power quality.However,traditional aluminum electrolytic capacitors(AECs)...Filter capacitors play an important role in altern-ating current(AC)-line filtering for stabilizing voltage,sup-pressing harmonics,and improving power quality.However,traditional aluminum electrolytic capacitors(AECs)suffer from a large size,short lifespan,low power density,and poor reliability,which limits their use.In contrast,ultrafast supercapacitors(SCs)are ideal for replacing commercial AECs because of their extremely high power densities,fast charging and discharging,and excellent high-frequency re-sponse.We review the design principles and key parameters for ultrafast supercapacitors and summarize research pro-gress in recent years from the aspects of electrode materials,electrolytes,and device configurations.The preparation,structures,and frequency response performance of electrode materials mainly consisting of carbon materials such as graphene and carbon nanotubes,conductive polymers,and transition metal compounds,are focused on.Finally,future research directions for ultrafast SCs are suggested.展开更多
A novel malonamide-linked zinc bisporphyrinate[Zn_(2)-1]has been designed and synthesized.UV-vis and NMR spectroscopic studies suggest the molecule aggregates in solution.Such zinc bisporphyrinate is very CD-sensitive...A novel malonamide-linked zinc bisporphyrinate[Zn_(2)-1]has been designed and synthesized.UV-vis and NMR spectroscopic studies suggest the molecule aggregates in solution.Such zinc bisporphyrinate is very CD-sensitive when it is mixed with amino acid ethyl esters.The amplitude value of the induced circular dichroism(ICD)is up to ca.1500 L•mol^(−1)•cm^(−1).Further studies by ^(1)H NMR and UV-vis spectroscopies reveal amino acid esters function as monodentate ligands,and[Zn_(2)-1]interacts with amino acid ethyl esters through coordination and hydrogen bonding interactions.展开更多
基金supported by the National Natural Science Foundation of China(Nos.41876189 and 81703388)the State Key Laboratory of Bioreactor Engineering and Shanghai Collaborative Innovation Center for Biomanufacturing Technology.
文摘Two novel diketopiperazines(1 and 5),along with ten known compounds(2−4,6−12)demonstrating significant skin inflammation inhibition,were isolated from a marine-derived fungus identified as Aspergillus sp.FAZW0001.The structural elucidation and configurational reassessments of compounds 1−5 were established through comprehensive spectral analyses,with their absolute configurations determined via single crystal X-ray diffraction using Cu Kαradiation,Marfey’s method,and comparison between experimental and calculated electronic circular dichroism(ECD)spectra.Compounds 1,2,and 8 exhibited significant anti-inflammatory activities in Propionibacterium acnes(P.acnes)-induced human monocyte cell lines.Compound 8 demonstrated the ability to down-regulate interleukin-1β(IL-1β)expression by inhibiting Toll-like receptor 2(TLR2)expression and modulating the activation of myeloid differentiation factor 88(MyD88),mitogen-activated protein kinase(MAPK),and nuclear factorκB(NF-κB)signaling pathways,thus reducing the cellular inflammatory response induced by P.acnes.Additionally,compound 8 showed the capacity to suppress mitochondrial reactive oxygen species(ROS)production and nucleotide-binding oligomerization domain-like receptor protein 3(NLRP3)inflammasome activation,thereby reducing IL-1βmaturation and secretion.A three-dimensional quantitative structure-activity relationships(3D-QSAR)model was applied to compounds 5−12 to analyze their anti-inflammatory structure-activity relationships.
基金the financial support provided by the National Natural Science Foundation of China[Grant No.72373138 and 71973131]Major Project of National Social Science Foundation of China[Grant No.19VHQ002].
文摘The promotion of energy efficiency(EE)helps address energy constraints and promote environmental sustainability.This study comprehensively explores the spatiotemporal variations,influencing factors,and configuration promotion paths of EE in 284 Chinese cities during 2003‒2019 using the global super-efficiency minimum distance to strong efficient frontier(G-S-MinDS),exploratory spatial data analysis(ESDA),multiscale geographically weighted regression(MGWR),and fuzzy set qualitative comparative analysis(fsQCA)methods.The findings are:①China’s cities have an annual average EE of 0.658 with a growth rate of 0.53%,showing considerable promotion potential.②Industrial structure optimization,population agglomeration,economic development,and increased green coverage contribute positively,while government intervention and openness hinder China’s urban EE.③Four configurational promotion paths for enhancing China’s urban EE are identified,where among those paths population density is a core condition,while government intervention is not.This study provides valuable insights into substantially improving urban EE,emphasizing the need for targeted policies to address energy and environmental crises in China.
基金supported by the National Natural Science Foundation of China(Nos.11975091 and U1732135)the Program for Innovative Research Team(in Science and Technology)in University of Henan Province,China(No.21IRTSTHN011)。
文摘Configurational information entropy(CIE)theory was employed to determine the neutron-skin thickness of neutron-rich calcium isotopes.The nuclear density distributions and fragment cross sections in 350 MeV/u ^(40-60)Ca+^(9)Be projectile fragmentation reactions were calculated using a modified statistical abrasion-ablation model.CIE quantities were determined from the nuclear density,isotopic,mass,and charge distributions.The linear correlations between the CIE determined using the isotopic,mass,and charge distributions and the neutron-skin thickness of the projectile nucleus show that CIE provides new methods to extract the neutron-skin thickness of neutron-rich nuclei.
基金financially supported by the National Natural Science Foundation of China(Nos.51772035 and 11874356)the Fundamental Research Funds for the Central Universities(No.2020CDJ-LHZZ-011)Chongqing Entrepreneurship and Innovation Program for the Returned Overseas Chinese Scholars(No.cx2019002)
文摘ABX_(2)(A=Ag,Na,Cu;B=Sb,Bi;X=S,Se,Te)(GroupsⅠ-Ⅴ-Ⅵ_(2))compounds,which are all characterized by the ultralow lattice thermal conductivity because of their strong lattice anharmonicity caused by lone-pair electrons,have aroused wide attention in thermoelectric community.The practical application of thermoelectric devices usually requires both the compatible n-type and p-type materials simultaneously.However,most ofⅠ-Ⅴ-Ⅵ_(2)compounds are intrinsic p-type semiconductors,lacking their n-type counterparts for thermoelectrics.Herein,in this work,we increase the configuration entropy of AgBiTe_(2)by alloying SnTe,in order to stabilize the cubic phase at room temperature.With further optimization of thermal and electrical performance,the thermoelectric performance could be improved simultaneously in both n-and p-type(AgBiTe_(2))_(1-x)(SnTe)_(x)(x=0.3,0.4)solid solutions.Finally,p-type compound with the nominal composition of(AgBi_(0.99)Cd_(0.01)Te_(2))_(0.6)(SnTe)_(0.4)and n-type of(AgBiTe_(2))_(0.7)(SnTe)_(0.3)~Br 6%show the maximum zT of~0.33 and~0.21,at 381 and 423 K,respectively.
基金the National Natural Science Foundation of China(No.11975091)the Program for Innovative Research Team(in Science and Technology)in the University of Henan Province,China(No.21IRTSTHN011).
文摘Configurational information entropy(CIE)analysis has been shown to be applicable for determining the neutron skin thickness(δnp)of neutron-rich nuclei from fragment production in projectile fragmentation reactions.The BNN+FRACS machine learning model was adopted to predict the fragment mass cross-sections(σ_(A))of the projectile fragmentation reactions induced by calcium isotopes from ^(36)Ca to ^(56)Ca on a ^(9)Be target at 140MeV/u.The fast Fourier transform was adopted to decompose the possible information compositions inσA distributions and determine the quantity of CIE(S_(A)[f]).It was found that the range of fragments significantly influences the quantity of S_(A)[f],which results in different trends of S_(A)[f]~δnp correlation.The linear S_(A)[f]~δnp correlation in a previous study[Nucl.Sci.Tech.33,6(2022)]could be reproduced using fragments with relatively large mass fragments,which verifies that S_(A)[f]determined from fragmentσAis sensitive to the neutron skin thickness of neutron-rich isotopes.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174162,51962010,12064015,and 12064014).
文摘The spinel-type LiMn_(2)O_(4) is a promising candidate as cathode material for rechargeable Li-ion batteries due to its good thermal stability and safety.Experimentally,it is observed that in this compound there occur the structural phase transitions from cubic(Fd3m)to tetragonal(I4_(1)/amd)phase at slightly below room temperature.To understand the phase transition mechanism,we compare the Gibbs free energy between cubic phase and tetragonal phase by including the configurational entropy.Our results show that the configurational entropy contributes substantially to the stability of the cubic phase at room temperature due to the disordered Mn^(3+)/Mn^(4+)distribution as well as the orientation of the Jahn-Teller elongation of the Mn^(3+)O_(6) octahedron in the the spinel phase.Meanwhile,the phase transition temperature is predicted to be 267.8 K,which is comparable to the experimentally observed temperature.These results serve as a good complement to the experimental study,and are beneficial to the improving of the electrochemical performance of LiMn_(2)O_(4) cathode.
基金financially supported by the National Natural Science Foundation of China(Nos.51690163 and 51601147)the Science Challenge Project(No.TZZT2019-D1.5)+4 种基金the Ministry of Science and Technology of China(No.2017YFA0700700)the United States National Science Foundation(Nos.DMR-1006557,1611180,and 1809640)the Fundamental Research Funds for the Central Universities in China(No.G2016KY0302)the CyberStar cluster funded by NSF through grant No.OCI-0821527the XSEDE clusters supported by NSF through Grant No.ACI-1053575。
文摘Metallic amorphous/crystalline(A/C)nanolaminates exhibit excellent ductility while retaining their high strength.However,the underlying physical mechanisms and the resultant structural changes during plastic deformation still remain unclear.In the present work,the structure-property relationship of CuZr/Cu A/C nanolaminates is established through integrated high-throughput micro-compression tests and molecular dynamics simulations together with high-resolution transmission electron microcopy.The serrated flow of nanolaminates results from the formation of hexagonal-close-packed(HCP)-type stacking faults and twins inside the face-centered-cubic(FCC)Cu nano-grains,the body-centered-cubic(BCC)-type ordering at their grain boundaries,and the crystallization of the amorphous CuZr layers.The serration behavior of CuZr/Cu A/C nanolaminates is determined by several factors,including the formation of dense dislocation networks from the multiplication of initial dislocations that formed after yielding,weak-spots-related configurational-transitions and shear-transition-zone activities,and deformation-induced devitrification.The present work provides an insight into the heterogeneous deformation mechanism of A/C nanolaminates at the atomic scale,and mechanistic base for the microstructural design of self-toughening metallic-glass(MG)-based composites and A/C nanolaminates.
基金This work has been supported by the National Science Foundation of China,the Youth Science Foundation of Academia Sinica,the China Postdoctoral Science Foundation and Polymer Physics Laboratory, Academia Sinica.
文摘A full-relaxation optimization of molecule and the popular MM2 force field are employed to obtain the geometry parameters and the conformational energy surface of a meso or a racemic dyad of poly(methyl acrylate) (PMA) with a specified carbonyl-bond orientation in side-groups. It is found that the conformational energy maps calculated here considerably differ from those calculated with the rigid molecular model as reported in the earlier studies. The g(-) state cannot be omitted in the obtained contour maps. Two important conformers tg(-) and g(-t) with energy minima were newly detected for a racemic dyad. The analysis on the conformations with energy minima confirmed that the ester groups are not always perpendicular to the plane defined by the two adjacent skeletal bonds and may change their relative orientations to meet the requirement of lower energies during the conformational state transition. Instead of the early way of adjusting the interaction energy parameters to fit the experimental data, we attempt to predict unperturbed chain dimensions via the reliable force field and the configurational statistical mechanics. The proposed scheme with three rotational states identified from the contour maps allowed us to satisfactorily reproduce the experimental dimensions of random PMA chains.
文摘This paper concerns the theme of the universal accessibility to urban spaces, proposing the contribution of configurational approach to their inclusive design. Born in the first Nineties on the roots of the efforts and the studies for reducing material and architectural barriers for disabled people, such discipline extends its sphere and purposes so as to mitigate the effects of spatial exclusion of a wider and wider variety of human categories, up to virtually include any potential urban user. Several questions persuade that a merely functional approach, essentially based on the position of the located activities, cannot be said satisfying： only a configurational approach can account for the effects of the grid configuration on the actual accessibility of its spaces. Our research focuses on Italian urban settlements, which appear as ideal case studies, due to the typical consistency of their urban spaces, which, especially in the inner historical cores, are densely build, geometrically irregular and hence generally far from actually providing a universal material accessibility. Here the impedance of space is much more than a theoretical hypothesis and concrete interventions are generally requested to eliminate or reduce its barriers and to make space actually and safely usable. Rather than at indicating the technical solution of single urban problems, which of course are strongly different each other, the research aims at defining a method suitable for any local context. Such method, integrating into a reliable tool the configurational vision with the functional and interactional approach, will provide a hierarchy of urban spaces with reference to the necessity of their universal accessibility.
基金financially supported by the National Natural Science Foundation of China(grant nos.92156010,22071247,22101283,and 22101284)the Strategic Priority Research Program(grant no.XDB20000000)+1 种基金the Key Research Program of Frontier Sciences(grant no.QYZDB-SSW-SLH030)of Chinese Academy of Sciences,Natural Science Foundation of Fujian Province(grant nos.2020J06035 and 2022J05085)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(grant no.2021ZR112)for support.
文摘Molecular photoswitches hold an important position in chemical research,and it is of significance to develop novel structures and mechanisms.Herein we report a new type of E/Z photoswitches in tellurazole/tellurazolium-based olefin scaffolds,wherein intramolecular through-space n→π^(*)orbital interaction plays a stabilizing role in the Z isomer approaching quantitative conversion.The manipulation of diverse noncovalent interactions,including intermolecular chalcogen bonding,further provided versatile handles for regulating molecular recognition and multiaddressable switching.Despite bidirectional E/Z photoisomerization with neutral tellurazole derivatives,protonation-induced cationic tellurazoliums allowed significant enhancement in the efficiency of Z→E switching(E up to 73%)while maintaining high percentage E→Z switching(Z up to 95%),as chalcogen bonding with counteranions contributes to the stabilization of electron-accepting tellurazoliums affording a larger wavelength difference between E/Z isomers.Furthermore,the n→π^(*)orbital interaction enables the preference of Z isomer in the ground state for N-methyl tellurazoliums.Bidirectional E/Z photoswitching with high conversion(Z up to 99%,E up to 81%)was attained,and E→Z isomerization can also be invoked by nucleophilic catalysis,making N-methyl tellurazoliums as T-type photoswitches.The results showcase the power of noncovalent interactions for controlling molecular photoswitches and should set the scene for vip recognition,dynamic assemblies,and responsive materials.
基金funding support from the U.S.Department of Energy,Office of Science,Basic Energy Sciences,under Award No.DE-SC0023664。
文摘The prediction of configurational disorder properties,such as configurational entropy and orderdisorder phase transition temperature,of compound materials relies on efficient and accurate evaluations of configurational energies.Previous cluster expansion methods are not applicable to configurationally-complex material systems,including those with atomic distortions and long-range orders.In this work,we propose to leverage the versatile expressive capabilities of graph neural networks(GNNs)for efficient evaluations of configurational energies and present a workflow combining attention-based GNNs and Monte Carlo simulations to calculate the disorder properties.Using the dataset of face-centered tetragonal gold copper without and with local atomic distortions as an example,we demonstrate that the proposed data-driven framework enables the prediction of phase transition temperatures close to experimental values.We also elucidate that the variance of the energy deviations among configurations controls the prediction accuracy of disorder properties and can be used as the target loss function when training and selecting the GNN models.The work serves as a fundamental step toward a data-driven paradigm for the accelerated design of configurationallycomplex functional material systems.
基金funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Materials Sciences and Engineering Division under Contract No.DE-AC02-05-CH11231(Materials Project program KC23MP)。
文摘The cluster expansion method(CEM)is a widely used lattice-based technique in the study of multicomponent alloys.Despite its prevalent use,a clear understanding of expansion terms is lacking.Wepresent amodern mathematical formalism of the CEM and introduce the cluster decomposition-a unique and basis-independent decomposition for functions of the atomic configuration in a crystal.
基金supported by the Biological Breeding-National Science and Technology Major Project(2023ZD0403305)National Natural Science Foundation of China(32101845)+1 种基金the National Key Research and Development Program of China(2023YFE0105000)the China Agriculture Research System(CARS-04).
文摘Dense cropping increases crop yield but intensifies resource competition,which reduces single plant yield and limits potential yield growth.Optimizing canopy spacing could enhance resource utilization,support crop morphological development and increase yield.Here,a three-year study was performed to verify the feasibility of adjusting row spacing to further enhance yield in densely planted soybeans.Of three row-spacing configurations(40-40,20-40,and 20-60 cm)and two planting densities(normal 180,000 plants ha 1 and high 270,000 plants ha 1).The differences in canopy structure,plant morphological development,photosynthetic capacity and their impact on yield were analyzed.Row spacing configurations have a significant effect on canopy transmittance(CT).The 20-60 cm row spacing configuration increased CT and creates a favorable canopy light environment,in which plant height is reduced,while branching is promoted.This approach reduces plant competition,optimizes the developments of leaf area per plant,specific leaf area,leaf area development rate,leaf area duration and photosynthetic physiological indices(F_(v)/F_(m),ETR,P_(n)).The significant increase of 11.9%-34.2%in canopy apparent photosynthesis(CAP)is attributed to the significant optimization of plant growth and photosynthetic physiology through CT,an important contributing factor to yield increases.The yield in the 20-60 cm treatment is 4.0%higher than in equidistant planting under normal planting density,but 5.9%under high density,primarily driven by CAP and pod number.These findings suggest that suitable row spacing configurations optimize the light environment for plants,promote source-sink transformation in soybeans,and further improve yield.In practice,a 20-60 cm row spacing configuration could be employed for high-density soybean planting to achieve a more substantial yield gain.
基金National Natural Science Foundation of ChinaChina Postdoctoral Science Foundation+1 种基金Youth Science Foundation of Academia SinicaPolymer Physics Laboratory, Academia Sinica.
文摘One sort of very important polyelectrolytes, polyacrylamide (PAA) and its copolymers with acrylic acid, on the one hand, have been widely applied as commercial products as flocculants and mobility control fluids in enhanced oil recovery. On the other hand, these polymers relate to the fundamental point of polymer physics, a configuration of very long chain molecules containing many hydrogen-bonding groups.
基金supported by the“National Natural Science Foundation of China”(Grants.52271109 and 52001223)Support from the“National Key Research and Development Program for Young Scientists”(Grant.2021YFB3703300)+1 种基金the Major Special Plan for Science and Technology in Shanxi Province(202201050201012)the Special Fund Project for Guiding Local Science and Technology Development by the Central Government(Grant.YDZJSX2021B019)。
文摘To obtain the Ti_(p)with different aspect ratios,the Ti_(p)/Mg-5Zn-0.3Ca composite prepared by semi-solid stir casting was subjected to extrusion at 220℃,180℃,and 140℃,respectively.Then,the effect of the Ti_(p)’s aspect ratio on the microstructure,mechanical properties,work hardening and softening behaviors of Ti_(p)/Mg-5Zn-0.3Ca composites was investigated.The results indicated that the Ti_(p)could be elongated obviously after low-temperature extrusion,and the aspect ratio of which would reach to 13.7:1 as the extrusion temperature deceased to 140℃.Then the“Ti/Mg”layer-like structure was formed in the Ti_(p)/Mg-5Zn-0.3Ca composite.Accompanied with the elongation of Ti_(p),the dynamic recrystallized grains and dynamic precipitates were both refined significantly,however,the dynamic recrystallization rate changed a little.The elongated Ti_(p)endowed the Ti_(p)/Mg-5Zn-0.3Ca composites with better matching of strength and toughness without the sacrifice of elongation and bending strain.Both the work hardening rate and softening rate of Ti_(p)/Mg-5Zn-0.3Ca composites increased with the increasing aspect ratio of Ti_(p).The formation of“Ti/Mg”layer-like structure contributed to the redistribution of strain from large aggregations to a network-like distribution,which effectively suppresses the initiation and propagation of micro-cracks,thus enhancing the plasticity of the Ti_(p)/Mg-5Zn-0.3Ca composites.
基金financial supports from the National Natural Science Foundation of China(52201237)the Talent Introduction Project of Chinese Academy of Sciences(E344011)+4 种基金the Shenzhen High Level Talent Team Project(KQTD2022110109364705)the Joint Research Project of China Merchants Group and SIAT(E2Z1521)the Cross Institute Joint Research Youth Team Project of SIAT(E25427)National Natural Science Foundation of China(52402136)the China Postdoctoral Science Foundation(E325281005)。
文摘Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.
基金funded by the National Natural Science Foundation of China(52167013)the Key Program of Natural Science Foundation of Gansu Province(24JRRA225)Natural Science Foundation of Gansu Province(23JRRA891).
文摘In the context of the“dual carbon”goals,to address issues such as high energy consumption,high costs,and low power quality in the rapid development of electrified railways,this study focused on the China Railways High-Speed 5 Electric Multiple Unit and proposed a mathematical model and capacity optimization method for an onboard energy storage system using lithium batteries and supercapacitors as storage media.Firstly,considering the electrical characteristics,weight,and volume of the storage media,a mathematical model of the energy storage system was established.Secondly,to tackle problems related to energy consumption and power quality,an energy management strategy was proposed that comprehensively considers peak shaving and valley filling and power quality by controlling the charge/discharge thresholds of the storage system.Thecapacity optimization adopted a bilevel programming model,with the series/parallel number of storage modules as variables,considering constraints imposed by the Direct Current to Direct Current converter,train load,and space.An improved Particle Swarm Optimization algorithm and linear programming solver were used to solve specific cases.The results show that the proposed onboard energy storage system can effectively achieve energy savings,reduce consumption,and improve power qualitywhile meeting the load and space limitations of the train.
文摘Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.
文摘Filter capacitors play an important role in altern-ating current(AC)-line filtering for stabilizing voltage,sup-pressing harmonics,and improving power quality.However,traditional aluminum electrolytic capacitors(AECs)suffer from a large size,short lifespan,low power density,and poor reliability,which limits their use.In contrast,ultrafast supercapacitors(SCs)are ideal for replacing commercial AECs because of their extremely high power densities,fast charging and discharging,and excellent high-frequency re-sponse.We review the design principles and key parameters for ultrafast supercapacitors and summarize research pro-gress in recent years from the aspects of electrode materials,electrolytes,and device configurations.The preparation,structures,and frequency response performance of electrode materials mainly consisting of carbon materials such as graphene and carbon nanotubes,conductive polymers,and transition metal compounds,are focused on.Finally,future research directions for ultrafast SCs are suggested.
基金This work was supported by the Natural Science Foundation of China(No.21271133)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘A novel malonamide-linked zinc bisporphyrinate[Zn_(2)-1]has been designed and synthesized.UV-vis and NMR spectroscopic studies suggest the molecule aggregates in solution.Such zinc bisporphyrinate is very CD-sensitive when it is mixed with amino acid ethyl esters.The amplitude value of the induced circular dichroism(ICD)is up to ca.1500 L•mol^(−1)•cm^(−1).Further studies by ^(1)H NMR and UV-vis spectroscopies reveal amino acid esters function as monodentate ligands,and[Zn_(2)-1]interacts with amino acid ethyl esters through coordination and hydrogen bonding interactions.
