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1.
The deposition kinetics of RNA extracted from both virus and bacteria on silica surfaces were examined in both monovalent (NaCl) and divalent (CaCl(2)) solutions under a wide range of environmentally relevant ionic strength and pH conditions by utilizing a quartz crystal microbalance with dissipation (QCM-D). To better understand the RNA deposition mechanisms, QCM-D data were complemented by diffusion coefficients and zeta potentials of RNA as a function of examined solution chemistry conditions. Favorable deposition of RNA on poly-l-lysine-coated (positively charged) silica surfaces was governed by the convective-diffusive transport of RNA to the surfaces. The deposition kinetics of RNA on bare silica surfaces were controlled by classic Derjaguin-Landau-Verwey-Overbeek (DLVO) interactions. The presence of divalent cations (Ca(2+)) in solutions greatly enhanced the deposition kinetics of RNA on silica surfaces. Solution pH also affected the deposition behavior of RNA on silica surfaces. Release experiments showed that detachment of RNA from silica surfaces was significant in NaCl solutions, whereas, the deposited RNA on silica surfaces in CaCl(2) solutions was more likely to be irreversible.  相似文献   

2.
The role of solution chemistry on bacterial adhesion has been investigated using a radial stagnation point flow (RSPF) system. This experimental system utilized an optical microscope and an image-capturing device to directly observe the deposition kinetics of a groundwater bacterium, Burkholderia cepacia G4g, and a marine bacterium, Halomonas pacifica g. Experiments were carried out under well-controlled hydrodynamic and solution chemistry conditions, allowing for the sensitivity of bacterial adhesion behavior to be examined under a range of ionic strength and valence (KCl vs CaCl2) simulating groundwater and marine environments. Complimentary cell characterization techniques were conducted to evaluate the electrophoretic mobility, hydrophobicity, surface charge density, and viability of the bacteria under the same range of conditions. Solution chemistry was found to have a marked effect on the electrokinetic and surface properties of bacteria and the quartz collector, as well as on the resulting rate of bacterial deposition. Comparable adhesion trends were observed for B. cepacia G4g and H. pacifica g. Specifically, the deposition rates of the two bacteria species in both KCl and CaCl2 solutions increased with ionic strength, a trend consistent with traditional Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, which considers the combination of van der Waals and electrostatic double-layer interaction forces. However, in some cases, experimental results showed bacterial deposition behavior to deviate from DLVO predictions. On the basis of the systematic investigation of bacterial cell characteristics, it was found that Ca2+ ions play a distinct role on bacterial surface charge, hydrophobicity, and deposition behaviors. It is further suggested that bacterial adhesion is determined by the combined influence of DLVO interactions, electrosteric interactions associated with solution chemistry, and the hydrodynamics of the deposition system.  相似文献   

3.
Dual low-angle light scattering and refractometric detection coupled to size-exclusion chromatography provided proof for the presence of a low amount of stable aggregates/particles in ethyl(hydroxyethyl)cellulose. Unlike the correct size-exclusion chromatographic behavior of the parent polysaccharide itself, the aggregates exhibit variable size-dependent weak retention as a function of flow-rate and of ionic strength of the aqueous mobile phase. Therefore, determination of the molecular mass of non-aggregated polymer is possible in aqueous mobile phase containing 0.1 M NaCl under conditions at which aggregates are completely adsorbed on the column packing irrespective of the flow-rate used. Flow-rate and ionic strength-dependent variations of aggregate behavior as well as model size-exclusion experiments with latex particles indicate that they partly carry a minute charge and have a compact structure. Their weak retention under the separation conditions used suggests a difference in their surface chemistry when compared with the dissolved polymer coils which exhibit a correct size-exclusion behavior.  相似文献   

4.
The significance of natural organic matter (NOM, both humic acid and alginate) on the transport and deposition kinetics of ZnO nanoparticles (NPs) in irregular quartz sand was examined by direct comparison of both breakthrough curves and retained profiles with NOM present in NPs suspension versus those obtained without NOM. Packed column experiments were conducted in both NaCl and CaCl(2) solutions under a series of environmentally relevant ionic strengths. Under all examined conditions, breakthrough plateaus with NOM even at concentration as low as 1mgL(-1) of total organic carbon (TOC) were higher than those without NOM, indicating that presence of NOM in NPs suspensions enhanced ZnO NPs transport. Although hyper-exponential retained profiles were observed both in the presence and absence of NOM, the amount of retained ZnO NPs acquired in the presence of NOM decreased slowly as the transport distance increased. Straining induced by concurrent aggregation is found to cause the hyper-exponential decrease. In the presence of NOM, electrosteric interaction effectively reduced the ZnO NPs deposition on collector surfaces and NPs-NPs aggregation. Subsequently, the amount of NPs that jammed in the column inlet in the absence of NOM were markedly decreased, which therefore exhibited as flatter retained profiles.  相似文献   

5.
Adsorption from electrolyte solutions of fully hydrolyzed polyvinylamine on cellulose fibers was investigated by supplying the polymer to the fibers at controlled rate. This was implemented by employing a reactor only open to the fluid in which the fiber dispersion were confined and homogenized. The adsorbed layers may be defined as diffuse or dense layers. Diffuse layers are characterized by a surface coverage limited to 0.65 mg/g cellulose in salt-free solutions. Addition of NaCl or CaCl(2) to the fiber dispersion and the polymer solution promotes the adsorption rate and increases the amount of adsorption to 1.5 mg/g cellulose. For dense polymer layers, for which the coverage amounts to values close to 10 mg/g cellulose in salt-free systems, addition of electrolyte does not change the kinetic and adsorption characteristics. Insofar as the variation of the molecular areas of the polymer within the diffuse layers as a function of the ionic strength parallels the variation of the molecular characteristics of solute molecules, the formation of diffuse layers is expected to proceed by random deposition of solute molecules which later individually sustain strong reconformation. Adsorption isotherms show a limited influence of the ionic strength. Obviously, the passage from dense layers of high surface coverage to low adsorption values at equilibrium requires extended reconformation of adsorbed macromolecules and desorption of a great part of the molecules already adsorbed.  相似文献   

6.
The stability of the sodium and calcium forms of montmorillonite was studied at different NaCl and CaCl2 concentrations. The aggregation kinetics was determined from the decrease in particle concentration with time at different electrolyte concentrations. The DLVO theory defines the critical coagulation concentration (CCC) value as the electrolyte concentration that balances the attractive and repulsive potential energies between the particles, making aggregation diffusion-controlled. Therefore CCC values were obtained by extrapolation of the aggregation rate constants measured as a function of ionic strength to conditions where the rate constant value is determined by diffusion only. When the electrolyte was CaCl2, the CCC value was found to be approximately two orders of magnitude lower than the CCC values obtained using NaCl as electrolyte.  相似文献   

7.
New kinds of solid fuels and propellants comprised of nanomaterials are making their way into civilian and military applications yet the impact of their release on the environment remains largely unknown. One such material is nano boron, a promising solid fuel and propellant. The fate and transport of nano boron under various aquatic systems was investigated in aggregation and deposition experiments. Column experiments were performed to examine the effects of electrolyte concentration and flow velocity on the transport of boron nanoparticles under saturated conditions, whereas aggregation tests were conducted to assess the effects of electrolytes on the aggregation of the boron nanoparticles. Aggregation tests indicated the presence of different reaction-controlled and diffusion-controlled regimes and yielded critical coagulation concentrations (CCC) of 200 mM, 0.7 mM and 1.5 mM for NaCl, CaCl(2), and MgCl(2), respectively. Aggregation and deposition experimental data corresponded with the classic Derjaguin-Landau-Verwey-Overbeek (DLVO) model and the constant attachment efficiency filtration model, respectively. Theoretical calculations indicated that both the primary and secondary energy minima play important roles in the deposition of nano boron in sand columns.  相似文献   

8.
Transport and deposition of nanoparticles (NPs) have drawn great attention in different fields of engineering in recent years because of their potential risk to the environment. In this study, mobility of aluminum oxide NP, one of the most popular metal oxide NPs, was studied in synthetic saturated porous media. The impacts of ionic strength using monovalent (NaCl) and divalent (MgCl2) salt solution, pH, and NPs concentrations on nano-alumina mobility were investigated. The experimental results showed that the transport of nano-alumina was influenced by ionic strength; the highest mobility was observed at the 0.01 M solution and decreased by increasing ionic strength. Moreover, the suspension containing alumina NPs presented the best mobility behavior in the acidic solution (pH = 2) in comparison with neutral and basic solutions. Consequently, transport of NPs with particle size distribution lower than 100 nm through porous media was facilitated at the acidic, low ionic strength condition. In addition, faster elution occurred when the influent concentration was increased from 0.1 wt% to 0.3 wt%. Finally, it is expected that ionic strength, pH of solution, and NPs concentration will be key parameters to control the nano-alumina mobility.  相似文献   

9.
In this study, a microscope-based technique was utilized to understand the fundamental mechanisms involved in deposition of TiO(2) nanoparticles (TNPs). Transport and deposition studies were conducted in a parallel plate (PP) flow chamber with TNP labeled with fluorescein isothiocyanate (FITC) for visualization. Attachment of FITC-labeled TNPs on surfaces is a function of a combination of parameters, including ionic strength (IS), pH and flowrate. Significantly higher deposition rates were observed at pH 5 versus pH 7. This is attributed to the conditions being chemically favorable for deposition at pH 5 as compared to pH 7, as predicted by DLVO theory. Additionally, deposition rates at pH 5 were reduced with IS below 10 mM due to the decrease in range of electrostatic attractive forces. Above 10 mM, aggregate size increased, resulting in higher deposition rates. At pH 7, no deposition was observed below 10 mM and above this concentration, deposition increased with IS. The impact of flowrate was also observed, with decreasing flowrate leading to greater deposition due to the reduction in drag force acting on the aggregate (regardless of pH). Comparisons between experimental and theoretical approximations indicate that non-DLVO type forces also play a significant role. This combination of observations suggest that the deposition of these model nanoparticles on glass surfaces was controlled by a combination of DLVO and non-DLVO-type forces, shear rate, aggregation state, and gravitational force acting on TNPs.  相似文献   

10.
The early stage aggregation kinetics of fullerene C60 nanoparticles were investigated in the presence of Suwannee River humic acid and common monovalent and divalent electrolytes through time-resolved dynamic light scattering (DLS). In the absence of humic acid, the aggregation behavior of the fullerene nanoparticles in the presence of NaCl, MgCl2, and CaCl2 was found to be consistent with the classic Derjaguin-Landau-Verwey-Overbeek (DLVO) theory of colloidal stability. In the presence of humic acid and NaCl or MgCl2 electrolytes, the adsorbed humic acid on the fullerene nanoparticles led to steric repulsion, which effectively stabilized the nanoparticle suspension. This behavior manifested in a dramatic drop in the rate of aggregation, an increase in the critical coagulation concentration (CCC), and an attained value of less than unity for the inverse stability ratio (or attachment efficiency) at high MgCl2 concentrations. While the increase in the nanoparticle stability was similarly observed in the presence of humic acid at low CaCl2 concentrations, enhanced aggregation occurred at higher CaCl2 concentrations. Measurement of scattered light intensities over time indicated significant aggregation of the humic acid macromolecules in solutions of high CaCl2 concentrations. Transmission electron microscopy (TEM) imaging of the fullerene aggregate structures in the presence of humic acid revealed that bridging of the fullerene nanoparticles and aggregates by the humic acid aggregates is the likely mechanism for the enhanced aggregation at high CaCl2 concentrations.  相似文献   

11.
12.
Negatively charged silica sol is known to lead to fouling of anion exchange membranes during electrodialysis (ED) as a result of its deposition on the membrane surface. It is known that the fouling potential is related to the physical and electrochemical properties of the silica particles as well as those of the anion exchange membranes. In this study, the properties of the silica sol were characterized in terms of its particle size, turbidity, and zeta potential in order to predict their effects on the electrodialysis performance. In the stability of colloidal particles, the critical coagulation concentrations of silica sol were determined as functions of ionic strength, cation species, and solution pH. In the electrodialysis of NaCl solution containing silica sol with various concentrations of CaCl(2), the colloidal behavior related to deposition and transport was examined during and after electrodialysis. The electrodialysis experiments clearly showed that the deposition and transport of silica sol during electrodialysis were related to the colloidal stability of dispersion.  相似文献   

13.
The aggregation and deposition kinetics of two multiwalled carbon nanotubes (MWNTs) with different degrees of surface oxidation are investigated using time-resolved dynamic light scattering (DLS) and quartz crystal microbalance with dissipation monitoring (QCM-D), respectively. Carboxyl groups are determined to be the predominant oxygen-containing surface functional groups for both MWNTs through X-ray photoelectron spectroscopy (XPS). The aggregation and deposition behavior of both MWNTs is in qualitative agreement with the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The critical coagulation concentration (CCC) of the highly oxidized MWNTs (HO-MWNTs) is significantly higher than the lowly oxidized MWNTs (LO-MWNTs) in the presence of NaCl (210 and 53 mM, respectively) since HO-MWNTs have a higher surface charge density. In contrast, the aggregation inverse stability profiles of HO-MWNTs and LO-MWNTs are identical and yield comparable CCCs (0.9 and 1.0 mM, respectively) in the presence of CaCl(2). Similar to the results obtained from the aggregation study, HO-MWNTs are considerably more stable to deposition on silica surfaces compared to LO-MWNTs in the presence of NaCl. However, both MWNTs have the same propensity to undergo deposition in the presence of CaCl(2). The remarkable similarity in the aggregation and deposition kinetics of HO-MWNTs and LO-MWNTs in CaCl(2) may be due to Ca(2+) cations having a higher affinity to form complexes with adjacent carboxyl groups on HO-MWNTs than with isolated carboxyl groups on LO-MWNTs.  相似文献   

14.
This study investigated the sedimentation and aggregation kinetics of titanium dioxide (TiO(2)) nanoparticles with varying material properties (i.e., crystallinity, morphology, and chemical composition). Used in the study were various types of commercially available TiO(2) nanoparticles: three spherical anatase (nominal diameters of 5, 10, and 50 nm) and two rutile nanoparticles (10×40 and 30×40 nm). The 50 nm anatase and 10×40 nm rutile showed higher stability in deionized water and 5 mM NaCl solutions at pH 7 than the 5, and 10 nm anatase nanoparticles in sedimentation experiments. In aggregation experiments, critical coagulation concentration values for the 50 nm anatase were the highest, followed by the 10×40 nm rutile and the 5 nm anatase nanoparticles in NaCl and CaCl(2) solutions. The aggregation kinetics was fitted reasonably well with the Derjaguin-Landau-Verwey-Overbeek (DLVO) equations for the TiO(2) nanoparticles tested. Results showed that crystallinity and morphology are not influential factors in determining the stability of TiO(2) nanoparticle suspensions; however, the differences in their chemical compositions, notably, the varying concentrations of impurities (i.e., silicon and phosphorus) in the pristine materials, determined the surface charge and therefore the sedimentation and aggregation of TiO(2) nanoparticles in the aqueous phase.  相似文献   

15.
The stability and aggregation behavior of iron oxide colloids in natural waters play an important role in controlling the fate, transport, and bioavailability of trace metals. Time-resolved dynamic light scattering experiments were carried out in a study of the aggregation kinetics and aggregate structure of natural organic matter (NOM) coated hematite colloids and bare hematite colloids. The aggregation behavior was examined over a range of solution chemistries, by adjusting the concentration of the supporting electrolyte-NaCl, CaCl2, or simulated seawater. With the solution pH adjusted so that NOM-coated and bare hematite colloids were at the same zeta potential, we observed a significant difference in colloid stability which results from the stability imparted to the colloids by the adsorbed NOM macromolecules. This enhanced stability of NOM-coated hematite colloids was not observed with CaCl2. Aggregate form expressed as fractal dimension was determined for both NOM-coated and bare hematite aggregates in both NaCl and CaCl2. The fractal dimensions of aggregates formed in the diffusion-limited regime indicate slightly more loosely packed aggregates for bare hematite than theory predicts. For NOM-coated hematite, a small decrease in fractal dimension was observed when the solution composition changed from NaCl to CaCl2. For systems in the reaction-limited regime, the measured fractal dimensions agreed with those in the literature. Colloid aggregation was also studied in synthetic seawater, a mixed cation system to simulate estuarine mixing. Those results describe the important phenomena of iron oxide aggregation and sedimentation in estuaries. When compared to field data from the Mullica Estuary, U.S.A., it is shown that collision efficiency is a good predictor of the iron removal in this natural system.  相似文献   

16.
The effects of salt with different valences (NaCl, CaCl2 and CrCl3) on the aggregation of O-carboxylmethylchitosan (OCMCS) in dilute aqueous solution were investigated using viscometry, dynamic laser light scattering (DLS) and atomic force microscopy (AFM). With increasing OCMCS concentration beyond a critical aggregation concentration (cac) of approximately 0.045 g/l, the aggregation of OCMCS appears in solution. The driving forces of the OCMCS aggregation are intermolecular hydrogen bond, hydrophobic interaction and electrostatic repulsion. The OCMCS aggregation behavior strongly depends on the valence of salt. When NaCl is added, the aggregate size increases with NaCl concentration. When CaCl2 or CrCl3 is added to a given OCMCS concentration, there exists a critical concentration each of Ca2+ and Cr3+. Before the critical concentration, the aggregates decrease in size with increasing salt concentration due to the intra-aggregate complexation; while after the critical concentration, the size of the aggregates increases with salt concentration due to the inter-aggregate complexation. Moreover, the effect of Cr3+ on the OCMCS aggregation is greater than that of Ca2+. The formation of the intra-aggregate complexation is found to be a kinetic process and the aggregate size decreases with time; the formation of the inter-aggregate complexation is also kinetic where the aggregate size increases with time. The aggregates dominated by the intra-aggregate complexation are small, compact and spherical, while the aggregates dominated by the inter-aggregate complexation show the big, compact and spherical morphology.  相似文献   

17.
Transport of colloidal particles in porous media is governed by the rate at which the colloids strike and stick to collector surfaces. Classic filtration theory has considered the influence of system hydrodynamics on determining the rate at which colloids strike collector surfaces, but has neglected the influence of hydrodynamic forces in the calculation of the collision efficiency. Computational simulations based on the sphere-in-cell model were conducted that considered the influence of hydrodynamic and Derjaguin-Landau-Verwey-Overbeek (DLVO) forces on colloid attachment to collectors of various shape and size. Our analysis indicated that hydrodynamic and DLVO forces and collector shape and size significantly influenced the colloid collision efficiency. Colloid attachment was only possible on regions of the collector where the torque from hydrodynamic shear acting on colloids adjacent to collector surfaces was less than the adhesive (DLVO) torque that resists detachment. The fraction of the collector surface area on which attachment was possible increased with solution ionic strength, collector size, and decreasing flow velocity. Simulations demonstrated that quantitative evaluation of colloid transport through porous media will require nontraditional approaches that account for hydrodynamic and DLVO forces as well as collector shape and size.  相似文献   

18.
The influence of humic acid and alginate, two major components of natural organic matter (NOM), on deposition kinetics of extracellular polymeric substances (EPS) on silica was examined in both NaCl and CaCl(2) solutions over a wide range of environmentally relevant ionic strengths utilizing a quartz crystal microbalance with dissipation. Deposition kinetics of both soluble EPS and bound EPS extracted from four bacterial strains with different characteristics was investigated. EPS deposition on humic acid-coated silica surfaces was found to be much lower than that on bare silica surfaces under all examined conditions. In contrast, pre-coating the silica surfaces with alginate enhanced EPS deposition in both NaCl and CaCl(2) solutions. More repulsive electrostatic interaction between EPS and surface contributed to the reduced EPS deposition on humic acid-coated silica surface. The trapping effect induced by the rough alginate layer resulted in the greater EPS deposition on alginate-coated surfaces in NaCl solutions, whereas surface heterogeneities on alginate layer facilitated favorable interactions with EPS in CaCl(2) solutions. The presence of dissolved background humic acid and alginate in solutions both significantly retarded EPS deposition on silica surfaces due to the greater steric and electrostatics repulsion.  相似文献   

19.
The deposition of eight bacterial strains on Teflon and glass in aqueous media with ionic strengths varying between 0.0001 and 1 M was measured and interpreted. Two types of interactions were considered: (1) those described by the DLVO theory, which comprise van der Waals attraction and electrostatic repulsion (bacteria and surfaces are both negatively charged); and (2) steric interactions between the outer cell surface macromolecules and the substrata. As a trend, at low ionic strength (<0.001 M), deposition is inhibited by DLVO-type electrostatic repulsion, but at high ionic strength (≥0.1 M) it is dominated by steric interactions. The ionic strength at which the transition from the DLVO-controlled to the sterically controlled deposition occurs, is determined by the extension of the macromolecules into the surrounding medium, which varied between 5 and 100 nm among the bacterial strains studied. The steric interactions either promote deposition by bridging or inhibit it by steric repulsion. Between Teflon and hydrophobic bacteria, bridging is generally observed. The surface of one bacterial strain contains amphiphilic macromolecules that form bridges with Teflon but induce steric repulsion on glass. The presence of highly polar anionic polysaccharide coatings on the cell impedes attachment on both glass and Teflon. For practice, the general conclusion is that the deposition of most bacteria is: (1) strongly inhibited by DLVO-type electrostatic repulsion in aqueous environments of low ionic strength such as rain water, streams and lakes; (2) controlled by DLVO and/or steric interactions in systems as domestic waste waters and saliva; and (3) determined by steric interactions only in more saline environments as milk, urine, blood and sea water.  相似文献   

20.
Small-angle X-ray scattering (SAXS) together with static (SLS) and dynamic light scattering (DLS) measurements were carried out on aqueous solutions of lysozyme (LY) and of the ionic biological detergent sodium glycocholate (NaGC). Apparent diffusion coefficients (D app), excess Rayleigh ratio, and SAXS spectra were measured for 0.1 M NaGC solutions at different ionic strengths (0.05-0.30 M NaCl). The same data were collected for LY in sodium acetate buffer 50 mM without and with 92 mM NaCl as a function of protein concentration (10-80 g L(-1)). A correlated analysis of SLS data and SAXS spectra was first tested on the LY samples and then extended to the interpretation of the NaGC data to infer information on particle structure and interaction potential. A hard-core (HC) interaction shell of uniform thickness, a screened Coulomb potential of the electric double layer (EDL) or the complete DLVO potential were alternatively used to represent the long-range tail of the interaction potential. Whenever an essentially repulsive tail is expected, all the representations give reasonable results, but the data analysis does not allow the discrimination between the oblate and the prolate symmetries of the NaGC aggregates. The DLVO model allows the interpretation of the data even when the attractive component determines the tail character. With this model an overall fit of the micelle data at all the NaCl concentrations was successfully performed by assuming a simple spherical symmetry of the micelles and invariant values of their ionization degree and Hamaker constant, thus considering just the screening effect of the added electrolyte. Whatever model is used, the results point out that the aggregates are quite hydrated (26-38 water molecules per monomer) and very slightly grow by increasing the NaCl concentration. When spherical symmetry is assumed the aggregate radii for all the samples fall in the range 15-16 A. From the SAXS and SLS, best fitting geometrical parameters, and interparticle structure factor, a D app value was calculated for each sample. An excellent consistence is achieved for LY results. On the contrary, calculated D app values systematically lower than the experimental values are always obtained for the NaGC micelles. Micelle polydispersity and internal dynamics seem to be the most probable reasons of the bad agreement.  相似文献   

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