Multi-component occupancies of perovskite materials(ABO_(3))have brought diverse crystallographic distortions and highly tunable defect structures.These structural features enable ABO_(3)to have customizable dielectri...Multi-component occupancies of perovskite materials(ABO_(3))have brought diverse crystallographic distortions and highly tunable defect structures.These structural features enable ABO_(3)to have customizable dielectric and magnetic properties,offering new opportunities for advancing microwave absorbing materials.In this study,entropy-driven strategies,including composition optimization,structural/defective design,microstructure engineering,and microwave absorption simulation,are proposed to improve the microwave absorption capacity of(Ba_(1/3)Sr_(1/3)Ca_(1/3))FeO_(3).The hexagonal perovskite structure(Ba_(1/3)Sr_(1/3)Ca_(1/3))FeO_(3)prepared at 1100℃exhibits exceptional electromagnetic wave absorption properties,with a minimum reflection loss of−40.58 dB at a thickness of 1.2 mm and a maximum effective absorption bandwidth of 4.16 GHz.The results indicate that the interconnection of octahedra,and structural distortions,oxygen vacancies,and other defects enhance the dielectric polarization of the material,leading to excellent wave absorption performance.The entropy-driven design strategy for perovskite ABO_(3)materials offers valuable insights for the development of advanced electromagnetic wave absorption materials.展开更多
The dielectric ceramic capacitor serves as the core energy storage element in the pulsed power system.However,the inability to balance high energy storage density(W_(rec))and energy storage efficiency(η)has become a ...The dielectric ceramic capacitor serves as the core energy storage element in the pulsed power system.However,the inability to balance high energy storage density(W_(rec))and energy storage efficiency(η)has become a technical challenge limiting the miniaturisation of pulsed power devices.This work proposes an entropy-driven strategy,through introducing Sr(Sc0.5Nb0.5)O_(3)(SSN)as an end-member,to modulate the phase structure and suppress interfacial polarization in the medium entropy matrix,(Bi_(0.5)Na_(0.5))_(0.5)Ba_(0.5)TiO_(3)(BN50BT).The introduction of SSN endows BN50BT ceramics with a multiphase structure of P4mm and Pm m and successfully establishes a super-paraelectric(SPE)state at room temperature,improving the polarization response.Furthermore,the incorporation of SSN effectively suppresses interfacial polarization and enhances the Eb of the system.Thus,the 0.80[(Bi_(0.5)Na_(0.5))_(0.5)Ba_(0.5)TiO_(3)]-0.20Sr(Sc_(0.5)Nb_(0.5))O_(3) ceramics exhibit a decent W_(rec) of 6.24 J/cm^(3) and a highηof 89.02%,along with remarkable stabilities over a wide frequency range(5-150 Hz)and temperature range(25-140℃).This work demonstrates that the entropy-driven construction of a multiphase-coexisting SPE state,along with suppressed interfacial polarization,represents a feasible approach to optimizing the energy storage properties of dielectric ceramics.展开更多
Early detection of cancer biomarkers applied in real-time disease diagnosis and therapies can increase the survival rate of patients.Circulating tumor DNA(ct DNA)as a typical cancer biomarker plays a great role in the...Early detection of cancer biomarkers applied in real-time disease diagnosis and therapies can increase the survival rate of patients.Circulating tumor DNA(ct DNA)as a typical cancer biomarker plays a great role in the process of tumor disease monitoring,especially in early diagnosis.Unfortunately,most ct DNA detection systems have not been widely used due to their low sensitivity,poor specificity,and high cost.Herein,we developed an alternative ct DNA detection system to present the levels of ct DNA by recording the fluorescence signals of the system containing upconversion nanoparticles(UCNPs),Fe_(3)O_(4),and entropy-driven strand displacement reaction.The method has a practical sensitivity with a wide linear range from 100 amol L^(-1)to 1 nmol L^(-1)and a low detection limit of 1.6 amol L^(-1).Furthermore,the system demonstrates a practical application in mouse blood serum samples and meets the requirements for rapid,sensitive,specific,and economical diagnosis of cancers.Thus,this ct DNA detection system may have great potential for ct DNAdetection and clinical diagnosis.展开更多
Understanding the effect of curvature and topological frustration on self-assembly yields insight into the mechanistic details of the ordering of identical subunits in curved spaces,such as the assembly of viral capsi...Understanding the effect of curvature and topological frustration on self-assembly yields insight into the mechanistic details of the ordering of identical subunits in curved spaces,such as the assembly of viral capsids,growth of solid domains on vesicles,and the self-assembly of molecular monolayers.However,the self-assembly of nanoparticles with anisotropic surface topology and compartmentalization on curved surfaces remains elusive.By combining large-scale molecular simulations as well as theoretical analysis,we demonstrate here that the interplay among anisotropy,curvature,and chain conformation induces tethered Janus nanoparticles to self-assemble into diverse novel structures on a sphere,including binary nanocluster(C_(B)),trinary nanocluster(C_(T)),nanoribbon(R_(N))and hexagon with centered reverse(HR),which are mapped on a phase diagram related to the length asymmetry of tethered chains and Janus balance of the nanoparticles.The dynamical mechanism for the formation of these structure states is analyzed by examining the detailed kinetic pathways as well as free energy.We also show that the centered-reverse state is more prone to emerging around the topological defects,indicating the defect-enhanced entropy effect on a curved surface.Finally,the analytical model that rationalizes the regimes of these structure states is developed and fits simulations reasonably well,resulting in a mechanistic interpretation based on the order through entropy.Our findings shed light on curvature engineering as a versatile strategy to tailor the superstructures formed by anisotropic building blocks toward unique properties.展开更多
基金supported by the Natural Science Foundation Outstanding Youth Fund Project of Henan Province(No.242300421009)the Henan Provincial Science and Technology Research Project(Nos.241111232800 and 232102230115)+1 种基金the Joint Fund of Research and Development Program of Henan Province(No.222301420002)the National Natural Science Foundation of China(No.U21A2064).
文摘Multi-component occupancies of perovskite materials(ABO_(3))have brought diverse crystallographic distortions and highly tunable defect structures.These structural features enable ABO_(3)to have customizable dielectric and magnetic properties,offering new opportunities for advancing microwave absorbing materials.In this study,entropy-driven strategies,including composition optimization,structural/defective design,microstructure engineering,and microwave absorption simulation,are proposed to improve the microwave absorption capacity of(Ba_(1/3)Sr_(1/3)Ca_(1/3))FeO_(3).The hexagonal perovskite structure(Ba_(1/3)Sr_(1/3)Ca_(1/3))FeO_(3)prepared at 1100℃exhibits exceptional electromagnetic wave absorption properties,with a minimum reflection loss of−40.58 dB at a thickness of 1.2 mm and a maximum effective absorption bandwidth of 4.16 GHz.The results indicate that the interconnection of octahedra,and structural distortions,oxygen vacancies,and other defects enhance the dielectric polarization of the material,leading to excellent wave absorption performance.The entropy-driven design strategy for perovskite ABO_(3)materials offers valuable insights for the development of advanced electromagnetic wave absorption materials.
基金supported by Guangxi Science and Technology Plan Project(GuikeAD25069100)Guangxi Natural Science Foundation Project(2025GXNSFBA069167).
文摘The dielectric ceramic capacitor serves as the core energy storage element in the pulsed power system.However,the inability to balance high energy storage density(W_(rec))and energy storage efficiency(η)has become a technical challenge limiting the miniaturisation of pulsed power devices.This work proposes an entropy-driven strategy,through introducing Sr(Sc0.5Nb0.5)O_(3)(SSN)as an end-member,to modulate the phase structure and suppress interfacial polarization in the medium entropy matrix,(Bi_(0.5)Na_(0.5))_(0.5)Ba_(0.5)TiO_(3)(BN50BT).The introduction of SSN endows BN50BT ceramics with a multiphase structure of P4mm and Pm m and successfully establishes a super-paraelectric(SPE)state at room temperature,improving the polarization response.Furthermore,the incorporation of SSN effectively suppresses interfacial polarization and enhances the Eb of the system.Thus,the 0.80[(Bi_(0.5)Na_(0.5))_(0.5)Ba_(0.5)TiO_(3)]-0.20Sr(Sc_(0.5)Nb_(0.5))O_(3) ceramics exhibit a decent W_(rec) of 6.24 J/cm^(3) and a highηof 89.02%,along with remarkable stabilities over a wide frequency range(5-150 Hz)and temperature range(25-140℃).This work demonstrates that the entropy-driven construction of a multiphase-coexisting SPE state,along with suppressed interfacial polarization,represents a feasible approach to optimizing the energy storage properties of dielectric ceramics.
基金supported by the Science and Technology Cooperation Project between Chinese and Australian Governments (2017YFE0132300)the National Natural Science Foundation of China (NSFC 51929201, 51672268, 51720105015, 51972138, 51872263, and 51828202)+1 种基金the Science and Technology Development Planning Project of Jilin Province (20190201232JC)the CASCroucher Funding Scheme for Joint Laboratories (CAS18204)
文摘Early detection of cancer biomarkers applied in real-time disease diagnosis and therapies can increase the survival rate of patients.Circulating tumor DNA(ct DNA)as a typical cancer biomarker plays a great role in the process of tumor disease monitoring,especially in early diagnosis.Unfortunately,most ct DNA detection systems have not been widely used due to their low sensitivity,poor specificity,and high cost.Herein,we developed an alternative ct DNA detection system to present the levels of ct DNA by recording the fluorescence signals of the system containing upconversion nanoparticles(UCNPs),Fe_(3)O_(4),and entropy-driven strand displacement reaction.The method has a practical sensitivity with a wide linear range from 100 amol L^(-1)to 1 nmol L^(-1)and a low detection limit of 1.6 amol L^(-1).Furthermore,the system demonstrates a practical application in mouse blood serum samples and meets the requirements for rapid,sensitive,specific,and economical diagnosis of cancers.Thus,this ct DNA detection system may have great potential for ct DNAdetection and clinical diagnosis.
基金supported by the National Natural Science Foundation of China(Grants No.22025302 and 21873053)L.T.Y.acknowledges financial support from the Ministry of Science and Technology of China(Grant No.2016YFA0202500).
文摘Understanding the effect of curvature and topological frustration on self-assembly yields insight into the mechanistic details of the ordering of identical subunits in curved spaces,such as the assembly of viral capsids,growth of solid domains on vesicles,and the self-assembly of molecular monolayers.However,the self-assembly of nanoparticles with anisotropic surface topology and compartmentalization on curved surfaces remains elusive.By combining large-scale molecular simulations as well as theoretical analysis,we demonstrate here that the interplay among anisotropy,curvature,and chain conformation induces tethered Janus nanoparticles to self-assemble into diverse novel structures on a sphere,including binary nanocluster(C_(B)),trinary nanocluster(C_(T)),nanoribbon(R_(N))and hexagon with centered reverse(HR),which are mapped on a phase diagram related to the length asymmetry of tethered chains and Janus balance of the nanoparticles.The dynamical mechanism for the formation of these structure states is analyzed by examining the detailed kinetic pathways as well as free energy.We also show that the centered-reverse state is more prone to emerging around the topological defects,indicating the defect-enhanced entropy effect on a curved surface.Finally,the analytical model that rationalizes the regimes of these structure states is developed and fits simulations reasonably well,resulting in a mechanistic interpretation based on the order through entropy.Our findings shed light on curvature engineering as a versatile strategy to tailor the superstructures formed by anisotropic building blocks toward unique properties.
