Emulsification is one of the important mechanisms of surfactant flooding. To improve oil recovery for low permeability reservoirs, a highly efficient emulsification oil flooding system consisting of anionic surfactant...Emulsification is one of the important mechanisms of surfactant flooding. To improve oil recovery for low permeability reservoirs, a highly efficient emulsification oil flooding system consisting of anionic surfactant sodium alkyl glucosyl hydroxypropyl sulfonate(APGSHS) and zwitterionic surfactant octadecyl betaine(BS-18) is proposed. The performance of APGSHS/BS-18 mixed surfactant system was evaluated in terms of interfacial tension, emulsification capability, emulsion size and distribution, wettability alteration, temperature-resistance and salt-resistance. The emulsification speed was used to evaluate the emulsification ability of surfactant systems, and the results show that mixed surfactant systems can completely emulsify the crude oil into emulsions droplets even under low energy conditions. Meanwhile,the system exhibits good temperature and salt resistance. Finally, the best oil recovery of 25.45% is achieved for low permeability core by the mixed surfactant system with a total concentration of 0.3 wt%while the molar ratio of APGSHS:BS-18 is 4:6. The current study indicates that the anionic/zwitterionic mixed surfactant system can improve the oil flooding efficiency and is potential candidate for application in low permeability reservoirs.展开更多
For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and kinetics.In this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of sol...For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and kinetics.In this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of solvent on the mechanism and kinetics of LAP was revealed through a strategy combining density functional theory(DFT)calculations and kinetic modeling.In terms of mechanism,it is found that the stronger the solvent polarity,the more electrons transfer from initiator to solvent through detailed energy decomposition analysis of electrostatic interactions between initiator and solvent molecules.Furthermore,we also found that the stronger the solvent polarity,the higher the monomer initiation energy barrier and the smaller the initiation rate coefficient.Counterintuitively,initiation is more favorable at lower temperatures based on the calculated results ofΔG_(TS).Finally,the kinetic characteristics in different solvents were further examined by kinetic modeling.It is found that in benzene and n-pentane,the polymerization rate exhibits first-order kinetics.While,slow initiation and fast propagation were observed in tetrahydrofuran(THF)due to the slow free ion formation rate,leading to a deviation from first-order kinetics.展开更多
The anionic redox has been widely studied in layered-oxide-cathodes in attempts to achieve highenergy-density for Na-ion batteries(NIBs).It is known that an oxidation state of Mn^(4+) or Ru^(5+) is essential for the a...The anionic redox has been widely studied in layered-oxide-cathodes in attempts to achieve highenergy-density for Na-ion batteries(NIBs).It is known that an oxidation state of Mn^(4+) or Ru^(5+) is essential for the anionic reaction of O^(2-)/O~-to occur during Na^(+) de/intercalation.However,here,we report that the anionic redox can occur in Ru-based layered-oxide-cathodes before full oxidation of Ru^(4+)/Ru^(5+).Combining studies using first-principles calculation and experimental techniques reveals that further Na^(+) deintercalation from P2-Na_(0.33)[Mg_(0.33)Ru_(0.67)]O_(2) is based on anionic oxidation after 0.33 mol Na^(+) deintercalation from P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) with cationic oxidation of Ru^(4+)/Ru^(4.5+).Especially,it is revealed that the only oxygen neighboring 2Mg/1 Ru can participate in the anionic redox during Na^(+) de/intercalation,which implies that the Na-O-Mg arrangement in the P2-Na_(0.33)[M9_(0.33)Ru_(0.67)]O_(2) structure can dramatically lower the thermodynamic stability of the anionic redox than that of cationic redox.Through the O anionic and Ru cationic reaction,P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) exhibits not only a large specific capacity of~172 mA h g^(-1) but also excellent power-capability via facile Na^(+) diffusion and reversible structural change during charge/discharge.These findings suggest a novel strategy that can increase the activity of anionic redox by modulating the local environment around oxygen to develop high-energy-density cathode materials for NIBs.展开更多
The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy.In this context,metal-organic frameworks(MOFs),with their unique 3D porous st...The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy.In this context,metal-organic frameworks(MOFs),with their unique 3D porous structure and tunable chemical functionality,have shown enormous potential as energy storage materials for accommodating or transporting electrochemically active ions.In this perspective,we specifically focus on the current status and prospects of anionic MOF-based quasi-solid-state-electrolytes(anionic MOF-QSSEs)for lithium metal batteries(LMBs).An overview of the definition,design,and properties of anionic MOF-QSSEs is provided,including recent advances in the understanding of their ion transport mechanism.To illustrate the advantages of using anionic MOF-QSSEs as electrolytes for LMBs,a thorough comparison between anionic MOF-QSSEs and other well-studied electrolyte systems is made.With these in-depth understandings,viable techniques for tuning the chemical and topological properties of anionic MOF-QSSEs to increase Li+conductivity are discussed.Beyond modulation of the MOFs matrix,we envisage that solvent and solid-electrolyte interphase design as well as emerging fabrication techniques will aid in the design and practical application of anionic MOF-QSSEs.展开更多
A new electrophilic polymer, 2,4-dinitrophenyl ether of polyvinyl alcohol (PVA-DNP), having a degree of substitution of 0.5 was prepared from polyvinyl alcohol (PVA) and 1-fluro-2,4-dinitrobenzene (DNFB). The PVA-DNP ...A new electrophilic polymer, 2,4-dinitrophenyl ether of polyvinyl alcohol (PVA-DNP), having a degree of substitution of 0.5 was prepared from polyvinyl alcohol (PVA) and 1-fluro-2,4-dinitrobenzene (DNFB). The PVA-DNP polymer was characterized by NMR, IR, and UV-visible spectroscopy. The reaction of PVA-DNP with sodium methoxide was followed by NMR and UV-visible spectroscopy. Evidence of polymer bound spirocyclic SIGMA complex, C-1 and C-3 polymer bound DNP-methoxy SIGMA complexes and the formation and C-1 methoxy complex of 2,4-dinitroanisole was observed.展开更多
In order to reduce the impact of eutrophication caused by agricultural residues (i.e., excess nitrate) in aqueous solution, economic and effective anionic sorbents are required. In this article, we prepared anionic ...In order to reduce the impact of eutrophication caused by agricultural residues (i.e., excess nitrate) in aqueous solution, economic and effective anionic sorbents are required. In this article, we prepared anionic sorbent using wheat straw. Its structural characteristics and adsorption properties for nitrate removal from aqueous solution were investigated. The results indicate that the yield of the prepared anionic sorbent, the total exchange capacity, and the maximum adsorption capacity were 350%, 2.57 mEq/g, and 2.08 mmol/g, respectively. The Freundlich isotherm mode is more suitable than the Langmuir mode and the adsorption process accords with the first order reaction kinetic rate equation. When multiple anions (SO4^2-, H2PO4^-, NO3^-, and NO2^-) were present, the isotherm mode of prepared anionic sorbent for nitrate was consistent with Freundlich mode; however, the capacity of nitrate adsorption was reduced by 50%. In alkaline solutions, about 90% of adsorbed nitrate ions could be desorbed from prepared anionic sorbent. The results of this study confirmed that the wheat straw anionic sorbent can be used as an excellent nitrate sorbent that removes nitrate from aqueous solutions.展开更多
Polyaniline(PANI) was one of the most extensively studied adsorbents due to its low cost and good environmental stability. The objective of the current study was to improve the selective capabilities of PANI for anion...Polyaniline(PANI) was one of the most extensively studied adsorbents due to its low cost and good environmental stability. The objective of the current study was to improve the selective capabilities of PANI for anionic dyes. We found that the acid doped PANI prepared with hydrochloric acid and p-toluenesulfonic acid(PTSA) could selectively adsorb anionic dyes. It exhibited very good selectivity for OG dye, the mechanism was proposed based on the chemical interaction of PANI with the sulfonate group of the dyes. The effects of solution p H, initial dye concentration, and different HCl/PTSA mole ratios on the adsorption capacity of OG have been investigated. Kinetic simulations indicated that the adsorption process could be well represented by pseudo-second-order kinetic plots. The isothermal adsorption curve fitting also showed that the adsorption process could be well described by the Langmuir isothermal equation. The results showed that acid doped PANI could be employed as a promising adsorbent for anion removal from dye wastewater.展开更多
A novel anionic organotin(Ⅳ) complex {[(pClCHCH)Sn(HO)(Cl)OCOCH(O)CH(O)COSn(HO)(Cl)(p-ClCHCH)]·2(HNEt)}(1) was synthesized by the reaction of di(p-chlorobenzy)tin dichloride with the D-tartaric acid in 2:1 molar...A novel anionic organotin(Ⅳ) complex {[(pClCHCH)Sn(HO)(Cl)OCOCH(O)CH(O)COSn(HO)(Cl)(p-ClCHCH)]·2(HNEt)}(1) was synthesized by the reaction of di(p-chlorobenzy)tin dichloride with the D-tartaric acid in 2:1 molar in the presence of an organic base triethylamine. The structure was characterized by elemental analysis, IR, TG, XRD and single-crystal X-ray diffraction. It crystallizes in triclinic, P1 space group, with a = 0.7067(1), b = 1.9762(3), c = 2.2383(3) nm, α = 91.544(2)°, β = 90.075(2)°, γ = 90.110(2)°, V = 3.1247(7) nm~3, Z = 3, Dc = 1.621 g/cm~3, m(Mo Kα) = 16.29 cm–1, F(000) = 1530, R = 0.0394, wR = 0.1092,(Δρ)max = 1224 and(Δρ)min = –840 e/nm~3. The stabilities, orbital energies and composition characteristics of some frontier molecular orbitals of 1 have been carefully investigated with quantum chemistry calculation. In addition, the in vitro antitumor activity suggested that 1 had stronger inhibitory activity on H460, MCF7 than on A549.展开更多
The objective of this study is to develop chitosaneanionic polymers based extendedrelease tablets and test the feasibility of using this system for the sustained release of highly water-soluble drugs with high drug lo...The objective of this study is to develop chitosaneanionic polymers based extendedrelease tablets and test the feasibility of using this system for the sustained release of highly water-soluble drugs with high drug loading.Here,the combination of sodium valproate(VPS)and valproic acid(VPA)were chosen as the model drugs.Anionic polymers studied include xanthan gum(XG),carrageenan(CG),sodium carboxymethyl cellulose(CMC-Na)and sodium alginate(SA).The tablets were prepared by wet granulation method.In vitro drug release was carried out under simulated gastrointestinal condition.Drug release mechanism was studied.Compared with single polymers,chitosaneanionic polymers based system caused a further slowdown of drug release rate.Among them,CS exanthan gum matrix system exhibited the best extended-release behavior and could extend drug release for up to 24 h.Differential scanning calorimetry(DSC)and Fourier transform infrared spectroscopy(FTIR)studies demonstrated that polyelectrolyte complexes(PECs)were formed on the tablet surface,which played an important role on retarding erosion and swelling of the matrix in the later stage.In conclusion,this study demonstrated that it is possible to develop highly water-soluble drugs loaded extendedrelease tablets using chitosaneanionic polymers based system.展开更多
With the merit of high capacity,high safety,and low cost,zinc-ion batteries(ZIBs)possess huge application potential in the domain of large-scale energy storage.However,due to the relatively narrow voltage window and l...With the merit of high capacity,high safety,and low cost,zinc-ion batteries(ZIBs)possess huge application potential in the domain of large-scale energy storage.However,due to the relatively narrow voltage window and large lattice distortion of cationic redox reaction,ZIBs tend to present low energy density,poor kinetics,and unstable cyclic performance.Anion chemistry seems to provide a novel strategy to solve these issues from different aspects,such as enhanced operating voltage,extra capacity contribution,and boosted reaction kinetics.Considering the significance of this theory and the lack of relevant literatures,herein,in-depth comprehension of anionic chemistry and its positive effects on zinc storage performance have been emphasized and summarized.This review aims to present a full scope of anionic chemistry and furnish systematic cognition for rational design of advanced ZIBs with high energy density.Furthermore,insightful analysis and perspectives based on the current research status also have been proposed,which may point out some scientific suggestions and directions for the future research.展开更多
Study on nanomaterials has attracted great interests in recent years. In this article, zirconia nanocrystallites of different structures have been successfully synthesized via hydrothermal methods with cationic surfac...Study on nanomaterials has attracted great interests in recent years. In this article, zirconia nanocrystallites of different structures have been successfully synthesized via hydrothermal methods with cationic surfactant (CTAB) and anionic surfactant (SDS), respectively. Differential Scanning Calorimeter (DSC-TG), X-ray Diffractometer (XRD), Transmission Electron Microscope (TEM), Ultraviolet-Visible (UV-vis) and N2 adsorption-desorption analyses are used for their structure characteristics. The results show that the cationic surfactant has a distinctive direction effect on the formation of zirconia nanocrystallites, while the anionic surfactant has a self-assembly synergistic effect on them. The sample synthesized with the cationic surfactant presents good dispersion with the main phase of tetragonal zirconia, and the average nanocrystal size is around 15 nm after calcination at 500 ℃. While the sample synthesized with the anionic surfactant exhibits a worm-like mesoporous structure with pure tetragonal phase after calcination at 500 ℃ and with good thermal stability.展开更多
Na-based layered iron-manganese oxide Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) containing only low-cost elements is a promising cathode for Na-ion batteries used in large-scale energy storage systems.However,the poor cycle stab...Na-based layered iron-manganese oxide Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) containing only low-cost elements is a promising cathode for Na-ion batteries used in large-scale energy storage systems.However,the poor cycle stability restricts its practical application.The capacity decay of Na_(0.67)Fe_(0.6)Mn_(0.5)O_(2) mainly originates from the irreversible anionic redox reaction charge compensation due to the high-level hybridization between oxygen and iron.Herein,we rationally design a surface Ti doping strategy to tune the anionic redox reaction activity of Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) and improve its Na-storage properties.The doped Ti ions not only enlarge the Na migration spacing layer but also improve the structure stability thanks to the strong Ti-O bond.More importantly,the d0-shell electronic structure of Ti^(4+) can suppress the charge transfer from the oxidized anions to cations,thus reducing the anionic redox reaction activity and enhancing the reversibility of charge compensation.The modified Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) cathode shows a reversible capacity of 198 mA h g^(-1) and an increased capacity retention from 15% to 73% after about1 month of cycling.Meanwhile,a superior Na-ion diffusion kinetics and rate capability are also observed.This work advances the commercialization process of Na-based layered iron-manganese oxide cathodes;on the other hand,the proposed modification strategy paves the way for the design of high-performance electrode materials relying on anionic redox reactions.展开更多
Selenium and zinc are used as anionic and cationic dopant elements to dope PbS nanostructures. The undoped and doped PbS nanostructures are grown using a thermal evaporation method. Scanning electron microscopy (SEM...Selenium and zinc are used as anionic and cationic dopant elements to dope PbS nanostructures. The undoped and doped PbS nanostructures are grown using a thermal evaporation method. Scanning electron microscopy (SEM) results show similar morphologies for the undoped and doped PbS nanostructures. X-ray diffraction (XRD) patterns of three sets of the nanostructures indicate that these nanostructures each have a PbS structure with a cubic phase. Evidence of dopant incorporation is demonstrated by X-ray photoelectron spectroscopy (XPS). Raman spectra of the synthesized samples con- firm the XRD results and indicate five Raman active modes, which relate to the PbS cubic phase for all the nanostructures. Room temperature photoluminescence (PL) and UV-Vis spectrometers are used to study optical properties of the undoped and doped PbS nanostructures. Optical characterization shows that emission and absorption peaks are in the infrared (IR) region of the electromagnetic spectrum for all PbS nanostructures. In addition, the optical studies of the doped PbS nanos- tructures reveal that the band gap of the Se-doped PbS is smaller, and the band gap of the Zn-doped PbS is bigger than the band gap of the undoped PbS nanostructures.展开更多
A noncrystallizable semiaromatic polyamide copolymer(NSAP) was dissolved in molten caprolactam, and PA6/ NSAP blends were produced in-situ via the anionic ring-opening polymerization of caprolactam. The presence of ...A noncrystallizable semiaromatic polyamide copolymer(NSAP) was dissolved in molten caprolactam, and PA6/ NSAP blends were produced in-situ via the anionic ring-opening polymerization of caprolactam. The presence of a single loss tangent(tanS) peak measured by means of dynamic mechanical analysis(DMA) proves the miscibility between PA6 and NSAP in the blends. It was found that there existed drastic changes in the crystallographic form and crystallization kinetics for the in-situ blends, e.g. , when 20% NSAP was added, nearly all crystallites existed in the ,y form and the crystallization could hardly occur upon cooling even at a rate of 2.5 ℃/min. Moreover, cold crystallization appears during the subsequent heating, and its melting point is 40 ℃ lower than that of the virgin system. On the other hand, the size of the spherulites only decreases modestly. It is suggested that the introduction of irregular stiff segments originated from NSAP into PA6 macromolecule chain, which resulted from transamidation during the polymerization play a dominant role in the drastic change of crystallization kinetics and the resultant morphology of the in-situ blends.展开更多
The use of living, alkyllithium-initiated anionic polymerization to prepare chain-end functionalized polymers and heteroarm, star-branched polymers is discussed. The scope and limitations of specific termination react...The use of living, alkyllithium-initiated anionic polymerization to prepare chain-end functionalized polymers and heteroarm, star-branched polymers is discussed. The scope and limitations of specific termination reactions with a variety of electrophilic species are illustrated for carbonation, hydroxyethylation, amination, and sulfonation. The methodology of using substituted 1,1-diphenylethylenes to provide a general, quantitative functionalization procedure is outlined and illustrated with examples of amine and phenol end-functionalization. A methodology is described for the synthesis of functionalized, star-branched copolymers with compositionally heterogeneous arms of controlled molecular weight and narrow molecular weight distribution using 1, 3-bis(1-pbenylethenyl) benzene.展开更多
Silica hollow spheres(SHSs) have attracted great attention because of their low toxicity, low density, large surface area, high chemical and thermal stability, and surface permeability. They can be widely applied in...Silica hollow spheres(SHSs) have attracted great attention because of their low toxicity, low density, large surface area, high chemical and thermal stability, and surface permeability. They can be widely applied in storage^[l], catalysis^[2], drug deli- very^[3,4], low-dielectric-constant materials^[5], low-refractive materials^[6-8], and so on. Up to now, there have been various methods to produce SHSs. Inorganic^[9] or organic particles^[10], such as polystyrene or calcium carbonate, were used as hard templates to create hollow cavities, However, the multistep synthetic process and the lack of structural robustness of the shells upon template removal process weaken their applica- tion. Soft templates, including oil-in-water emulsions^[11,12], vesicles^[13], micelle^[14,15] and gas bubbles^[16], are applied widely.展开更多
The main purpose of this research work is to improve anti-static properties of Cashmere fabric by introducing application comprising anti-static agent by foaming which was made with cationic waterborne polyurethane an...The main purpose of this research work is to improve anti-static properties of Cashmere fabric by introducing application comprising anti-static agent by foaming which was made with cationic waterborne polyurethane and graphene-CNC. Cashmere fabric was cut into 10 pieces of sample cloth of 5 cm * 5 cm size, washed with acetone solution, and then dried in an oven at 60℃. Three forms of waterborne polyurethanes such as two forms of Cationic waterborne polyurethane (CWPU) and a form of Anionic waterborne polyurethane (AWPU) were synthesized. Cellulose nanocrystalline (CNC)/graphite powder solution with the ratio of 0.5/1, 1/1, 2/1 was prepared by ultrasonic probe stripping method, and the concentration of graphite powder was ensured to be 1 mg/ml. The fabric was treated with anionic and cationic WPUs foaming solution until the weight gain reached 2.5 - 3.5 wt%. After drying, the elastic cloth was foamed with graphene solution until the graphite content of the cloth was close to 10%, 20%, 40%, 60% respectively, and then dried for reserving. Characterization properties of pure graphite powder, pure CNC and graphene solution with different proportions of three components were tested by Fourier transform infrared spectrometer (FTIR), X-ray diffraction (XRD), Thermalgravitimetric analysis (TGA) and scanning electron microscopy (SEM). Take the original cloth, only WPU treated cloth and four clothes with different graphite content for the fabric performance test.展开更多
In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al ...In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.展开更多
基金financially supported by National Natural Science Foundation of China(No.22302229)Beijing Municipal Excellent Talent Training Funds Youth Advanced Individual Project(No.2018000020124G163)。
文摘Emulsification is one of the important mechanisms of surfactant flooding. To improve oil recovery for low permeability reservoirs, a highly efficient emulsification oil flooding system consisting of anionic surfactant sodium alkyl glucosyl hydroxypropyl sulfonate(APGSHS) and zwitterionic surfactant octadecyl betaine(BS-18) is proposed. The performance of APGSHS/BS-18 mixed surfactant system was evaluated in terms of interfacial tension, emulsification capability, emulsion size and distribution, wettability alteration, temperature-resistance and salt-resistance. The emulsification speed was used to evaluate the emulsification ability of surfactant systems, and the results show that mixed surfactant systems can completely emulsify the crude oil into emulsions droplets even under low energy conditions. Meanwhile,the system exhibits good temperature and salt resistance. Finally, the best oil recovery of 25.45% is achieved for low permeability core by the mixed surfactant system with a total concentration of 0.3 wt%while the molar ratio of APGSHS:BS-18 is 4:6. The current study indicates that the anionic/zwitterionic mixed surfactant system can improve the oil flooding efficiency and is potential candidate for application in low permeability reservoirs.
基金financially supported by the National Natural Science Foundation of China(U21A20313,22222807)。
文摘For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and kinetics.In this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of solvent on the mechanism and kinetics of LAP was revealed through a strategy combining density functional theory(DFT)calculations and kinetic modeling.In terms of mechanism,it is found that the stronger the solvent polarity,the more electrons transfer from initiator to solvent through detailed energy decomposition analysis of electrostatic interactions between initiator and solvent molecules.Furthermore,we also found that the stronger the solvent polarity,the higher the monomer initiation energy barrier and the smaller the initiation rate coefficient.Counterintuitively,initiation is more favorable at lower temperatures based on the calculated results ofΔG_(TS).Finally,the kinetic characteristics in different solvents were further examined by kinetic modeling.It is found that in benzene and n-pentane,the polymerization rate exhibits first-order kinetics.While,slow initiation and fast propagation were observed in tetrahydrofuran(THF)due to the slow free ion formation rate,leading to a deviation from first-order kinetics.
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (2021R1A2C1014280)supported by the “Regional Innovation Strategy (RIS)” through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (MOE) (2021RIS-004)+1 种基金the Fundamental Research Program of the Korea Institute of Material Science (KIMS) (PNK9370)the calculation resources were supported by the Supercomputing Center in Korea Institute of Science and Technology Information (KISTI) (KSC-2022-CRE-0030)。
文摘The anionic redox has been widely studied in layered-oxide-cathodes in attempts to achieve highenergy-density for Na-ion batteries(NIBs).It is known that an oxidation state of Mn^(4+) or Ru^(5+) is essential for the anionic reaction of O^(2-)/O~-to occur during Na^(+) de/intercalation.However,here,we report that the anionic redox can occur in Ru-based layered-oxide-cathodes before full oxidation of Ru^(4+)/Ru^(5+).Combining studies using first-principles calculation and experimental techniques reveals that further Na^(+) deintercalation from P2-Na_(0.33)[Mg_(0.33)Ru_(0.67)]O_(2) is based on anionic oxidation after 0.33 mol Na^(+) deintercalation from P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) with cationic oxidation of Ru^(4+)/Ru^(4.5+).Especially,it is revealed that the only oxygen neighboring 2Mg/1 Ru can participate in the anionic redox during Na^(+) de/intercalation,which implies that the Na-O-Mg arrangement in the P2-Na_(0.33)[M9_(0.33)Ru_(0.67)]O_(2) structure can dramatically lower the thermodynamic stability of the anionic redox than that of cationic redox.Through the O anionic and Ru cationic reaction,P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) exhibits not only a large specific capacity of~172 mA h g^(-1) but also excellent power-capability via facile Na^(+) diffusion and reversible structural change during charge/discharge.These findings suggest a novel strategy that can increase the activity of anionic redox by modulating the local environment around oxygen to develop high-energy-density cathode materials for NIBs.
基金financially supported by the Scientific Research Startup Funds from Tsinghua Shenzhen International Graduate School。
文摘The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy.In this context,metal-organic frameworks(MOFs),with their unique 3D porous structure and tunable chemical functionality,have shown enormous potential as energy storage materials for accommodating or transporting electrochemically active ions.In this perspective,we specifically focus on the current status and prospects of anionic MOF-based quasi-solid-state-electrolytes(anionic MOF-QSSEs)for lithium metal batteries(LMBs).An overview of the definition,design,and properties of anionic MOF-QSSEs is provided,including recent advances in the understanding of their ion transport mechanism.To illustrate the advantages of using anionic MOF-QSSEs as electrolytes for LMBs,a thorough comparison between anionic MOF-QSSEs and other well-studied electrolyte systems is made.With these in-depth understandings,viable techniques for tuning the chemical and topological properties of anionic MOF-QSSEs to increase Li+conductivity are discussed.Beyond modulation of the MOFs matrix,we envisage that solvent and solid-electrolyte interphase design as well as emerging fabrication techniques will aid in the design and practical application of anionic MOF-QSSEs.
文摘A new electrophilic polymer, 2,4-dinitrophenyl ether of polyvinyl alcohol (PVA-DNP), having a degree of substitution of 0.5 was prepared from polyvinyl alcohol (PVA) and 1-fluro-2,4-dinitrobenzene (DNFB). The PVA-DNP polymer was characterized by NMR, IR, and UV-visible spectroscopy. The reaction of PVA-DNP with sodium methoxide was followed by NMR and UV-visible spectroscopy. Evidence of polymer bound spirocyclic SIGMA complex, C-1 and C-3 polymer bound DNP-methoxy SIGMA complexes and the formation and C-1 methoxy complex of 2,4-dinitroanisole was observed.
基金Project supported by the Key Science Project of Environmental Protection Foundation of Shandong Government(No.(2006)005).
文摘In order to reduce the impact of eutrophication caused by agricultural residues (i.e., excess nitrate) in aqueous solution, economic and effective anionic sorbents are required. In this article, we prepared anionic sorbent using wheat straw. Its structural characteristics and adsorption properties for nitrate removal from aqueous solution were investigated. The results indicate that the yield of the prepared anionic sorbent, the total exchange capacity, and the maximum adsorption capacity were 350%, 2.57 mEq/g, and 2.08 mmol/g, respectively. The Freundlich isotherm mode is more suitable than the Langmuir mode and the adsorption process accords with the first order reaction kinetic rate equation. When multiple anions (SO4^2-, H2PO4^-, NO3^-, and NO2^-) were present, the isotherm mode of prepared anionic sorbent for nitrate was consistent with Freundlich mode; however, the capacity of nitrate adsorption was reduced by 50%. In alkaline solutions, about 90% of adsorbed nitrate ions could be desorbed from prepared anionic sorbent. The results of this study confirmed that the wheat straw anionic sorbent can be used as an excellent nitrate sorbent that removes nitrate from aqueous solutions.
基金Funded by National Natural Science Foundation of China(No.51262028)Fundamental Research Funds for the Gansu UniversitiesYoung Teacher Research Foundation of Northwest Normal University(No.NWNU-LKQN-11-17)
文摘Polyaniline(PANI) was one of the most extensively studied adsorbents due to its low cost and good environmental stability. The objective of the current study was to improve the selective capabilities of PANI for anionic dyes. We found that the acid doped PANI prepared with hydrochloric acid and p-toluenesulfonic acid(PTSA) could selectively adsorb anionic dyes. It exhibited very good selectivity for OG dye, the mechanism was proposed based on the chemical interaction of PANI with the sulfonate group of the dyes. The effects of solution p H, initial dye concentration, and different HCl/PTSA mole ratios on the adsorption capacity of OG have been investigated. Kinetic simulations indicated that the adsorption process could be well represented by pseudo-second-order kinetic plots. The isothermal adsorption curve fitting also showed that the adsorption process could be well described by the Langmuir isothermal equation. The results showed that acid doped PANI could be employed as a promising adsorbent for anion removal from dye wastewater.
基金Supported by the Open Fund Project innovation platform of Key Laboratory of Higher Educational Institutions of Hunan Province(GN16K01)Scientific&Technological Projects of Hengyang(2016KL03)+1 种基金Aid programs for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Provincethe Key Discipline of Hunan Province,Project funding for research and innovation experiment of university students in Hunan Province
文摘A novel anionic organotin(Ⅳ) complex {[(pClCHCH)Sn(HO)(Cl)OCOCH(O)CH(O)COSn(HO)(Cl)(p-ClCHCH)]·2(HNEt)}(1) was synthesized by the reaction of di(p-chlorobenzy)tin dichloride with the D-tartaric acid in 2:1 molar in the presence of an organic base triethylamine. The structure was characterized by elemental analysis, IR, TG, XRD and single-crystal X-ray diffraction. It crystallizes in triclinic, P1 space group, with a = 0.7067(1), b = 1.9762(3), c = 2.2383(3) nm, α = 91.544(2)°, β = 90.075(2)°, γ = 90.110(2)°, V = 3.1247(7) nm~3, Z = 3, Dc = 1.621 g/cm~3, m(Mo Kα) = 16.29 cm–1, F(000) = 1530, R = 0.0394, wR = 0.1092,(Δρ)max = 1224 and(Δρ)min = –840 e/nm~3. The stabilities, orbital energies and composition characteristics of some frontier molecular orbitals of 1 have been carefully investigated with quantum chemistry calculation. In addition, the in vitro antitumor activity suggested that 1 had stronger inhibitory activity on H460, MCF7 than on A549.
文摘The objective of this study is to develop chitosaneanionic polymers based extendedrelease tablets and test the feasibility of using this system for the sustained release of highly water-soluble drugs with high drug loading.Here,the combination of sodium valproate(VPS)and valproic acid(VPA)were chosen as the model drugs.Anionic polymers studied include xanthan gum(XG),carrageenan(CG),sodium carboxymethyl cellulose(CMC-Na)and sodium alginate(SA).The tablets were prepared by wet granulation method.In vitro drug release was carried out under simulated gastrointestinal condition.Drug release mechanism was studied.Compared with single polymers,chitosaneanionic polymers based system caused a further slowdown of drug release rate.Among them,CS exanthan gum matrix system exhibited the best extended-release behavior and could extend drug release for up to 24 h.Differential scanning calorimetry(DSC)and Fourier transform infrared spectroscopy(FTIR)studies demonstrated that polyelectrolyte complexes(PECs)were formed on the tablet surface,which played an important role on retarding erosion and swelling of the matrix in the later stage.In conclusion,this study demonstrated that it is possible to develop highly water-soluble drugs loaded extendedrelease tablets using chitosaneanionic polymers based system.
基金supported by the National Natural Science Foundation of China(Grant no.52072411,51932011,51972346)。
文摘With the merit of high capacity,high safety,and low cost,zinc-ion batteries(ZIBs)possess huge application potential in the domain of large-scale energy storage.However,due to the relatively narrow voltage window and large lattice distortion of cationic redox reaction,ZIBs tend to present low energy density,poor kinetics,and unstable cyclic performance.Anion chemistry seems to provide a novel strategy to solve these issues from different aspects,such as enhanced operating voltage,extra capacity contribution,and boosted reaction kinetics.Considering the significance of this theory and the lack of relevant literatures,herein,in-depth comprehension of anionic chemistry and its positive effects on zinc storage performance have been emphasized and summarized.This review aims to present a full scope of anionic chemistry and furnish systematic cognition for rational design of advanced ZIBs with high energy density.Furthermore,insightful analysis and perspectives based on the current research status also have been proposed,which may point out some scientific suggestions and directions for the future research.
基金Funded by High and New-Technology Project from Science and Technology Department of Fujian Province (No. 2004H008)
文摘Study on nanomaterials has attracted great interests in recent years. In this article, zirconia nanocrystallites of different structures have been successfully synthesized via hydrothermal methods with cationic surfactant (CTAB) and anionic surfactant (SDS), respectively. Differential Scanning Calorimeter (DSC-TG), X-ray Diffractometer (XRD), Transmission Electron Microscope (TEM), Ultraviolet-Visible (UV-vis) and N2 adsorption-desorption analyses are used for their structure characteristics. The results show that the cationic surfactant has a distinctive direction effect on the formation of zirconia nanocrystallites, while the anionic surfactant has a self-assembly synergistic effect on them. The sample synthesized with the cationic surfactant presents good dispersion with the main phase of tetragonal zirconia, and the average nanocrystal size is around 15 nm after calcination at 500 ℃. While the sample synthesized with the anionic surfactant exhibits a worm-like mesoporous structure with pure tetragonal phase after calcination at 500 ℃ and with good thermal stability.
基金supported by the National Natural Science Foundation of China (Grant No. 12105197)the Science Center of the National Science Foundation of China (Grant No. 52088101)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Scientific Instrument Developing Project of the Chinese Academy of Sciences (Grant ZDKYYQ20170001)。
文摘Na-based layered iron-manganese oxide Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) containing only low-cost elements is a promising cathode for Na-ion batteries used in large-scale energy storage systems.However,the poor cycle stability restricts its practical application.The capacity decay of Na_(0.67)Fe_(0.6)Mn_(0.5)O_(2) mainly originates from the irreversible anionic redox reaction charge compensation due to the high-level hybridization between oxygen and iron.Herein,we rationally design a surface Ti doping strategy to tune the anionic redox reaction activity of Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) and improve its Na-storage properties.The doped Ti ions not only enlarge the Na migration spacing layer but also improve the structure stability thanks to the strong Ti-O bond.More importantly,the d0-shell electronic structure of Ti^(4+) can suppress the charge transfer from the oxidized anions to cations,thus reducing the anionic redox reaction activity and enhancing the reversibility of charge compensation.The modified Na_(0.67)Fe_(0.5)Mn_(0.5)O_(2) cathode shows a reversible capacity of 198 mA h g^(-1) and an increased capacity retention from 15% to 73% after about1 month of cycling.Meanwhile,a superior Na-ion diffusion kinetics and rate capability are also observed.This work advances the commercialization process of Na-based layered iron-manganese oxide cathodes;on the other hand,the proposed modification strategy paves the way for the design of high-performance electrode materials relying on anionic redox reactions.
基金the Iranian National Science Foundation (INSF) for a research grant support the Islamic Azad University(I.A.U.), Masjed-Soleiman and Ahwaz Branches, respectively, for their financial support of this research workthe financial support from the Ministry of Higher Education of Malaysia for the High Impact Research Grant (UM.C/1/HIR/MOHE/SC/21)
文摘Selenium and zinc are used as anionic and cationic dopant elements to dope PbS nanostructures. The undoped and doped PbS nanostructures are grown using a thermal evaporation method. Scanning electron microscopy (SEM) results show similar morphologies for the undoped and doped PbS nanostructures. X-ray diffraction (XRD) patterns of three sets of the nanostructures indicate that these nanostructures each have a PbS structure with a cubic phase. Evidence of dopant incorporation is demonstrated by X-ray photoelectron spectroscopy (XPS). Raman spectra of the synthesized samples con- firm the XRD results and indicate five Raman active modes, which relate to the PbS cubic phase for all the nanostructures. Room temperature photoluminescence (PL) and UV-Vis spectrometers are used to study optical properties of the undoped and doped PbS nanostructures. Optical characterization shows that emission and absorption peaks are in the infrared (IR) region of the electromagnetic spectrum for all PbS nanostructures. In addition, the optical studies of the doped PbS nanos- tructures reveal that the band gap of the Se-doped PbS is smaller, and the band gap of the Zn-doped PbS is bigger than the band gap of the undoped PbS nanostructures.
基金Supported by the National Natural Science Foundation of China(No50373037)
文摘A noncrystallizable semiaromatic polyamide copolymer(NSAP) was dissolved in molten caprolactam, and PA6/ NSAP blends were produced in-situ via the anionic ring-opening polymerization of caprolactam. The presence of a single loss tangent(tanS) peak measured by means of dynamic mechanical analysis(DMA) proves the miscibility between PA6 and NSAP in the blends. It was found that there existed drastic changes in the crystallographic form and crystallization kinetics for the in-situ blends, e.g. , when 20% NSAP was added, nearly all crystallites existed in the ,y form and the crystallization could hardly occur upon cooling even at a rate of 2.5 ℃/min. Moreover, cold crystallization appears during the subsequent heating, and its melting point is 40 ℃ lower than that of the virgin system. On the other hand, the size of the spherulites only decreases modestly. It is suggested that the introduction of irregular stiff segments originated from NSAP into PA6 macromolecule chain, which resulted from transamidation during the polymerization play a dominant role in the drastic change of crystallization kinetics and the resultant morphology of the in-situ blends.
文摘The use of living, alkyllithium-initiated anionic polymerization to prepare chain-end functionalized polymers and heteroarm, star-branched polymers is discussed. The scope and limitations of specific termination reactions with a variety of electrophilic species are illustrated for carbonation, hydroxyethylation, amination, and sulfonation. The methodology of using substituted 1,1-diphenylethylenes to provide a general, quantitative functionalization procedure is outlined and illustrated with examples of amine and phenol end-functionalization. A methodology is described for the synthesis of functionalized, star-branched copolymers with compositionally heterogeneous arms of controlled molecular weight and narrow molecular weight distribution using 1, 3-bis(1-pbenylethenyl) benzene.
基金Supported by the National Natural Science Foundation of China(No.20890121)the National Basic Research Program of China(No.2009CB930403)
文摘Silica hollow spheres(SHSs) have attracted great attention because of their low toxicity, low density, large surface area, high chemical and thermal stability, and surface permeability. They can be widely applied in storage^[l], catalysis^[2], drug deli- very^[3,4], low-dielectric-constant materials^[5], low-refractive materials^[6-8], and so on. Up to now, there have been various methods to produce SHSs. Inorganic^[9] or organic particles^[10], such as polystyrene or calcium carbonate, were used as hard templates to create hollow cavities, However, the multistep synthetic process and the lack of structural robustness of the shells upon template removal process weaken their applica- tion. Soft templates, including oil-in-water emulsions^[11,12], vesicles^[13], micelle^[14,15] and gas bubbles^[16], are applied widely.
文摘The main purpose of this research work is to improve anti-static properties of Cashmere fabric by introducing application comprising anti-static agent by foaming which was made with cationic waterborne polyurethane and graphene-CNC. Cashmere fabric was cut into 10 pieces of sample cloth of 5 cm * 5 cm size, washed with acetone solution, and then dried in an oven at 60℃. Three forms of waterborne polyurethanes such as two forms of Cationic waterborne polyurethane (CWPU) and a form of Anionic waterborne polyurethane (AWPU) were synthesized. Cellulose nanocrystalline (CNC)/graphite powder solution with the ratio of 0.5/1, 1/1, 2/1 was prepared by ultrasonic probe stripping method, and the concentration of graphite powder was ensured to be 1 mg/ml. The fabric was treated with anionic and cationic WPUs foaming solution until the weight gain reached 2.5 - 3.5 wt%. After drying, the elastic cloth was foamed with graphene solution until the graphite content of the cloth was close to 10%, 20%, 40%, 60% respectively, and then dried for reserving. Characterization properties of pure graphite powder, pure CNC and graphene solution with different proportions of three components were tested by Fourier transform infrared spectrometer (FTIR), X-ray diffraction (XRD), Thermalgravitimetric analysis (TGA) and scanning electron microscopy (SEM). Take the original cloth, only WPU treated cloth and four clothes with different graphite content for the fabric performance test.
基金supported by the National Key R&D Program of China(No.2017YFB0602702-02)。
文摘In this work,a facile and effective strategy to prepare three-dimensional(3D)hierarchical flower-like Mg–Al layered double hydroxides(3D-LDH)was developed via a one-step double-drop coprecipitation method usingγ-Al 2O 3particles as a template.The characterization and experimental results showed that the calcined product,3D-LDO,features a large specific surface area of 204.2 m^(2)/g,abundant active sites,and excellent adsorption performance for Congo red(CR),methyl orange(MO),and methyl blue(MB).The maximum adsorption capacities of 3D-LDO for CR,MO,and MB were 1428.6,476.2,and 1666.7 mg/g,respectively;such performance is superior to that of most reported adsorbents.The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption,the memory effect of 3D-LDO,and the unique 3D hierarchical flower-like structure of the adsorbent.Recycling performance tests revealed that3D-LDO has satisfactory reusability for the three organic anionic dyes.