With the rapid development of portable electronics and electric road vehicles,high-energy-density batteries have been becoming front-burner issues.Traditionally,homogeneous electrolyte cannot simultaneously meet diame...With the rapid development of portable electronics and electric road vehicles,high-energy-density batteries have been becoming front-burner issues.Traditionally,homogeneous electrolyte cannot simultaneously meet diametrically opposed demands of high-potential cathode and low-potential anode,which are essential for high-voltage batteries.Meanwhile,homogeneous electrolyte is difficult to achieve bi-or multi-functions to meet different requirements of electrodes.In comparison,the asymmetric electrolyte with bi-or multi-layer disparate components can satisfy distinct requirements by playing different roles of each electrolyte layer and meanwhile compensates weakness of individual electrolyte.Consequently,the asymmetric electrolyte can not only suppress by-product sedimentation and continuous electrolyte decomposition at the anode while preserving active substances at the cathode for high-voltage batteries with long cyclic lifespan.In this review,we comprehensively divide asymmetric electrolytes into three categories:decoupled liquid-state electrolytes,bi-phase solid/liquid electrolytes and decoupled asymmetric solid-state electrolytes.The design principles,reaction mechanism and mutual compatibility are also studied,respectively.Finally,we provide a comprehensive vision for the simplification of structure to reduce costs and increase device energy density,and the optimization of solvation structure at anolyte/catholyte interface to realize fast ion transport kinetics.展开更多
Mercury ion(Hg^(2+)),a highly noxious of heavy metalion,has detrimental effects on the ecological environment and human health.Herein,we have developed an exonuclease III(Exo III)assisted catalytic hairpin assembly fo...Mercury ion(Hg^(2+)),a highly noxious of heavy metalion,has detrimental effects on the ecological environment and human health.Herein,we have developed an exonuclease III(Exo III)assisted catalytic hairpin assembly formation of a trivalent G-quadruplex/hemin DNAzyme for colorimetric detection of Hg^(2+).A hairpin DNA(Hr)was designed with thymine-Hg^(2+)-thymine pairs that catalyzed by Exo III is prompted to happen upon binding Hg^(2+).A released DNA fragment triggers the catalytic assembly of other three hairpins(H1,H2,and H3)to form many trivalent G-quadruplex/hemin DNA enzymes for signal output.The developed sensor shows a dynamic range from 2 pM to 2μM,with an impressively low detection limit of 0.32 pM for Hg^(2+)detection.Such a sensor also has good selectivity toward Hg^(2+)detection in the presence of other common metal ions.This strategy shows the great potential for visual detection with portable type.展开更多
Objective:This study aimed to describe,optimize and evaluate a method for preparing multivalent conjugate vaccines by simultaneous conjugation of two different bacterial capsular polysaccharides(CPs)with tetanus toxoi...Objective:This study aimed to describe,optimize and evaluate a method for preparing multivalent conjugate vaccines by simultaneous conjugation of two different bacterial capsular polysaccharides(CPs)with tetanus toxoid(TT)as bivalent conjugates.Methods:Different molecular weights(MWs)of polysaccharides,activating agents and capsular polysaccharide/protein(CP/Pro)ratio that may influence conjugation and immunogenicity were investigated and optimized to prepare the bivalent conjugate bulk.Using the described method and optimized parameters,a 20-valent pneumococcal conjugate vaccine and a bivalent meningococcal vaccine were developed and their effectiveness was compared to that of corresponding licensed vaccines in rabbit or mouse models.Results:The immunogenicity test revealed that polysaccharides with lower MWs were better for Pn1-TT-Pn3 and MenA-TT-MenC,while higher MWs were superior for Pn4-TT-Pn14,Pn6A-TT-Pn6B,Pn7F-TT-Pn23F and Pn8-TT-Pn11A.For activating polysaccharides,1-cyano-4-dimethylaminopyridinium tetrafluoroborate(CDAP)was superior to cyanogen bromide(CNBr),but for Pn1,Pn3 and MenC,N-(3-dimethylaminopropyl)-N’-ethylcarbodiimide hydrochloride(EDAC)was the most suitable option.For Pn6A-TT-Pn6B and Pn8-TT-Pn11A,rabbits immunized with bivalent conjugates with lower CP/Pro ratios showed significantly stronger CP-specific antibody responses,while for Pn4-TT-Pn14,higher CP/Pro ratio was better.Instead of interfering with the respective immunological activity,our bivalent conjugates usually induced higher IgG titers than their monovalent counterparts.Conclusion:The result indicated that the described conjugation technique was feasible and efficacious to prepare glycoconjugate vaccines,laying a solid foundation for developing extended-valent multivalent or combined conjugate vaccines without potentially decreased immune function.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
Making use of multivalent functions with negative coefficients of the type f (z)=z^(p)-~(∑)_(k=p+1)^(∞)a_(k)z^(k),which are analytic in the open unit disk and applying the q-derivative a q–differintegral operator i...Making use of multivalent functions with negative coefficients of the type f (z)=z^(p)-~(∑)_(k=p+1)^(∞)a_(k)z^(k),which are analytic in the open unit disk and applying the q-derivative a q–differintegral operator is considered.Furthermore by using the familiar Riesz-Dunford integral,a linear operator on Hilbert space H is introduced.A new subclass of p-valent functions related to an operator on H is defined.Coefficient estimate,distortion bound and extreme points are obtained.The convolution-preserving property is also investigated.展开更多
Multivalent metal-sulfur(M-S,where M=Mg,Al,Ca,Zn,Fe,etc.)batteries offer unique opportunities to achieve high specific capacity,elemental abundancy and cost-effectiveness beyond lithium-ion batteries(LIBs).However,the...Multivalent metal-sulfur(M-S,where M=Mg,Al,Ca,Zn,Fe,etc.)batteries offer unique opportunities to achieve high specific capacity,elemental abundancy and cost-effectiveness beyond lithium-ion batteries(LIBs).However,the slow diffusion of multivalent-metal ions and the shuttle of soluble polysulfide result in impoverished reversible capacity and limited cycle performance of M-S(Mg-S,Al-S,Ca-S,Zn-S,Fe-S,etc.)batteries.It is a necessity to optimize the electrochemical performance,while deepening the understanding of the unique electrochemical reaction mechanism,such as the intrinsic multi-electron reaction process,polysulfides dissoluti on and the in stability of metal an odes.To solve these problems,we have summarized the state-of-the-art progress of current M-S batteries,and sorted out the existing challen ges for different multivalent M-S batteries according to sulfur cathode,electrolytes,metallic an ode and current collectors/separators,respectively.In this literature,we have surveyed and exemplified the strategies developed for better M-S batteries to strengthen the application of green,cost-effective and high energy density M-S batteries.展开更多
In this paper we derive certain sufficient conditions for starlikeness and convexity of order α of meromorphically multivalent functions in the punctured unit disk.
Wearable self-powered systems integrated with energy conversion and storage devices such as solar-charging power units arouse widespread concerns in scientific and industrial realms.However,their applications are hamp...Wearable self-powered systems integrated with energy conversion and storage devices such as solar-charging power units arouse widespread concerns in scientific and industrial realms.However,their applications are hampered by the restrictions of unbefitting size matching between integrated modules,limited tolerance to the variation of input current,reliability,and safety issues.Herein,flexible solar-charging self-powered units based on printed Zn-ion hybrid micro-capacitor as the energy storage module is developed.Unique 3D micro-/nano-architecture of the biomass kelp-carbon combined with multivalent ion(Zn2+)storage endows the aqueous Zn-ion hybrid capacitor with high specific capacity(196.7 mAh g^−1 at 0.1 A g^−1).By employing an in-plane asymmetric printing technique,the fabricated quasi-solid-state Zn-ion hybrid microcapacitors exhibit high rate,long life and energy density up to 8.2μWh cm^−2.After integrating the micro-capacitor with organic solar cells,the derived self-powered system presents outstanding energy conversion/storage efficiency(ηoverall=17.8%),solar-charging cyclic stability(95%after 100 cycles),wide current tolerance,and good mechanical flexibility.Such portable,wearable,and green integrated units offer new insights into design of advanced self-powered systems toward the goal of developing highly safe,economic,stable,and long-life smart wearable electronics.展开更多
Flexible aqueous batteries have been thriving with the growing demand for wearable and portable electrical devices.In particular,flexible aqueous mul tivalent ion batteries(FAMIBs),the charge carriers of which include...Flexible aqueous batteries have been thriving with the growing demand for wearable and portable electrical devices.In particular,flexible aqueous mul tivalent ion batteries(FAMIBs),the charge carriers of which include Zn^(2+),Al^(3+),Mg^(2+),and Ca^(2+),have great potential for development owing to their high safety,high elemental abundance in the Earth's crust,and a multi-electron redox mechanism with a high theoretical specific capacity.Therefore,for a comprehensive understanding of this developing field,it is necessary to summarize the recent research progress of FAMIBs in a timely manner.Herein,the advancements of the state-of-the-art FAMIBs are reviewed,and the prospects toward this field are also proposed.This study focuses on the rational material and configuration design for FAMIBs in recent studies to achieve high battery performances under deformation conditions,which is elaborated on by classification of the anode,cathode,hydrogel electrolyte,and configurations of FAMIBs.Besides,the electrochemical performance of FAMIBs under flexible conditions is also reviewed from the perspective of their working voltage,specific capacity,and cycling stability.Finally,the ap proaches to improve the performance of FAMIBs are comprehensively eval uated,followed by the outlook on the challenges and opportunities in future development of FAMIBs.展开更多
In recent years,the pursuit of high-efficiency electrochemical storage technology,the multivalent metalion batteries (MIBs) based on aqueous electrolytes have been widely explored by researchers because of their safet...In recent years,the pursuit of high-efficiency electrochemical storage technology,the multivalent metalion batteries (MIBs) based on aqueous electrolytes have been widely explored by researchers because of their safety,environmental friendliness,abundant reserves and low price,and especially the merits in energy and power densities.This review firstly expounds on the problems existing in the electrode materials of aqueous multivalent MIBs (Zn^(2+),Mg^(2+),Al^(3+),Ca^(2+)),from the classical inorganic materials to the emerging organic compounds,and then summarizes the design strategies in bulk and interface structure of electrodes with favorable kinetics and stable cycling performance,especially laying the emphasis on the charge storage mechanism of cathode materials and dendrite-free Zinc anode from the aspect of electrolyte optimization strategies,which can be extended to other aqueous multivalent MIBs.Ultimately,the possible development directions of the aqueous multivalent MIBs in the future are provided,anticipating to provide a meaningful guideline for researchers in this area.展开更多
Rechargeable aluminum batteries(RABs),which use earth-abundant and high-volumetric-capacity metal anodes(8040 m Ah cm-3),have great potential as next-generation power sources because they use cheaper resources to deli...Rechargeable aluminum batteries(RABs),which use earth-abundant and high-volumetric-capacity metal anodes(8040 m Ah cm-3),have great potential as next-generation power sources because they use cheaper resources to deliver higher energies,compared to current lithium ion batteries.However,the mechanism of charge delivery in the newly developed,ionic liquid-based electrolytic system for RABs differs from that in conventional organic electrolytes.Thus,targeted research efforts are required to address the large overpotentials and cycling decay encountered in the ionic liquid-based electrolytic system.In this study,a nanoporous carbon(NPC)electrode with well-developed nanopores is used to develop a high-performance aluminum anode.The negatively charged nanopores can provide quenched dynamics of electrolyte molecules in the aluminum deposition process,resulting in an increased collision rate.The fast chemical equilibrium of anionic species induced by the facilitated anionic collisions leads to more favorable reduction reactions that form aluminum metals.The nanoconfinement effect causes separated nucleation and growth of aluminum nanoparticles in the multiple confined nanopores,leading to higher coulombic efficiencies and more stable cycling performance compared with macroporous carbon black and 2D stainless steel electrodes.展开更多
Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(U...Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(UF)is generally used for concentration of polymers.Furthermore,the introduction of multivalent metal ions into alginate may provide a promising method for the development of novel nanomaterials.In this study,membrane fouling mitigation by multivalent metal ions,both individually and in combination,and properties of recycled materials were investigated for UF recovery of sodium alginate(SA).The filtration resistance showed a significantly negative correlation with the concentration of metal ions,arranged in the order of Mg^2+<Ca^2+<Fe^3+<Al^3+(filtration resistance mitigation),and the moisture content of recycled filter cake showed a marked decrease.For Ca^2+,Mg^2+,Fe^3+,and Ca^2++Fe^3+,the filtration resistances were almost the same when the total charge concentration was less than 5 mmol·L^–1.However,when the total charge concentration was greater than 5 mmol·L^–1,membrane fouling mitigation increased significantly in the presence of Ca^2+or Fe^3+and remained constant for Mg^2+with the increase of total charge concentration.The filtration resistance mitigation was arranged in the order of Fe^3+>Fe^3++Ca^2+>Ca^2+>Mg^2+.Three mechanisms were proposed in the presence of Fe^3+,such as the decrease of SA concentration,change in p H,and production of hydroxide iron colloids from hydrolysis.The properties of recycled materials(filter cake)were investigated via optical microscope observation,dynamic light scattering,Fourier transform infrared,X-ray photoelectron spectroscopy(XPS),and scanning electron microscopy.The results provide further insight into UF recoveries of alginate extracted from AGS.展开更多
The condensation of DNA induced by spermine is studied by atomic force microscopy (AFM) and molecular dynamics (MD) simulation in this paper. In our experiments, an equivalent amount of multivalent cations is adde...The condensation of DNA induced by spermine is studied by atomic force microscopy (AFM) and molecular dynamics (MD) simulation in this paper. In our experiments, an equivalent amount of multivalent cations is added to the DNA solutions in different numbers of steps, and we find that the process of DNA condensation strongly depends on the speed of adding cations. That is, the slower the spermine cations are added, the slower the DNA aggregates. The MD and steered molecular dynamics (SMD) simulation results agree well with the experimental results, and the simulation data also show that the more steps of adding multivalent cations there are, the more compact the condensed DNA structure will be. This investigation can help us to control DNA condensation and understand the complicated structures of DNA--cation complexes.展开更多
In this paper, we introduce some new subclasses of meromorphically uniformly reciprocal starlike functions associated with the generalized Dziok-Srivastava operator and its corresponding integral operator defined by s...In this paper, we introduce some new subclasses of meromorphically uniformly reciprocal starlike functions associated with the generalized Dziok-Srivastava operator and its corresponding integral operator defined by subordination. We obtain the inclusion relation,sufficient conditions and majorization property of the class. Moreover, we point out some new and interesting corollaries of our main result. These results generalize some known results.展开更多
The purpose of this article is to obtain some subordination and superordi- nation preserving properties of meromorphic multivalent functions in the punctured open unit disk associated with the Liu-Srivastava operator....The purpose of this article is to obtain some subordination and superordi- nation preserving properties of meromorphic multivalent functions in the punctured open unit disk associated with the Liu-Srivastava operator. The sandwich-type results for these meromorphic multivalent functions are also considered.展开更多
Using molecular dynamics simulations and atomic force microscopy (AFM), we study the decondensation process of DNA chains induced by multivalent cations at high salt concentrations in the presence of short cationic ...Using molecular dynamics simulations and atomic force microscopy (AFM), we study the decondensation process of DNA chains induced by multivalent cations at high salt concentrations in the presence of short cationic chains in solutions. The typical simulation conformations of DNA chains with varying salt concentrations for multivalent cations imply that the concentration of salt cations and the valence of multivalent cations have a strong influence on the process of DNA decondensation. The DNA chains are condensed in the absence of salt or at low salt concentrations, and the compacted conformations of DNA chains become loose when a number of cations and anions are added into the solution. It is explicitly demonstrated that cations can overcompensate the bare charge of the DNA chains and weaken the attraction interactions between the DNA chains and short cationic chains at high salt concentrations. The condensation-decondensation transi- tions of DNA are also experimentally observed in mixing spermidine with X-phage DNA at different concentrations of NaCl/MgCl2 solutions.展开更多
Based on the density functional theory(DFT) calculations,we showed that the interactions between different valence anions(PO_(4)^(3-),CH_(3)PO_(4)^(2-),(CH_(3))_(2)PO_(4)^(-)) and graphene significantly increased as t...Based on the density functional theory(DFT) calculations,we showed that the interactions between different valence anions(PO_(4)^(3-),CH_(3)PO_(4)^(2-),(CH_(3))_(2)PO_(4)^(-)) and graphene significantly increased as the valence of anion increased from negative monovalence to negative trivalence.The adsorption energy of(CH_(3))_(2)PO_(4)^(-)on the electron-rich graphene flake(C84H24)is-8.3 kcal/mol.The adsorption energy of CH_(3)PO_(4)^(2-) on the electron-rich graphene flake(C_(84)H_(24)) is-48.0 kcal/mol,which is about six times that of(CH_(3))_(2)PO_(4) adsorption on electron-rich graphene flake(C_(84)H_(24)) and is even much larger than that of CO_(3)^(2-) adsorption on electron-deficient aromatic ring C_(6)F_(6)(-28.4 kcal/mol).The adsorption energy of PO_(4)^(3-)on the electron-rich graphene flake(C_(84)H_(24)) is-159.2 kcal/mol,which is about 20 times that of(CH_(3))_(2)PO_(4) adsorption on the graphene flake(C_(84)H_(24)).The super-strong adsorption energy is mainly attributed to the orbital interactions between multivalent anions and graphene.This work provides new insights for understanding the interaction between multivalent anions and π-electron-rich carbon-based nanomaterials and is helpful for the design of graphene-based DNA biosensor.展开更多
Zinc metal anodes(ZMA)have high theoretical capacities(820 mAh g−1 and 5855 mAh cm−3)and redox potential(−0.76 V vs.standard hydrogen electrode),similar to the electrochemical voltage window of the hydrogen evolution ...Zinc metal anodes(ZMA)have high theoretical capacities(820 mAh g−1 and 5855 mAh cm−3)and redox potential(−0.76 V vs.standard hydrogen electrode),similar to the electrochemical voltage window of the hydrogen evolution reaction(HER)in a mild acidic electrolyte system,facilitating aqueous zinc batteries competitive in next-generation energy storage devices.However,the HER and byproduct formation effectuated by water-splitting deteriorate the electrochemical performance of ZMA,limiting their application.In this study,a key factor in promoting the HER in carbon-based electrode materials(CEMs),which can provide a larger active surface area and guide uniform zinc metal deposition,was investigated using a series of threedimensional structured templating carbon electrodes(3D-TCEs)with different local graphitic orderings,pore structures,and surface properties.The ultramicropores of CEMs are the determining critical factors in initiating HER and clogging active surfaces by Zn(OH)2 byproduct formation,through a systematic comparative study based on the 3D-TCE series samples.When the 3D-TCEs had a proper graphitic structure with few ultramicropores,they showed highly stable cycling performances over 2000 cycles with average Coulombic efficiencies of≥99%.These results suggest that a well-designed CEM can lead to high-performance ZMA in aqueous zinc batteries.展开更多
Making use of the Cho-Kwon-Srivastava operator, we introduce and study a certain SCn (j, p, λ, α, δ) of p-valently analytic functions with negative coefficients. In this paper, we obtain coefficient estimates, dist...Making use of the Cho-Kwon-Srivastava operator, we introduce and study a certain SCn (j, p, λ, α, δ) of p-valently analytic functions with negative coefficients. In this paper, we obtain coefficient estimates, distortion theorem, radii of close-to-convexity, starlikeness and convexity and modified Hadamard products of functions belonging to the class SCn (j, p, λ, α, δ). Finally, several applications investigate an integral operator, and certain fractional calculus operators also considered.展开更多
By using a method based upon the Briot-Bouquet differential subordination, we investigate some subordination properties of the generalized fractional integral operator which was defined by Owa, Saigo and Srivastava [1...By using a method based upon the Briot-Bouquet differential subordination, we investigate some subordination properties of the generalized fractional integral operator which was defined by Owa, Saigo and Srivastava [1]. Some interesting further consequences are also considered.展开更多
基金National Natural Science Foundation of China(52202299)the Analytical&Testing Center of Northwestern Polytechnical University(2022T006).
文摘With the rapid development of portable electronics and electric road vehicles,high-energy-density batteries have been becoming front-burner issues.Traditionally,homogeneous electrolyte cannot simultaneously meet diametrically opposed demands of high-potential cathode and low-potential anode,which are essential for high-voltage batteries.Meanwhile,homogeneous electrolyte is difficult to achieve bi-or multi-functions to meet different requirements of electrodes.In comparison,the asymmetric electrolyte with bi-or multi-layer disparate components can satisfy distinct requirements by playing different roles of each electrolyte layer and meanwhile compensates weakness of individual electrolyte.Consequently,the asymmetric electrolyte can not only suppress by-product sedimentation and continuous electrolyte decomposition at the anode while preserving active substances at the cathode for high-voltage batteries with long cyclic lifespan.In this review,we comprehensively divide asymmetric electrolytes into three categories:decoupled liquid-state electrolytes,bi-phase solid/liquid electrolytes and decoupled asymmetric solid-state electrolytes.The design principles,reaction mechanism and mutual compatibility are also studied,respectively.Finally,we provide a comprehensive vision for the simplification of structure to reduce costs and increase device energy density,and the optimization of solvation structure at anolyte/catholyte interface to realize fast ion transport kinetics.
基金Supported by The Science and Technology Project of General Administration of Quality Supervision,Inspection and Quarantine (2015IK126)The Science and Technology Project of Changsha City of Hunan Province of China (KQ1602124).
文摘Mercury ion(Hg^(2+)),a highly noxious of heavy metalion,has detrimental effects on the ecological environment and human health.Herein,we have developed an exonuclease III(Exo III)assisted catalytic hairpin assembly formation of a trivalent G-quadruplex/hemin DNAzyme for colorimetric detection of Hg^(2+).A hairpin DNA(Hr)was designed with thymine-Hg^(2+)-thymine pairs that catalyzed by Exo III is prompted to happen upon binding Hg^(2+).A released DNA fragment triggers the catalytic assembly of other three hairpins(H1,H2,and H3)to form many trivalent G-quadruplex/hemin DNA enzymes for signal output.The developed sensor shows a dynamic range from 2 pM to 2μM,with an impressively low detection limit of 0.32 pM for Hg^(2+)detection.Such a sensor also has good selectivity toward Hg^(2+)detection in the presence of other common metal ions.This strategy shows the great potential for visual detection with portable type.
文摘Objective:This study aimed to describe,optimize and evaluate a method for preparing multivalent conjugate vaccines by simultaneous conjugation of two different bacterial capsular polysaccharides(CPs)with tetanus toxoid(TT)as bivalent conjugates.Methods:Different molecular weights(MWs)of polysaccharides,activating agents and capsular polysaccharide/protein(CP/Pro)ratio that may influence conjugation and immunogenicity were investigated and optimized to prepare the bivalent conjugate bulk.Using the described method and optimized parameters,a 20-valent pneumococcal conjugate vaccine and a bivalent meningococcal vaccine were developed and their effectiveness was compared to that of corresponding licensed vaccines in rabbit or mouse models.Results:The immunogenicity test revealed that polysaccharides with lower MWs were better for Pn1-TT-Pn3 and MenA-TT-MenC,while higher MWs were superior for Pn4-TT-Pn14,Pn6A-TT-Pn6B,Pn7F-TT-Pn23F and Pn8-TT-Pn11A.For activating polysaccharides,1-cyano-4-dimethylaminopyridinium tetrafluoroborate(CDAP)was superior to cyanogen bromide(CNBr),but for Pn1,Pn3 and MenC,N-(3-dimethylaminopropyl)-N’-ethylcarbodiimide hydrochloride(EDAC)was the most suitable option.For Pn6A-TT-Pn6B and Pn8-TT-Pn11A,rabbits immunized with bivalent conjugates with lower CP/Pro ratios showed significantly stronger CP-specific antibody responses,while for Pn4-TT-Pn14,higher CP/Pro ratio was better.Instead of interfering with the respective immunological activity,our bivalent conjugates usually induced higher IgG titers than their monovalent counterparts.Conclusion:The result indicated that the described conjugation technique was feasible and efficacious to prepare glycoconjugate vaccines,laying a solid foundation for developing extended-valent multivalent or combined conjugate vaccines without potentially decreased immune function.
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.
文摘Making use of multivalent functions with negative coefficients of the type f (z)=z^(p)-~(∑)_(k=p+1)^(∞)a_(k)z^(k),which are analytic in the open unit disk and applying the q-derivative a q–differintegral operator is considered.Furthermore by using the familiar Riesz-Dunford integral,a linear operator on Hilbert space H is introduced.A new subclass of p-valent functions related to an operator on H is defined.Coefficient estimate,distortion bound and extreme points are obtained.The convolution-preserving property is also investigated.
基金supported by the National Natural Science Foundation of China (22075028)the Beijing Institute of Technology Research Fund Program for Young Scholars (2019CX04092).
文摘Multivalent metal-sulfur(M-S,where M=Mg,Al,Ca,Zn,Fe,etc.)batteries offer unique opportunities to achieve high specific capacity,elemental abundancy and cost-effectiveness beyond lithium-ion batteries(LIBs).However,the slow diffusion of multivalent-metal ions and the shuttle of soluble polysulfide result in impoverished reversible capacity and limited cycle performance of M-S(Mg-S,Al-S,Ca-S,Zn-S,Fe-S,etc.)batteries.It is a necessity to optimize the electrochemical performance,while deepening the understanding of the unique electrochemical reaction mechanism,such as the intrinsic multi-electron reaction process,polysulfides dissoluti on and the in stability of metal an odes.To solve these problems,we have summarized the state-of-the-art progress of current M-S batteries,and sorted out the existing challen ges for different multivalent M-S batteries according to sulfur cathode,electrolytes,metallic an ode and current collectors/separators,respectively.In this literature,we have surveyed and exemplified the strategies developed for better M-S batteries to strengthen the application of green,cost-effective and high energy density M-S batteries.
文摘In this paper we derive certain sufficient conditions for starlikeness and convexity of order α of meromorphically multivalent functions in the punctured unit disk.
基金the National Natural Science Foundation of Hubei Province(Grant No.2019CFB110)the fund of the Shaanxi Key Laboratory of Fiber Reinforced Light Composite Materials(Grant No.1-KF-2019).
文摘Wearable self-powered systems integrated with energy conversion and storage devices such as solar-charging power units arouse widespread concerns in scientific and industrial realms.However,their applications are hampered by the restrictions of unbefitting size matching between integrated modules,limited tolerance to the variation of input current,reliability,and safety issues.Herein,flexible solar-charging self-powered units based on printed Zn-ion hybrid micro-capacitor as the energy storage module is developed.Unique 3D micro-/nano-architecture of the biomass kelp-carbon combined with multivalent ion(Zn2+)storage endows the aqueous Zn-ion hybrid capacitor with high specific capacity(196.7 mAh g^−1 at 0.1 A g^−1).By employing an in-plane asymmetric printing technique,the fabricated quasi-solid-state Zn-ion hybrid microcapacitors exhibit high rate,long life and energy density up to 8.2μWh cm^−2.After integrating the micro-capacitor with organic solar cells,the derived self-powered system presents outstanding energy conversion/storage efficiency(ηoverall=17.8%),solar-charging cyclic stability(95%after 100 cycles),wide current tolerance,and good mechanical flexibility.Such portable,wearable,and green integrated units offer new insights into design of advanced self-powered systems toward the goal of developing highly safe,economic,stable,and long-life smart wearable electronics.
基金supported by the National Natural Science Foundation of China(51822201,52172178,and 21972007).
文摘Flexible aqueous batteries have been thriving with the growing demand for wearable and portable electrical devices.In particular,flexible aqueous mul tivalent ion batteries(FAMIBs),the charge carriers of which include Zn^(2+),Al^(3+),Mg^(2+),and Ca^(2+),have great potential for development owing to their high safety,high elemental abundance in the Earth's crust,and a multi-electron redox mechanism with a high theoretical specific capacity.Therefore,for a comprehensive understanding of this developing field,it is necessary to summarize the recent research progress of FAMIBs in a timely manner.Herein,the advancements of the state-of-the-art FAMIBs are reviewed,and the prospects toward this field are also proposed.This study focuses on the rational material and configuration design for FAMIBs in recent studies to achieve high battery performances under deformation conditions,which is elaborated on by classification of the anode,cathode,hydrogel electrolyte,and configurations of FAMIBs.Besides,the electrochemical performance of FAMIBs under flexible conditions is also reviewed from the perspective of their working voltage,specific capacity,and cycling stability.Finally,the ap proaches to improve the performance of FAMIBs are comprehensively eval uated,followed by the outlook on the challenges and opportunities in future development of FAMIBs.
基金supported by the National Key R&D Program of China(2016YFA0202500)the Natural Science Foundation of China(51803054,51772093)+1 种基金the Natural Science Foundation of Hunan province(2020JJ3022,2019JJ50223,2019JJ20010)the foundation from Education Department of Hunan Province(19B270,SYL201802008)。
文摘In recent years,the pursuit of high-efficiency electrochemical storage technology,the multivalent metalion batteries (MIBs) based on aqueous electrolytes have been widely explored by researchers because of their safety,environmental friendliness,abundant reserves and low price,and especially the merits in energy and power densities.This review firstly expounds on the problems existing in the electrode materials of aqueous multivalent MIBs (Zn^(2+),Mg^(2+),Al^(3+),Ca^(2+)),from the classical inorganic materials to the emerging organic compounds,and then summarizes the design strategies in bulk and interface structure of electrodes with favorable kinetics and stable cycling performance,especially laying the emphasis on the charge storage mechanism of cathode materials and dendrite-free Zinc anode from the aspect of electrolyte optimization strategies,which can be extended to other aqueous multivalent MIBs.Ultimately,the possible development directions of the aqueous multivalent MIBs in the future are provided,anticipating to provide a meaningful guideline for researchers in this area.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)Funded by the Ministry of Education(NRF-2019R1A2C1084836,NRF-2018M1A2A2061994,and NRF-2021R1A4A2001403)the KU-KIST School Program。
文摘Rechargeable aluminum batteries(RABs),which use earth-abundant and high-volumetric-capacity metal anodes(8040 m Ah cm-3),have great potential as next-generation power sources because they use cheaper resources to deliver higher energies,compared to current lithium ion batteries.However,the mechanism of charge delivery in the newly developed,ionic liquid-based electrolytic system for RABs differs from that in conventional organic electrolytes.Thus,targeted research efforts are required to address the large overpotentials and cycling decay encountered in the ionic liquid-based electrolytic system.In this study,a nanoporous carbon(NPC)electrode with well-developed nanopores is used to develop a high-performance aluminum anode.The negatively charged nanopores can provide quenched dynamics of electrolyte molecules in the aluminum deposition process,resulting in an increased collision rate.The fast chemical equilibrium of anionic species induced by the facilitated anionic collisions leads to more favorable reduction reactions that form aluminum metals.The nanoconfinement effect causes separated nucleation and growth of aluminum nanoparticles in the multiple confined nanopores,leading to higher coulombic efficiencies and more stable cycling performance compared with macroporous carbon black and 2D stainless steel electrodes.
基金partially supported by the Beijing Outstanding Talents TrainingScience and Technology Programs of the Beijing Municipal Education Commission(SQKM201710016001)+1 种基金the BUCEA Post Graduate Innovation Projectthe Beijing Advanced Innovation Center for Future Urban Design。
文摘Recovery of alginate extracted from aerobic granular sludge(AGS)has given rise to a novel research direction.However,these extracted alginate solutions have a water content of nearly 100%.Alternately,ultrafiltration(UF)is generally used for concentration of polymers.Furthermore,the introduction of multivalent metal ions into alginate may provide a promising method for the development of novel nanomaterials.In this study,membrane fouling mitigation by multivalent metal ions,both individually and in combination,and properties of recycled materials were investigated for UF recovery of sodium alginate(SA).The filtration resistance showed a significantly negative correlation with the concentration of metal ions,arranged in the order of Mg^2+<Ca^2+<Fe^3+<Al^3+(filtration resistance mitigation),and the moisture content of recycled filter cake showed a marked decrease.For Ca^2+,Mg^2+,Fe^3+,and Ca^2++Fe^3+,the filtration resistances were almost the same when the total charge concentration was less than 5 mmol·L^–1.However,when the total charge concentration was greater than 5 mmol·L^–1,membrane fouling mitigation increased significantly in the presence of Ca^2+or Fe^3+and remained constant for Mg^2+with the increase of total charge concentration.The filtration resistance mitigation was arranged in the order of Fe^3+>Fe^3++Ca^2+>Ca^2+>Mg^2+.Three mechanisms were proposed in the presence of Fe^3+,such as the decrease of SA concentration,change in p H,and production of hydroxide iron colloids from hydrolysis.The properties of recycled materials(filter cake)were investigated via optical microscope observation,dynamic light scattering,Fourier transform infrared,X-ray photoelectron spectroscopy(XPS),and scanning electron microscopy.The results provide further insight into UF recoveries of alginate extracted from AGS.
基金supported by the National Natural Science Foundation of China (Grant Nos. 20974081, 20934004, 21174131, and 21104060)the Zhejiang Provincial Natural Science Foundation of China (Grant No. Y4110357)
文摘The condensation of DNA induced by spermine is studied by atomic force microscopy (AFM) and molecular dynamics (MD) simulation in this paper. In our experiments, an equivalent amount of multivalent cations is added to the DNA solutions in different numbers of steps, and we find that the process of DNA condensation strongly depends on the speed of adding cations. That is, the slower the spermine cations are added, the slower the DNA aggregates. The MD and steered molecular dynamics (SMD) simulation results agree well with the experimental results, and the simulation data also show that the more steps of adding multivalent cations there are, the more compact the condensed DNA structure will be. This investigation can help us to control DNA condensation and understand the complicated structures of DNA--cation complexes.
基金Supported by the National Natural Science Foundation of China(11561001)Supported by the Natural Science Foundation of Inner Mongolia Province(2014MS0101)Supported by the Higher School Foundation of Inner Mongolia Province(2015NJZY240)
文摘In this paper, we introduce some new subclasses of meromorphically uniformly reciprocal starlike functions associated with the generalized Dziok-Srivastava operator and its corresponding integral operator defined by subordination. We obtain the inclusion relation,sufficient conditions and majorization property of the class. Moreover, we point out some new and interesting corollaries of our main result. These results generalize some known results.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF) funded by the Ministry of Education,Science and Technology (2010-0017111)
文摘The purpose of this article is to obtain some subordination and superordi- nation preserving properties of meromorphic multivalent functions in the punctured open unit disk associated with the Liu-Srivastava operator. The sandwich-type results for these meromorphic multivalent functions are also considered.
基金supported by the National Natural Science Foundation of China(Grant No.31340026)the Natural Science Foundation of Zhejiang Province,China(Grant Nos.Z13F20019 and LQ12E01003)the Science and Technology Project of Zhejiang Science and Technology Department,China(Grant No.2014C31147)
文摘Using molecular dynamics simulations and atomic force microscopy (AFM), we study the decondensation process of DNA chains induced by multivalent cations at high salt concentrations in the presence of short cationic chains in solutions. The typical simulation conformations of DNA chains with varying salt concentrations for multivalent cations imply that the concentration of salt cations and the valence of multivalent cations have a strong influence on the process of DNA decondensation. The DNA chains are condensed in the absence of salt or at low salt concentrations, and the compacted conformations of DNA chains become loose when a number of cations and anions are added into the solution. It is explicitly demonstrated that cations can overcompensate the bare charge of the DNA chains and weaken the attraction interactions between the DNA chains and short cationic chains at high salt concentrations. The condensation-decondensation transi- tions of DNA are also experimentally observed in mixing spermidine with X-phage DNA at different concentrations of NaCl/MgCl2 solutions.
基金Project supported by the National Natural Science Foundation of China for Outstanding Young Scholars(Grant No.11722548)the China Postdoctoral Science Foundation(Grant No.2019M651462)+4 种基金the National Natural Science Foundation of China(Grant No.U1932123)the Innovative Research Team of High-Level Local Universities in Shanghaithe Open Project of State Key Laboratory of Advanced Special Steel,Shanghai Key Laboratory of Advanced Ferrometallurgy and the Science and Technology Commission of Shanghai Municipality(Gant No.19DZ2270200)the Deepcomp7000 and Sc Grid of Supercomputing Center,Computer Network Information Center of the Chinese Academy of Sciences,the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund(second phase)the Shanghai Supercomputer Center of China,the High Performance Computing Platform of Shanghai University。
文摘Based on the density functional theory(DFT) calculations,we showed that the interactions between different valence anions(PO_(4)^(3-),CH_(3)PO_(4)^(2-),(CH_(3))_(2)PO_(4)^(-)) and graphene significantly increased as the valence of anion increased from negative monovalence to negative trivalence.The adsorption energy of(CH_(3))_(2)PO_(4)^(-)on the electron-rich graphene flake(C84H24)is-8.3 kcal/mol.The adsorption energy of CH_(3)PO_(4)^(2-) on the electron-rich graphene flake(C_(84)H_(24)) is-48.0 kcal/mol,which is about six times that of(CH_(3))_(2)PO_(4) adsorption on electron-rich graphene flake(C_(84)H_(24)) and is even much larger than that of CO_(3)^(2-) adsorption on electron-deficient aromatic ring C_(6)F_(6)(-28.4 kcal/mol).The adsorption energy of PO_(4)^(3-)on the electron-rich graphene flake(C_(84)H_(24)) is-159.2 kcal/mol,which is about 20 times that of(CH_(3))_(2)PO_(4) adsorption on the graphene flake(C_(84)H_(24)).The super-strong adsorption energy is mainly attributed to the orbital interactions between multivalent anions and graphene.This work provides new insights for understanding the interaction between multivalent anions and π-electron-rich carbon-based nanomaterials and is helpful for the design of graphene-based DNA biosensor.
基金National Research Foundation of Korea,Grant/Award Numbers:NRF-2019R1A2C1084836,NRF-2021R1A4A2001403,NRF-2022R1C1C1011484。
文摘Zinc metal anodes(ZMA)have high theoretical capacities(820 mAh g−1 and 5855 mAh cm−3)and redox potential(−0.76 V vs.standard hydrogen electrode),similar to the electrochemical voltage window of the hydrogen evolution reaction(HER)in a mild acidic electrolyte system,facilitating aqueous zinc batteries competitive in next-generation energy storage devices.However,the HER and byproduct formation effectuated by water-splitting deteriorate the electrochemical performance of ZMA,limiting their application.In this study,a key factor in promoting the HER in carbon-based electrode materials(CEMs),which can provide a larger active surface area and guide uniform zinc metal deposition,was investigated using a series of threedimensional structured templating carbon electrodes(3D-TCEs)with different local graphitic orderings,pore structures,and surface properties.The ultramicropores of CEMs are the determining critical factors in initiating HER and clogging active surfaces by Zn(OH)2 byproduct formation,through a systematic comparative study based on the 3D-TCE series samples.When the 3D-TCEs had a proper graphitic structure with few ultramicropores,they showed highly stable cycling performances over 2000 cycles with average Coulombic efficiencies of≥99%.These results suggest that a well-designed CEM can lead to high-performance ZMA in aqueous zinc batteries.
文摘Making use of the Cho-Kwon-Srivastava operator, we introduce and study a certain SCn (j, p, λ, α, δ) of p-valently analytic functions with negative coefficients. In this paper, we obtain coefficient estimates, distortion theorem, radii of close-to-convexity, starlikeness and convexity and modified Hadamard products of functions belonging to the class SCn (j, p, λ, α, δ). Finally, several applications investigate an integral operator, and certain fractional calculus operators also considered.
文摘By using a method based upon the Briot-Bouquet differential subordination, we investigate some subordination properties of the generalized fractional integral operator which was defined by Owa, Saigo and Srivastava [1]. Some interesting further consequences are also considered.