Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy...Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.展开更多
The surface charge accumulation on polymers often leads to surface flashover.Current solutions are mainly based on the introduction of inorganic fillers.The high-cost process and low compatibility remain formidable ch...The surface charge accumulation on polymers often leads to surface flashover.Current solutions are mainly based on the introduction of inorganic fillers.The high-cost process and low compatibility remain formidable challenges.Moreover,existing researches on all-organic insulation focus on capturing electrons,contrary to alleviating charge accumulation.Here,an all-organic modification coating was prepared on polystyrene(PS)with the large-scale atmospheric-pressure plasma,which exhibits outperformed function in mitigating surface charge accumulation.The surface charge dissipation rate and surface conductivity are promoted by about 1.37 and 9.45 times,respectively.Simulation and experimental results show that this all-organic modification coating has a smaller electron affinity potential compared with PS.The decrease of electron affinity potential may result in accelerated surface charge decay of PS,which has never been involved in previous works.Moreover,this coating also has good reliability in a repeated surface flashover.This facile and large-scale approach brings up a novel idea for surface charge regulation and the manufacture of advanced dielectric polymers.展开更多
Speciation and fractionation of heavy metals in soil subsamples experimentally loaded with Pb, Cd, Cu and Zn in orthogonal design was investigated by sequential extraction, and operationally defined as water soluble ...Speciation and fractionation of heavy metals in soil subsamples experimentally loaded with Pb, Cd, Cu and Zn in orthogonal design was investigated by sequential extraction, and operationally defined as water soluble and exchangeable(SE), weakly specific adsorbed(WSA), Fe and Mn oxides bound(OX) and organic bound(ORG). The results showed that fractions of heavy metals in the soil subsamples depended on their speciation. About 90% of Cd and 75% of Zn existed in soil subsamples in the SE fraction. Lead and Cu existed in soil subsamples as SE, WSA and OX fractions simultaneously, although SE was still the major fraction. Organic bound heavy metals were not clearly apparent in all the soil subsamples. The concentration of some heavy metal fractions in soil subsamples showed the good correlation with ionic impulsion of soil, especially for the SE fraction. Continuous saturation of soil subsamples with 0.20 mol/L NH 4Cl, which is the first step for determination of the negative surface charge of soil by the ion retention method, resulted in desorption of certain heavy metals from the soil. It was found that the percentage desorption of heavy metals from soil subsamples depended greatly on pH, the composition and original heavy metal content of the soil subsamples. However, most of the heavy metals in the soil subsamples were still be retained after multiple saturation. Compared with the parent soil, the negative surface charge of soil subsamples loaded with heavy metals did not show difference significantly from that of the parent one by statistical analysis. Heavy metals existed in the soil subsamples mainly as exchangeable and precipitated simultaneously.展开更多
Surface charges greatly affect the discharge/flashover development process across an insulator. The relationship between surface charge distribution on insulating materials and measurement data based on Pockels techni...Surface charges greatly affect the discharge/flashover development process across an insulator. The relationship between surface charge distribution on insulating materials and measurement data based on Pockels technique is discussed, and an improved algorithm is built to calculate the real surface charge density from original data. In this algorithm, two-dimensional Fourier transform technique and Wiener filter are employed to reduce the amount of numerical calculation and improve the stability of computation, Moreover, this algorithm considers not only the influence of sample's thickness and permittivity, but also the impact of charges at different positions. The achievement of this calibration algorithm is demonstrated in details. Compared with traditional algorithms, the improved one supplies a better solution in the calibration of surface charge distribution on different samples with different thickness.展开更多
The ion flow field on the ground is one of the significant parameters used to evaluate the electromagnetic environment of high voltage direct current(HVDC) power lines.HVDC lines may cross the greenhouses due to the...The ion flow field on the ground is one of the significant parameters used to evaluate the electromagnetic environment of high voltage direct current(HVDC) power lines.HVDC lines may cross the greenhouses due to the restricted transmission corridors.Under the condition of ion flow field,the dielectric films on the greenhouses will be charged,and the electric fields in the greenhouses may exceed the limit value.Field mills are widely used to measure the groundlevel direct current electric fields under the HVDC power lines.In this paper,the charge inversion method is applied to calculate the surface charges on the dielectric film according to the measured ground-level electric fields.The advantages of hiding the field mill probes in the ground are studied.The charge inversion algorithm is optimized in order to decrease the impact of measurement errors.Based on the experimental results,the surface charge distribution on a piece of quadrate dielectric film under a HVDC corona wire is studied.The enhanced effect of dielectric film on ground-level electric field is obviously weakened with the increase of film height.Compared with the total electric field strengths,the normal components of film-free electric fields at the corresponding film-placed positions have a higher effect on surface charge accumulation.展开更多
Surface charges and hydration are predominant properties of colloidal particles that govern colloidal stability in aqueous suspensions.These properties usually coexist and interact with each other.The correlation betw...Surface charges and hydration are predominant properties of colloidal particles that govern colloidal stability in aqueous suspensions.These properties usually coexist and interact with each other.The correlation between the surface charge and hydration of minerals is summarized on the basis of innovative experimental,theoretical,and molecular dynamics simulation studies.The factors affecting the adsorption behavior of ions and water molecules,such as ion concentration,ion hydration radius and valence,and surface properties,are discussed.For example,the hydration and adsorption states completely differ between monovalent and divalent ions.For ions of the same valence,the effect of surface charge on the hydration force follows the Hofmeister adsorption series.Electrolyte concentration exerts a significant effect on the hydration force at high ion concentrations.Meanwhile,the ion correlations in high-concentration electrolyte systems become long range.The interfacial water structure largely depends on surface chemistry.The hydration layer between different surfaces shows large qualitative differences.展开更多
Biodegradable polymeric materials are the most common carriers for use in drug delivery systems. With this trend, newer drug delivery systems using targeted and controlled release polymeric nanoparticles (NPs) are bei...Biodegradable polymeric materials are the most common carriers for use in drug delivery systems. With this trend, newer drug delivery systems using targeted and controlled release polymeric nanoparticles (NPs) are being developed to manipulate their navigation in complex in vivo environment. However, a clear understanding of the interactions between biological systems and these nanoparticulates is still unexplored. Different studies have been performed to correlate the physicochemical properties of polymeric NPs with the biological responses. Size and surface charge are the two fundamental physicochemical properties that provide a key direction to design an effective NP formulation. In this critical review, our goal is to provide a brief overview on the influences of size and surface charge of different polymeric NPs in vitro and to highlight the challenges involved with in vivo trials.展开更多
Pathological effects of asbestos are probably dependent on the special surface properties of the fibers, such as surface charge, surface metal ions. The present study was designed to determine whether the pretreatment...Pathological effects of asbestos are probably dependent on the special surface properties of the fibers, such as surface charge, surface metal ions. The present study was designed to determine whether the pretreatment of chrysotile asbestos fibers (CAF) with rare earth compounds (REC) solution can reduce their pathogenicity. The results showed that REC-pretreated CAF induced less nitrogen oxide (NO) production by alveolar macrophages (AM). In addition, the pretreatment lowered the capacity of hemolysis and the methylene blue (MB) adsorption of the native CAF. These findings suggested that the pretreatment of CAF with REC solution reduced the in vitro toxicity of CAF by lessening its surface charges. Nevertheless, the pathogenicity and the carcinogenicity of REC-pretreated CAF in vivo remain to be investigated.展开更多
We present the variations of electrical parameters of dielectric barrier discharge(DBD)when the DBD generator is used for the material modification,whereas the relevant physical mechanism is also elaborated.An equival...We present the variations of electrical parameters of dielectric barrier discharge(DBD)when the DBD generator is used for the material modification,whereas the relevant physical mechanism is also elaborated.An equivalent circuit model is applied for a DBD generator working in a filament discharging mode,considering the addition of epoxy resin(EP)as the plasma modified material.The electrical parameters are calculated through the circuit model.The surface conductivity,surface potential decay,trap distributions and surface charge distributions on the EP surface before and after plasma treatments were measured and calculated.It is found that the coverage area of micro-discharge channels on the EP surface is increased with the discharging time under the same applied AC voltage.The results indicate that the plasma modified material could influence the ignition of new filaments in return during the modification process.Moreover,the surface conductivity and density of shallow traps with low trap energy of the EP samples increase after the plasma treatment.The surface charge distributions indicate that the improved surface properties accelerate the movement and redistribution of charge carriers on the EP surface.The variable electrical parameters of discharge are attributed to the redistribution of deposited surface charge on the plasma modified EP sample surface.展开更多
A surface charge measuring system using the capacitive probe method is analysed. The present study shows that the measuring system cannot have a steady-state output and that the error resulting from the finite leakage...A surface charge measuring system using the capacitive probe method is analysed. The present study shows that the measuring system cannot have a steady-state output and that the error resulting from the finite leakage resistance of the measuring system will be accumulated during the measuring process. Based on the theoretical analysis a new type probe with a low charge leakage and high resolution is designed. The surface charge accumulated on the Teflon insulator under a DC voltage is measured using this new probe and some phenomena of the surface charging are reported.展开更多
The solar-driven reduction of CO_(2) into valuable products is a promising method to alleviate global environmental problems and energy crises.However,the low surface charge density limits the photocatalytic conversio...The solar-driven reduction of CO_(2) into valuable products is a promising method to alleviate global environmental problems and energy crises.However,the low surface charge density limits the photocatalytic conversion performance of CO_(2).Herein,a polymeric carbon nitride(PCN)photocatalyst with Zn single atoms(Zn1/CN)was designed and synthesized for CO_(2) photoreduction.The results of the CO_(2) photoreduction studies show that the CO and CH_(4) yields of Zn1/CN increased fivefold,reaching 76.9 and 22.9μmol/(g·h),respectively,in contrast to the unmodified PCN.Ar+plasma-etched X-ray photoelectron spectroscopy and synchrotron radiation-based X-ray absorption fine structure results reveal that Zn single atom is mainly present in the interlayer space of PCN in the Zn–N_(4) configuration.Photoelectrochemical characterizations indicate that the interlayer Zn–N_(4) configuration can amplify light absorption and establish an interlayer charge transfer channel.Light-assisted Kelvin probe force microscopy confirms that more photogenerated electrons are delivered to the catalyst surface through interlayer Zn–N_(4) configuration,which increases its surface charge density.Further,in-situ infrared spectroscopy combined with density functional theory calculation reveals that promoted surface charge density accelerates key intermediates(*COOH)conversion,thus achieving efficient CO_(2) conversion.This work elucidates the role of internal single atoms in catalytic surface reactions,which provides important implications for the design of single-atom catalysts.展开更多
Surface charge accumulation is considered to be a critical factor in flashover failure of three-post insulators.However,surface charge accumulation characteristics on threepost insulators with complex structures and u...Surface charge accumulation is considered to be a critical factor in flashover failure of three-post insulators.However,surface charge accumulation characteristics on threepost insulators with complex structures and uneven electric fields are still unclear.Furthermore,the temperature gradient field makes charge accumulation more complicated.In this presentation,surface charge profiles of DC three-post insulators under electro-thermal coupling stress are studied by establishing a multi-degree-of-freedom movement measurement system.The abdominal area of the three-post insulator accumulaftes charges of identical polarity as the DC voltage,while the leg area accumulates heteropolar charges.Charge density from the bottom of the leg to the center of the abdomen presents a trimodal distribution pattern,including two homopolar charge peaks and one heteropolar charge peak.Asymmetrical surface conductance distribution arising from the temperature gradient leads to a significant increase in amplitude and distribution range of the homopolar charge peak at the legs of insulator.Increase of the temperature gradient will further magnify the homopolar charge peak at the legs.When DC voltage is 100 kV and conductive pole temperature is 70℃,surface charge density of the three-post insulator can reach 100μC/m^(2).Therefore,surface conductance regulation of the leg region is the key to charge regulation and insulation optimization design of DC three-post insulators.展开更多
Surface charge transfer doping of graphene plays an important role in graphene-based electronics due to its simplicity,high doping efficiency,and easy-controllability.Here,we demonstrate the effective surface charge t...Surface charge transfer doping of graphene plays an important role in graphene-based electronics due to its simplicity,high doping efficiency,and easy-controllability.Here,we demonstrate the effective surface charge transfer hole doping of graphene by using a strong p-type molecular dopant hexacyanotrimethylene-cyclopropane (CN6-CP).The CN6-CP exhibits a very high intrinsic work function of 6.37 e V,which facilitates remarkable electron transfer from graphene to CN6-CP as revealed by in situ photoelectron spectroscopy investigations.Consequently,hole accumulation appears in the graphene layer at the direct contact with CN6-CP.As evidenced by Hall effect measurements,the areal hole density of graphene significantly increased from 8.3×10^(12)cm^(-2) to 2.21×10^(13)cm^(-2) upon 6 nm CN6-CP evaporation.The CN6-CP acceptor with strong p-doping effect has great implications for both graphene-based and organic electronics.展开更多
In an insulating system including solid and gas dielectrics, discharge type has a strong impact on charge accumulation at the interface between two dielectrics, and hence charge decay. In order to clarify the influenc...In an insulating system including solid and gas dielectrics, discharge type has a strong impact on charge accumulation at the interface between two dielectrics, and hence charge decay. In order to clarify the influence, a surface charge measurement system was constructed, and three types of discharge, i.e. surface discharge, and low intensity and high intensity coronas, were introduced to cause surface charge accumulation. The decay behavior of surface charges after different types of discharge was obtained at various temperatures. It was found that total surface charges monotonically decreased with time, and the decay rate became larger as temperature increased. However, after a surface discharge or a high intensity corona, surface charge density in the local area appeared to fluctuate during the decay process. Compared with this, the fluctuation of surface charge density was not observed after a low intensity corona. The mechanisms of surface charge accumulation and decay were analysed. Moreover, a microscopic physical model involving charge production, accumulation, and decay was proposed so that the experimental results could be explained.展开更多
Doping of semiconductors,i.e.,accurately modulating the charge carrier type and concentration in a controllable manner,is a key technology foundation for modern electronics and optoelectronics.However,the conventional...Doping of semiconductors,i.e.,accurately modulating the charge carrier type and concentration in a controllable manner,is a key technology foundation for modern electronics and optoelectronics.However,the conventional doping technologies widely utilized in silicon industry,such as ion implantation and thermal diffusion,always fail when applied to two-dimensional(2D)materials with atomically-thin nature.Surface charge transfer doping(SCTD)is emerging as an effective and non-destructive doping technique to provide reliable doping capability for 2D materials,in particular 2D semiconductors.Herein,we summarize the recent advances and developments on the SCTD of 2D semiconductors and its application in electronic and optoelectronic devices.The underlying mechanism of STCD processes on 2D semiconductors is briefly introduced.Its impact on tuning the fundamental properties of various 2D systems is highlighted.We particularly emphasize on the SCTD-enabled high-performance 2D functional devices.Finally,the challenges and opportunities for the future development of SCTD are discussed.展开更多
The use of microparticles(MPs) as adjuvants has attracted increasing interest in vaccine delivery systems.Many physiochemical characteristics of MPs including hydrodynamic size,surface properties,and morphology can ...The use of microparticles(MPs) as adjuvants has attracted increasing interest in vaccine delivery systems.Many physiochemical characteristics of MPs including hydrodynamic size,surface properties,and morphology can regulate the immune response.Surface charge is an important characteristic of MPs,but how it affects their adjuvanticity remains unknown.In this study,we prepared uniform-sized polylactide MPs coated with various polymers of different positive charge,and investigated how the surface charge affected antigen loading and macrophage phagocytosis and activation in vitro.A higher surface charge greatly enhanced antigen loading and antigen internalization into macrophages,promoted the expression of MHC 11 and CD80,and increased the secretion level of TNF-a.Taken together,these results indicated that surface charge was an important parameter for improving the adjuvanticity of MPs.展开更多
Surface charge transfer doping has been widely utilized to tune the electronic and optical properties of semiconductor photodetectors based on low-dimensional materials.Although many studies have been conducted on the...Surface charge transfer doping has been widely utilized to tune the electronic and optical properties of semiconductor photodetectors based on low-dimensional materials.Although many studies have been conducted on the performance(response time,responsivity,etc.)of doped photodetectors and their mechanisms,they merely examined a specific thickness and did not systematically explore the dependence of doping effects on the number of layers.This work performs a series of investigations on ReS_(2)photodetectors with different numbers of layers and demonstrates that the p-dopant tetrafluorotetracyanoquinodimethane(F_(4)-TCNQ)converts the deep trap states into recombination centers for few-layer ReS_(2)and induces a vertical p-n junction for thicker ReS_(2).A response time of 200 ms is observed in the decorated 2-layer ReS_(2)photodetector,more than two orders of magnitude faster than the response of the pristine photodetector,due to the disappearance of deep trap states.A current rectification ratio of 30 in the F_(4)-TCNQ-decorated sandwiched ReS_(2)device demonstrates the formation of a vertical p-n junction in a thicker ReS_(2)device.The responsivity is as high as 2,000 A/W owing to the strong carrier separation of the p-n junction.Different thicknesses of ReS_(2)enable switching of the prominent operating mechanism between transforming deep trap states into recombination centers and forming a vertical p-n junction.The thicknessdependent doping effect of a two-dimensional material serves as a new mechanism and provides a scheme toward improving the performance of other semiconductor devices,especially optical and electronic devices based on low-dimensional materials.展开更多
This work focuses on the interaction between polymeric micelles with different charged surfaces and cancer cells in order to study the influence of surface charge on the in vitro cellular uptake efficiency. The amphip...This work focuses on the interaction between polymeric micelles with different charged surfaces and cancer cells in order to study the influence of surface charge on the in vitro cellular uptake efficiency. The amphiphilic diblock copolymers poly(e-caprolaetone)-b-poly(ethylene oxide) (PCL-b-PEO) with different functional groups at the end of hydrophilic block were synthesized. The functional groups endue the micelles with different charges on the surfaces. The cellular uptake of micelles to T-24 cells (human bladder tumor cells), HepG2 cells (human liver hepatocellular carcinoma cell line) and Hela cells (human epithelial cervical cancer cells) was studied by means of flow cytometer and confbcal laser scanning microscopy. The results indicate that the surface charges showed great influence on zeta potential of micelles at different pH values. The in vitro cellular uptake efficiency of micelles with different charged surfaces demonstrated different cellular uptake patterns to three kinds of cancer cells.展开更多
The transport behavior of pressure-driven aqueous electrolyte solution through charged carbon nanotubes(CNTs) is studied by using molecular dynamics simulations. The results reveal that the presence of charges around ...The transport behavior of pressure-driven aqueous electrolyte solution through charged carbon nanotubes(CNTs) is studied by using molecular dynamics simulations. The results reveal that the presence of charges around the nanotube can remarkably reduce the flow velocity as well as the slip length of the aqueous solution, and the decreasing of magnitude depends on the number of surface charges and distribution. With 1-M KCl solution inside the carbon nanotube, the slip length decreases from 110 nm to only 14 nm when the number of surface charges increases from 0 to 12 e. This phenomenon is attributed to the increase of the solid–liquid friction force due to the electrostatic interaction between the charges and the electrolyte particles, which can impede the transports of water molecules and electrolyte ions. With the simulation results,we estimate the energy conversion efficiency of nanofluidic battery based on CNTs, and find that the highest efficiency is only around 30% but not 60% as expected in previous work.展开更多
Nanopartide (NP) drug delivery systems have been successfully designed and implemented to orally deliver small interfering RNAs (siRNAs) for inflammatory disorders. However, the influence of surface charge on oral...Nanopartide (NP) drug delivery systems have been successfully designed and implemented to orally deliver small interfering RNAs (siRNAs) for inflammatory disorders. However, the influence of surface charge on orally administered siRNA nanocarriers has not been investigated. In this study, we prepared structurally related poly(ethylene glycol)-block-poly(lactic-co-glycolic acid) (PEG5K-b-PLGA10K) NPs with the assistance of a synthesized lipid featuring surface amine groups for subsequent charge tuning. NPs were prepared by a double emulsion method, and their surface charge could be tuned and controlled by a succinylation reaction to yield NPs with different surface charges, while maintaining their size and composition. The prepared NPs were termed as aminated NPs (ANPs), plain NPs (PNPs), or carboxylated NPs (CNPs) based on their surface charge. All NPs exhibited the desired structural stability and siRNA integrity after enzymatic degradation. In vivo studies showed that ANPs significantly accumulated in inflamed colons, and they were successful in decreasing TNF-α secretion and mRNA expression levels while maintaining colonic histology in a murine model of acute ulcerative colitis (UC). This study described a methodology to modify the surface charge of siRNA-encapsulating polymeric NPs and highlighted the influence of surface charge on oral delivery of siRNA for localized inflammatory disorders.展开更多
基金funded by the National Key Research and Development Program of China(2018YFA0900702).
文摘Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.
基金the Graduate Student Research Innovation Project of Chongqing(No.CYB22016)National Natural Science Foundation of China(Nos.52237010,52277135,51907011)。
文摘The surface charge accumulation on polymers often leads to surface flashover.Current solutions are mainly based on the introduction of inorganic fillers.The high-cost process and low compatibility remain formidable challenges.Moreover,existing researches on all-organic insulation focus on capturing electrons,contrary to alleviating charge accumulation.Here,an all-organic modification coating was prepared on polystyrene(PS)with the large-scale atmospheric-pressure plasma,which exhibits outperformed function in mitigating surface charge accumulation.The surface charge dissipation rate and surface conductivity are promoted by about 1.37 and 9.45 times,respectively.Simulation and experimental results show that this all-organic modification coating has a smaller electron affinity potential compared with PS.The decrease of electron affinity potential may result in accelerated surface charge decay of PS,which has never been involved in previous works.Moreover,this coating also has good reliability in a repeated surface flashover.This facile and large-scale approach brings up a novel idea for surface charge regulation and the manufacture of advanced dielectric polymers.
文摘Speciation and fractionation of heavy metals in soil subsamples experimentally loaded with Pb, Cd, Cu and Zn in orthogonal design was investigated by sequential extraction, and operationally defined as water soluble and exchangeable(SE), weakly specific adsorbed(WSA), Fe and Mn oxides bound(OX) and organic bound(ORG). The results showed that fractions of heavy metals in the soil subsamples depended on their speciation. About 90% of Cd and 75% of Zn existed in soil subsamples in the SE fraction. Lead and Cu existed in soil subsamples as SE, WSA and OX fractions simultaneously, although SE was still the major fraction. Organic bound heavy metals were not clearly apparent in all the soil subsamples. The concentration of some heavy metal fractions in soil subsamples showed the good correlation with ionic impulsion of soil, especially for the SE fraction. Continuous saturation of soil subsamples with 0.20 mol/L NH 4Cl, which is the first step for determination of the negative surface charge of soil by the ion retention method, resulted in desorption of certain heavy metals from the soil. It was found that the percentage desorption of heavy metals from soil subsamples depended greatly on pH, the composition and original heavy metal content of the soil subsamples. However, most of the heavy metals in the soil subsamples were still be retained after multiple saturation. Compared with the parent soil, the negative surface charge of soil subsamples loaded with heavy metals did not show difference significantly from that of the parent one by statistical analysis. Heavy metals existed in the soil subsamples mainly as exchangeable and precipitated simultaneously.
基金supported in part by National Natural Science Foundation of China(Nos.50937004,50777051)
文摘Surface charges greatly affect the discharge/flashover development process across an insulator. The relationship between surface charge distribution on insulating materials and measurement data based on Pockels technique is discussed, and an improved algorithm is built to calculate the real surface charge density from original data. In this algorithm, two-dimensional Fourier transform technique and Wiener filter are employed to reduce the amount of numerical calculation and improve the stability of computation, Moreover, this algorithm considers not only the influence of sample's thickness and permittivity, but also the impact of charges at different positions. The achievement of this calibration algorithm is demonstrated in details. Compared with traditional algorithms, the improved one supplies a better solution in the calibration of surface charge distribution on different samples with different thickness.
基金supported by the National Key Research and Development Program(Grant No.2016YFB0900900)National Natural Science Foundation of China(Grant No.51577064)
文摘The ion flow field on the ground is one of the significant parameters used to evaluate the electromagnetic environment of high voltage direct current(HVDC) power lines.HVDC lines may cross the greenhouses due to the restricted transmission corridors.Under the condition of ion flow field,the dielectric films on the greenhouses will be charged,and the electric fields in the greenhouses may exceed the limit value.Field mills are widely used to measure the groundlevel direct current electric fields under the HVDC power lines.In this paper,the charge inversion method is applied to calculate the surface charges on the dielectric film according to the measured ground-level electric fields.The advantages of hiding the field mill probes in the ground are studied.The charge inversion algorithm is optimized in order to decrease the impact of measurement errors.Based on the experimental results,the surface charge distribution on a piece of quadrate dielectric film under a HVDC corona wire is studied.The enhanced effect of dielectric film on ground-level electric field is obviously weakened with the increase of film height.Compared with the total electric field strengths,the normal components of film-free electric fields at the corresponding film-placed positions have a higher effect on surface charge accumulation.
基金financially supported by the National Natural Science Foundation of China(Nos.51804213,51820105006,51474167,51674183,and 51674174)the China Scholarships Council(No.201906935041)。
文摘Surface charges and hydration are predominant properties of colloidal particles that govern colloidal stability in aqueous suspensions.These properties usually coexist and interact with each other.The correlation between the surface charge and hydration of minerals is summarized on the basis of innovative experimental,theoretical,and molecular dynamics simulation studies.The factors affecting the adsorption behavior of ions and water molecules,such as ion concentration,ion hydration radius and valence,and surface properties,are discussed.For example,the hydration and adsorption states completely differ between monovalent and divalent ions.For ions of the same valence,the effect of surface charge on the hydration force follows the Hofmeister adsorption series.Electrolyte concentration exerts a significant effect on the hydration force at high ion concentrations.Meanwhile,the ion correlations in high-concentration electrolyte systems become long range.The interfacial water structure largely depends on surface chemistry.The hydration layer between different surfaces shows large qualitative differences.
文摘Biodegradable polymeric materials are the most common carriers for use in drug delivery systems. With this trend, newer drug delivery systems using targeted and controlled release polymeric nanoparticles (NPs) are being developed to manipulate their navigation in complex in vivo environment. However, a clear understanding of the interactions between biological systems and these nanoparticulates is still unexplored. Different studies have been performed to correlate the physicochemical properties of polymeric NPs with the biological responses. Size and surface charge are the two fundamental physicochemical properties that provide a key direction to design an effective NP formulation. In this critical review, our goal is to provide a brief overview on the influences of size and surface charge of different polymeric NPs in vitro and to highlight the challenges involved with in vivo trials.
文摘Pathological effects of asbestos are probably dependent on the special surface properties of the fibers, such as surface charge, surface metal ions. The present study was designed to determine whether the pretreatment of chrysotile asbestos fibers (CAF) with rare earth compounds (REC) solution can reduce their pathogenicity. The results showed that REC-pretreated CAF induced less nitrogen oxide (NO) production by alveolar macrophages (AM). In addition, the pretreatment lowered the capacity of hemolysis and the methylene blue (MB) adsorption of the native CAF. These findings suggested that the pretreatment of CAF with REC solution reduced the in vitro toxicity of CAF by lessening its surface charges. Nevertheless, the pathogenicity and the carcinogenicity of REC-pretreated CAF in vivo remain to be investigated.
基金Project supported by the National Key R&D Program of China(Grant No.2018YFB0904400)the National Natural Science Foundation of China(Grant No.51977187)+3 种基金the“Science and Technology Innovation 2025”Key Project of Ningbo City,China(Grant No.2018B10019)the Natural Science Foundation of Zhejiang Province,China(Grant No.LY18E070003)the State Key Laboratory of HVDC,Electric Power Research Institute,China Southern Power Grid(Grant No.SKLHVDC-2019-KF-18)the Fundamental Research Funds for the Central Universities,China(Grant No.2018QNA4017).
文摘We present the variations of electrical parameters of dielectric barrier discharge(DBD)when the DBD generator is used for the material modification,whereas the relevant physical mechanism is also elaborated.An equivalent circuit model is applied for a DBD generator working in a filament discharging mode,considering the addition of epoxy resin(EP)as the plasma modified material.The electrical parameters are calculated through the circuit model.The surface conductivity,surface potential decay,trap distributions and surface charge distributions on the EP surface before and after plasma treatments were measured and calculated.It is found that the coverage area of micro-discharge channels on the EP surface is increased with the discharging time under the same applied AC voltage.The results indicate that the plasma modified material could influence the ignition of new filaments in return during the modification process.Moreover,the surface conductivity and density of shallow traps with low trap energy of the EP samples increase after the plasma treatment.The surface charge distributions indicate that the improved surface properties accelerate the movement and redistribution of charge carriers on the EP surface.The variable electrical parameters of discharge are attributed to the redistribution of deposited surface charge on the plasma modified EP sample surface.
基金supported by Science Foundation of Hunan University
文摘A surface charge measuring system using the capacitive probe method is analysed. The present study shows that the measuring system cannot have a steady-state output and that the error resulting from the finite leakage resistance of the measuring system will be accumulated during the measuring process. Based on the theoretical analysis a new type probe with a low charge leakage and high resolution is designed. The surface charge accumulated on the Teflon insulator under a DC voltage is measured using this new probe and some phenomena of the surface charging are reported.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences,China(Nos.XDA23010300 and XDA23010000)the National Natural Science Foundation of China(Nos.51878644 and 41573138)the CAS Youth Interdisciplinary Team.
文摘The solar-driven reduction of CO_(2) into valuable products is a promising method to alleviate global environmental problems and energy crises.However,the low surface charge density limits the photocatalytic conversion performance of CO_(2).Herein,a polymeric carbon nitride(PCN)photocatalyst with Zn single atoms(Zn1/CN)was designed and synthesized for CO_(2) photoreduction.The results of the CO_(2) photoreduction studies show that the CO and CH_(4) yields of Zn1/CN increased fivefold,reaching 76.9 and 22.9μmol/(g·h),respectively,in contrast to the unmodified PCN.Ar+plasma-etched X-ray photoelectron spectroscopy and synchrotron radiation-based X-ray absorption fine structure results reveal that Zn single atom is mainly present in the interlayer space of PCN in the Zn–N_(4) configuration.Photoelectrochemical characterizations indicate that the interlayer Zn–N_(4) configuration can amplify light absorption and establish an interlayer charge transfer channel.Light-assisted Kelvin probe force microscopy confirms that more photogenerated electrons are delivered to the catalyst surface through interlayer Zn–N_(4) configuration,which increases its surface charge density.Further,in-situ infrared spectroscopy combined with density functional theory calculation reveals that promoted surface charge density accelerates key intermediates(*COOH)conversion,thus achieving efficient CO_(2) conversion.This work elucidates the role of internal single atoms in catalytic surface reactions,which provides important implications for the design of single-atom catalysts.
基金supported by the National Natural Science Foundation of China(51737005,52127812,51929701).
文摘Surface charge accumulation is considered to be a critical factor in flashover failure of three-post insulators.However,surface charge accumulation characteristics on threepost insulators with complex structures and uneven electric fields are still unclear.Furthermore,the temperature gradient field makes charge accumulation more complicated.In this presentation,surface charge profiles of DC three-post insulators under electro-thermal coupling stress are studied by establishing a multi-degree-of-freedom movement measurement system.The abdominal area of the three-post insulator accumulaftes charges of identical polarity as the DC voltage,while the leg area accumulates heteropolar charges.Charge density from the bottom of the leg to the center of the abdomen presents a trimodal distribution pattern,including two homopolar charge peaks and one heteropolar charge peak.Asymmetrical surface conductance distribution arising from the temperature gradient leads to a significant increase in amplitude and distribution range of the homopolar charge peak at the legs of insulator.Increase of the temperature gradient will further magnify the homopolar charge peak at the legs.When DC voltage is 100 kV and conductive pole temperature is 70℃,surface charge density of the three-post insulator can reach 100μC/m^(2).Therefore,surface conductance regulation of the leg region is the key to charge regulation and insulation optimization design of DC three-post insulators.
基金financially supported by the National Key Research and Development Program of China(No.2017YFA0204700)the National Natural Science Foundation of China(Nos.21805285,22175186 and 21803008)。
文摘Surface charge transfer doping of graphene plays an important role in graphene-based electronics due to its simplicity,high doping efficiency,and easy-controllability.Here,we demonstrate the effective surface charge transfer hole doping of graphene by using a strong p-type molecular dopant hexacyanotrimethylene-cyclopropane (CN6-CP).The CN6-CP exhibits a very high intrinsic work function of 6.37 e V,which facilitates remarkable electron transfer from graphene to CN6-CP as revealed by in situ photoelectron spectroscopy investigations.Consequently,hole accumulation appears in the graphene layer at the direct contact with CN6-CP.As evidenced by Hall effect measurements,the areal hole density of graphene significantly increased from 8.3×10^(12)cm^(-2) to 2.21×10^(13)cm^(-2) upon 6 nm CN6-CP evaporation.The CN6-CP acceptor with strong p-doping effect has great implications for both graphene-based and organic electronics.
基金the financial support from National Natural Science Foundation of China (No. 51607128)Natural Science Foundation of Hubei Province (No. 2016CFB111)China Postdoctoral Science Foundation (No. 2016M602353)
文摘In an insulating system including solid and gas dielectrics, discharge type has a strong impact on charge accumulation at the interface between two dielectrics, and hence charge decay. In order to clarify the influence, a surface charge measurement system was constructed, and three types of discharge, i.e. surface discharge, and low intensity and high intensity coronas, were introduced to cause surface charge accumulation. The decay behavior of surface charges after different types of discharge was obtained at various temperatures. It was found that total surface charges monotonically decreased with time, and the decay rate became larger as temperature increased. However, after a surface discharge or a high intensity corona, surface charge density in the local area appeared to fluctuate during the decay process. Compared with this, the fluctuation of surface charge density was not observed after a low intensity corona. The mechanisms of surface charge accumulation and decay were analysed. Moreover, a microscopic physical model involving charge production, accumulation, and decay was proposed so that the experimental results could be explained.
基金the financial support from Natural Science Foundation of Jiangsu Province(No.BK20170005)the National Natural Science Foundation of China(No.21872100)+1 种基金Singapore MOE Grants MOE2019-T2-1-002 and R143-000-A43-114,Fundamental Research Foundation of Shenzhen(Nos.JCYJ20190808152607389 and JCYJ20170817100405375)Shenzhen Peacock Plan(No.KQTD2016053112042971).
文摘Doping of semiconductors,i.e.,accurately modulating the charge carrier type and concentration in a controllable manner,is a key technology foundation for modern electronics and optoelectronics.However,the conventional doping technologies widely utilized in silicon industry,such as ion implantation and thermal diffusion,always fail when applied to two-dimensional(2D)materials with atomically-thin nature.Surface charge transfer doping(SCTD)is emerging as an effective and non-destructive doping technique to provide reliable doping capability for 2D materials,in particular 2D semiconductors.Herein,we summarize the recent advances and developments on the SCTD of 2D semiconductors and its application in electronic and optoelectronic devices.The underlying mechanism of STCD processes on 2D semiconductors is briefly introduced.Its impact on tuning the fundamental properties of various 2D systems is highlighted.We particularly emphasize on the SCTD-enabled high-performance 2D functional devices.Finally,the challenges and opportunities for the future development of SCTD are discussed.
基金financially supported by the Special Fund for Agroscientific Research in the Public Interest(Grant No.201303046)the 973 Program(Grant No.2013C13531500)the Knowledge Innovation Program of the Chinese Academy of Sciences(Grant No.KSCX2-EW-R-19)
文摘The use of microparticles(MPs) as adjuvants has attracted increasing interest in vaccine delivery systems.Many physiochemical characteristics of MPs including hydrodynamic size,surface properties,and morphology can regulate the immune response.Surface charge is an important characteristic of MPs,but how it affects their adjuvanticity remains unknown.In this study,we prepared uniform-sized polylactide MPs coated with various polymers of different positive charge,and investigated how the surface charge affected antigen loading and macrophage phagocytosis and activation in vitro.A higher surface charge greatly enhanced antigen loading and antigen internalization into macrophages,promoted the expression of MHC 11 and CD80,and increased the secretion level of TNF-a.Taken together,these results indicated that surface charge was an important parameter for improving the adjuvanticity of MPs.
基金This work was supported by the National Natural Science Foundation of China(No.61904043)the Natural Science Foundation of Zhejiang Province(No.LQ19A040009).
文摘Surface charge transfer doping has been widely utilized to tune the electronic and optical properties of semiconductor photodetectors based on low-dimensional materials.Although many studies have been conducted on the performance(response time,responsivity,etc.)of doped photodetectors and their mechanisms,they merely examined a specific thickness and did not systematically explore the dependence of doping effects on the number of layers.This work performs a series of investigations on ReS_(2)photodetectors with different numbers of layers and demonstrates that the p-dopant tetrafluorotetracyanoquinodimethane(F_(4)-TCNQ)converts the deep trap states into recombination centers for few-layer ReS_(2)and induces a vertical p-n junction for thicker ReS_(2).A response time of 200 ms is observed in the decorated 2-layer ReS_(2)photodetector,more than two orders of magnitude faster than the response of the pristine photodetector,due to the disappearance of deep trap states.A current rectification ratio of 30 in the F_(4)-TCNQ-decorated sandwiched ReS_(2)device demonstrates the formation of a vertical p-n junction in a thicker ReS_(2)device.The responsivity is as high as 2,000 A/W owing to the strong carrier separation of the p-n junction.Different thicknesses of ReS_(2)enable switching of the prominent operating mechanism between transforming deep trap states into recombination centers and forming a vertical p-n junction.The thicknessdependent doping effect of a two-dimensional material serves as a new mechanism and provides a scheme toward improving the performance of other semiconductor devices,especially optical and electronic devices based on low-dimensional materials.
基金supported by the National Natural Science Foundation of China (Nos. 51025314, 50973122,)the Knowledge Innovation Program of the Chinese Academy of Sciences (No. KJCX2-YW-H19)
文摘This work focuses on the interaction between polymeric micelles with different charged surfaces and cancer cells in order to study the influence of surface charge on the in vitro cellular uptake efficiency. The amphiphilic diblock copolymers poly(e-caprolaetone)-b-poly(ethylene oxide) (PCL-b-PEO) with different functional groups at the end of hydrophilic block were synthesized. The functional groups endue the micelles with different charges on the surfaces. The cellular uptake of micelles to T-24 cells (human bladder tumor cells), HepG2 cells (human liver hepatocellular carcinoma cell line) and Hela cells (human epithelial cervical cancer cells) was studied by means of flow cytometer and confbcal laser scanning microscopy. The results indicate that the surface charges showed great influence on zeta potential of micelles at different pH values. The in vitro cellular uptake efficiency of micelles with different charged surfaces demonstrated different cellular uptake patterns to three kinds of cancer cells.
基金supported by the National Natural Science Foundation of China(Grant Nos.11375031 and 11335003)
文摘The transport behavior of pressure-driven aqueous electrolyte solution through charged carbon nanotubes(CNTs) is studied by using molecular dynamics simulations. The results reveal that the presence of charges around the nanotube can remarkably reduce the flow velocity as well as the slip length of the aqueous solution, and the decreasing of magnitude depends on the number of surface charges and distribution. With 1-M KCl solution inside the carbon nanotube, the slip length decreases from 110 nm to only 14 nm when the number of surface charges increases from 0 to 12 e. This phenomenon is attributed to the increase of the solid–liquid friction force due to the electrostatic interaction between the charges and the electrolyte particles, which can impede the transports of water molecules and electrolyte ions. With the simulation results,we estimate the energy conversion efficiency of nanofluidic battery based on CNTs, and find that the highest efficiency is only around 30% but not 60% as expected in previous work.
基金This work was supported by the National Basic Research Program of China (No. 2015CB932100), the National Natural Science Foundation of China (Nos. 51503195, 51390482 and 51633008), the National Key R&D Program of China (No. 2017YFA0205600), the Fundamental Research Funds for the Central Universities, and 111 Project (No. B17018). S. I. is also grateful for the CAS-TWAS president fellowship.
文摘Nanopartide (NP) drug delivery systems have been successfully designed and implemented to orally deliver small interfering RNAs (siRNAs) for inflammatory disorders. However, the influence of surface charge on orally administered siRNA nanocarriers has not been investigated. In this study, we prepared structurally related poly(ethylene glycol)-block-poly(lactic-co-glycolic acid) (PEG5K-b-PLGA10K) NPs with the assistance of a synthesized lipid featuring surface amine groups for subsequent charge tuning. NPs were prepared by a double emulsion method, and their surface charge could be tuned and controlled by a succinylation reaction to yield NPs with different surface charges, while maintaining their size and composition. The prepared NPs were termed as aminated NPs (ANPs), plain NPs (PNPs), or carboxylated NPs (CNPs) based on their surface charge. All NPs exhibited the desired structural stability and siRNA integrity after enzymatic degradation. In vivo studies showed that ANPs significantly accumulated in inflamed colons, and they were successful in decreasing TNF-α secretion and mRNA expression levels while maintaining colonic histology in a murine model of acute ulcerative colitis (UC). This study described a methodology to modify the surface charge of siRNA-encapsulating polymeric NPs and highlighted the influence of surface charge on oral delivery of siRNA for localized inflammatory disorders.