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PubMed2001

An investigation into the suitability of silica beads for cell separations based on density perturbation.

This study has investigated possible alternative types of beads for fractionating cells on the basis of density perturbation. It is well known that uniform magnetic beads can be extremely important tools for separating cells by both magnetic separation techniques and density perturbation. However, because of the inherent expense associated with the use of magnetic beads, it was decided to study the possible use of inexpensive silica beads for density perturbation in terms of their attachment and modification of density of cells and to compare them with uniform Dynabeads. Silica beads were analyzed to determine their size and effect on the density of cells. Differentiated HL60 cells were used as a model system. As differentiation occurs, different levels of antigens are expressed on the cell surface and this results in different numbers of beads binding to cells. DMSO-differentiated HL60 cells were mixed with anti-CD11b-coated beads at a ratio of 20:1 (beads/cell), and gentle mixing was carried out at 20 degrees C on the end-over-end mixer. The binding of antibody-coated silica beads and Dynabeads to partially differentiated HL60 cells were compared. The conclusions reached on the basis of these experiments are that antibody-coated silica beads (Ab-coated silica) can be used as alternative beads for some cell fractionations. However, compared with Dynabeads, there are more beads that are only transiently associated with cells, possibly indicating that higher levels of detachment of beads from cells occur when silica beads are used. In addition, silica beads are usually heterogeneous in size and this would make it difficult to use these beads for the isolation of purified subpopulations of differentiated cells.

Cell Count↗

PubMed2000

The concentration, apparent molecular weight and chemical reactivity of silica from groundwater in southern Nevada.

Sorption of radionuclides, metals and organic compounds to colloidal particles has been suggested to increase the mobility of these pollutants in groundwater. Because silicates and alumino-silicates can be important components of groundwater colloids, we have conducted a study to characterize the nature of silica in various springs and wells in Southern Nevada and to determine the extent that silica may be associated with colloidal particles that can participate in pollutant transport. The total silica content was measured using inductively coupled plasma emission spectroscopy (ICP). In addition, reactive silica was measured using the silica molybdate colorimetric technique. The apparent molecular weight of the silica was investigated using split-flow-lateral-transport-thin-cell-fractionation (SPLITT) which can readily distinguish between colloidal and low molecular weight associations. This study indicates that silica does not tend to form stable inorganic colloids in Southern Nevada groundwaters but exists as low molecular weight species. However, water from one of the test facilities on the Nevada Test Site (NTS) did contain stable siliceous colloids that could have important implications for the modeling the transport of radionuclides at this site.

Colloids↗

PubMed2003

Surface modification of hydroxyapatite. Part II. Silica.

Nanophase hydroxyapatite (HAP) particles were coated with varying amounts of silica (5-75wt%) via the hydrolysis of tetraethyl orthosilicate. The nanocomposite particles were characterized by transmission electron spectroscopy, X-ray diffraction (XRD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), BET N(2) gas adsorption, sedimentation time studies, acid dissolution, and zeta potential (zeta). A sequential decrease in infrared spectral features characteristic of HAP was accompanied by an increase in features characteristic of silica as revealed by DRIFTS. The specific surface area of the silica-coated HAP particles showed a non-systematic increase. In comparison to the uncoated HAP (50m(2)/g), silica coatings of 5, 25, 50 and 75wt% yielded specific surface areas of 55, 93, 70, and 138m(2)/g, respectively. This behavior can be explained based on a heterocoagulation coating mechanism in which silica clusters of approximately 14nm in diameter adsorb onto the HAP particle surface. The decrease in specific surface area at 50wt% silica corresponded to the attainment of a complete surface coating. This conclusion was substantiated by the observed resistance of these particles to dissolution in 1M HCl. However, the acid treatment transformed the silica-coated HAP core particles to CaCl(2).Ca(H(2)PO(4))(2).2H(2)O (calcium chloride phosphate hydrate) based on XRD analysis.

Biocompatible Materials↗

PubMed2003

Modelling of silica diffusion experiments with 32Si in Boom Clay.

A mathematical model describing the dissolution of nuclear glass directly disposed in clay combines a first-order dissolution rate law with the diffusion of dissolved silica in clay. According to this model, the main parameters describing the long-term dissolution of the glass are etaR, the product of the diffusion accessible porosity eta and the retardation factor R, and the apparent diffusion coefficient D(app) of dissolved silica in clay. For determining the migration parameters needed for long-term predictions, four Through-Diffusion (T-D) experiments and one percolation test have been performed on undisturbed clay cores. In the Through-Diffusion experiments, the concentration decrease after injection of 32Si (radioactive labelled silica) was measured in the inlet compartment. At the end of the T-D experiments, the clay cores were cut in thin slices and the activity of labelled silica in each slice was determined. The measured activity profiles for these four clay cores are well reproducible. Since no labelled silica could be detected in the outlet compartments, the Through-Diffusion experiments are fitted by two In-Diffusion models: one model assuming linear and reversible sorption equilibrium and a second model taking into account sorption kinetics. Although the kinetic model provides better fits, due to the sufficiently long duration of the experiments, both models give approximately similar values for the fit parameters. The single percolation test leads to an apparent diffusion coefficient value about two to three times lower than those of the Through-Diffusion tests. Therefore, dissolved silica appears to be strongly retarded in Boom Clay. A retardation factor R between 100 and 300 was determined. The corresponding in situ distribution coefficient K(d) is in the range 25-75 cm(3) g(-1). The apparent diffusion coefficient of dissolved silica in Boom Clay is estimated between 2 x 10(-13) and 7 x 10(-13) m(2) s(-1). The pore diffusion coefficient is in the range from 6 x 10(-11) to 1 x 10(-10) m(2) s(-1).

Aluminum Silicates↗

PubMed1984

Protection of mice against infection with mouse hepatitis virus type 3 by injection of silica.

Injection of silica did not brake the resistance against MHV3 conferred to C57BL/6 mice by injection of C. parvum. However, silica itself had a marked protective effect against MHV3 infection that was maximal when injecting 1 mg 2 hrs before virus infection. The protective effect of silica was observed in a number of inbred mouse strains that differ in their relative resistance to MHV3 infection. No viral titers were observed in the spleen and liver of mice which had received MHV3 plus silica, whereas high titers were observed in the virus-infected controls. Injection of silica caused a marked decrease in the number of esterase-positive macrophages in the peritoneal wash-out population, that may be compatible with the possibility that the cause of the protection is the depletion of target cells for the viral infection. This latter effect, however, was short-lived and 24-48 hrs after injection of silica, high numbers of esterase-positive cells were again observed. This may explain why only little protection was observed when silica was administered 2 days before virus infection.

Adjuvants, Immunologic↗

PubMed1988

The effect of silica treatment on accessory cell-dependent rat T lymphocyte proliferation.

Previous work has shown that purified rat macrophages lack both accessory activity for T lymphocyte responses to mitogens and stimulatory activity in a mixed leukocyte reaction, in marked contrast to the potent activity of dendritic cells. This study was designed to re-evaluate macrophages as accessory cells by treating various cell preparations with either silica or L-leucine methyl ester, which have been reported to be toxic to macrophages, and then determining the effect of the treated cells on responses to the mitogens, sodium periodate or concanavalin A. These studies indicated that treatment with L-leucine methyl ester failed to kill rat macrophages or dendritic cells, whereas silica was specifically toxic for rat macrophages. The studies therefore focused on silica. Co-culturing mitogen-treated lymph node cells with silica over a wide range of concentrations had no effect on responses. The same results were obtained if mitogen-treated lymphocytes were enriched with lymph node macrophages and dendritic cells and then co-cultured with silica. Preparations containing both macrophages and dendritic cells were incubated with silica for 24 h to ensure the death of virtually all macrophages; upon the addition of mitogen-treated lymphocytes, the macrophage-depleted accessory cells induced vigorous proliferative responses. Peritoneal exudate cells showed variable, but low accessory activity that increased after incubation with silica. Elimination of more than 90% of the macrophages from peritoneal exudate cells, as determined by staining for non-specific esterase, failed to eliminate this accessory activity. Taken together, these findings confirm and extend the conclusion that rat macrophages lack or have exceedingly low accessory activity.

Animals↗

PubMed1997

Selective hyperexpression of c-jun oncoprotein by glass fiber- and silica-transformed BALB/c-3T3 cells.

Mining and mineral processing are important industries in the United States. A large number of workers are potentially exposed to silica during mining and to glass fibers during manufacturing. There is a concern regarding lung cancer risk among workers exposed to silica and glass fibers. Our previous studies showed that both glass fibers and silica induced transformation of BALB/c-3T3 cells. In order to explore the relationship between silica and glass fiber-induced cell transformation and oncoprotein expression, the protein products of seven proto-oncogenes (c-K-ras, c-H-ras, c-sis, c-myc, c-myb, c-erb B1 and c-jun) and one tumor suppressor gene (p53) were examined in BALB/c-3T3 cells transformed by glass fibers or silica using immunoblotting with specific monoclonal or polyclonal antibodies. The results showed that all transformants, including eight induced by glass fibers and eight by silica (Min-U-Sil 5), were positive for c-jun protein expression; the level of c-jun protein was elevated 8-21-fold in these transformants. Other protooncogene proteins in transformed cells were either not detectable or not different from non-transformed cells. These results suggest that the overexpression of c-jun is common in BALB/c-3T3 transformed cells induced by glass fibers or silica. It seems, therefore, that the expression of c-jun may play an important role in the transformation process.

3T3 Cells↗

PubMed1999

Silica-induced apoptosis in vitro and in vivo.

Silica exposure results in an initially acute inflammatory response followed by chronic fibrotic change. The mechanism for the maintenance of silica-induced inflammation has not been understood yet. In silica-induced acute inflammation and chronic fibrosis, various mediators such as reactive oxygen species, cytokines and growth factors are released. And these substances are suggested to have the regulatory role for the inflammation and fibrosis by possessing the potential to influence apoptosis. To demonstrate the apoptosis as an underlying mechanism for the development of silicosis, in vitro and in vivo models were designed. In in vitro study, we evaluated that apoptotic cell fraction in silica (10, 50 microg/cm2)-treated A549 cells was significantly increased in comparison with control by FACS (fluorescein activated cell sorter). Also genomic DNA from silica (10, 50 microg/cm2)-treated A549 showed DNA ladder formation while control and 1 microg/cm2 groups didn't. In in vivo study, total cell numbers and apoptotic cell numbers of BAL (bronchoalveolar lavage) fluid from silica (10, 20, 40 mg/kg)-instilled rats were significantly higher than control group from 1 week. From these results, we concluded acute and chronic presence of apoptosis may contributes to silica-induced acute inflammation and chronic fibrosis.

Animals↗

PubMed2002

A case-control study of lung cancer in relation to silica exposure and silicosis in a rural area in Japan.

PURPOSE: In southeast Okayama Prefecture, Japan, there have been reports of a high prevalence of silicosis among refractory brick production workers. Recently, a high mortality rate of lung cancer among the local residents has been observed. Therefore, a population based case-control study was conducted concerning the relationship between silica, silicosis, and lung cancer using multiple cancer controls. METHODS: Cases and controls were restricted to male subjects and information was obtained from death certificates from 1986 to 1993 in the area. Three categories of deceased control groups were selected: a series of deaths from liver cancer, colon cancer, and cancers of other organs, which was assumed not to be related to silica exposure. Age and smoking habits were adjusted by stratified analysis using the Mantel-Haenszel odds ratio estimates. Unconditional logistic regression analysis was also conducted to control potential confounding factors; such as age and smoking habits. RESULTS: The age-, smoking-adjusted odds ratios were 1.94 (0.94-4.43) for the colon cancer control group, 2.13 (1.19-3.85) for the other cancer control group related to silica exposure, and 2.94 (1.30-8.90) and 2.69 (1.43-5.37) related to silicosis, respectively. The direct weighted average using the estimates for colon and the other cancer controls was 2.06 (1.29-3.29) for silica exposure, and 2.77 (1.60-4.77) for silicosis. Histological or cytological types of lung cancer cases were obtained from 64.1% of the subjects (118/184). As for the histologic type of lung cancer, small cell carcinoma was higher among those who had been silica-exposed workers than the unexposed lung cancer cases and the data from the general Japanese population. On chest x-ray findings, elevated lung cancer mortality compared with cancers other than lung cancer was demonstrated among patients without large opacities. CONCLUSIONS: Silica exposure increased the lung cancer mortality in the area. A high lung cancer mortality rate in the area could be explained by silica exposure and silicosis prevalence in this area.

Adult↗

PubMed1994

Silica-based room temperature phosphorescence substrates: wide dynamic ranges, low background, and programmable figures of merit.

The use of silica-based substrates for room temperature phosphorescence (RTP) was investigated. Contrary to reports in the literature, bare silica was shown to provide higher sensitivity (S/B) for RTP than filter paper when the specific surface areas of the two substrates were similar. The surface heterogeneity of bare silica resulted in nonlinear, discontinuous response curves for a model analyte, phenanthrene. However, analytically useful calibration curves were obtained on silica thin-layer phases in the presence of coadsorbed surfactant. The dynamic range on the silica substrate was 4 times greater and the background phosphorescence was 2 orders of magnitude lower than filter paper. The programming of figures of merit for silica-based substrates via the silica specific surface area is demonstrated.

Fluorometry↗

PubMed2004

Modifying the adsorption behavior of polyamidoamine dendrimers at silica surfaces investigated by total internal reflection fluorescence correlation spectroscopy.

Polyamidoamine (PAMAM) dendrimers were modified and tested for use as solution-phase diffusion probes in silica nanostructures. In order for the successful application of dendrimers as solution-phase probes, their interactions with silica surfaces must be understood and controlled, so that the motion of the probe is not influenced by adsorption. Adsorption/desorption kinetics of PAMAM dendrimers and their diffusion in solution near silica surfaces were investigated with total internal reflection fluorescence correlation spectroscopy (TIR-FCS). Dendrimers of generations 3, 5, and 7 were dye-labeled with carboxyrhodamine 6G. Because PAMAM dendrimers are positively charged in solution (having primary amines as end groups), significant adsorption of these molecules to the negatively charged silica surface was observed. Adsorption/desorption rates and the equilibrium constant for adsorption were determined by fitting the autocorrelation functions to a kinetic model. The desorption rate decreases and the absorption equilibrium constant increases with higher dendrimer generation. To reduce the adsorption of these probes to silica surfaces, the labeled dendrimers were reacted with succinic anhydride, converting the primary amine end groups to negatively charged carboxylic acid groups. These carboxylated dendrimers did not detectably adsorb to silica from aqueous solution. TIR-FCS was used to determine their free-solution diffusion constants near silica surfaces, and the corresponding hydrodynamic radii compare favorably with values reported from forced Rayleigh scattering measurements.

Journal Article↗

PubMed2005

Adsorption of duplex DNA on mesoporous silicas: possibility of inclusion of DNA into their mesopores.

It is well known that a silica surface cannot adsorb duplex DNA in common aqueous solution (not chaotropic solution) because of the electrostatic repulsion of the silica surface and polyanionic DNA. However, we recently found that when duplex DNA in phosphoric acid form (or in acidic solution) was used, DNA was successfully adsorbed into mesoporous silicas even in low-salt aqueous solution. The adsorption behaviors of DNA into mesoporous silicas were influenced by the pore diameter sizes. Mesoporous silicas with 2.80- or 3.82-nm peak pore diameters adsorbed DNA the best in diluted NaCl solution. Formation of the hydrogen bond between P(O)OH groups in DNA and adsorbed water, SiOH groups, or both on silica surfaces is regarded as a main factor in this adsorption. The coincidence of the pore sizes and DNA diameter realizes this unique adsorption promoted by the effect of encompassing DNA with the inner surface of mesoporous silica. Although there is no clear direct evidence for including duplex DNA in the mesopores yet, this adsorption technique is expected to provide a new tool for DNA science, because DNA in the pore size 2-5 nm in diameter has to be in unusual disentangled thread form.

Adsorption↗

PubMed2007

Preparation and evaluation of a molecularly imprinted polymer derivatized silica monolithic column for capillary electrochromatography and capillary liquid chromatography.

A method for preparation of molecularly imprinted polymer (MIP) derivatized onto the surface of a monolithic silica capillary column was successfully developed. The vinyl groups were first introduced onto the silica monolith by immobilization of gamma-methacryloxypropyltrimethoxysilane. Then the MIP coating was copolymerized and anchored onto the surface of the silica monolith. Acetonitrile was selected as porogen (solvent). The other preparation conditions, such as monomer concentration, temperature, and time of polymerization, were systematically studied. The obtained MIP-derivatized silica monolith using l-tetrahydropalmatine (l-THP) and (5S,11S)-(-)-Tröger's base (S-TB) as the imprinted template, respectively, was characterized in terms of the retention behavior of thiourea and toluene. Under the optimized CEC conditions, baseline enantioseparations of THP and TB were achieved in 4 min though the effective length of the columns was 8.5 cm. The result indicates that enough recognition sites were on the surface of silica monolith, resulting in strong recognition ability. Compared with a MIP organic monolith, the MIP-derivatized silica monolith exhibits better column efficiency and stability in CEC. Additionally, the comparison of these two kinds of monolithic columns was performed by capillary liquid chromatography. The separation on MIP-derivatized silica monolith was superior to that on the organic monolith.

Journal Article↗

PubMed2002

Is silica really an anomalous oxide? Surface acidity and aqueous hydrolysis revisited.

The single-site Solvation, Bond Strength, and Electrostatic (SBE) model accounts for the anomalous position of silica onthe surface acidity versus aqueous acidity correlation developed for metal oxides, by considering the solvation energy change in the protonation reaction implemented through the dielectric constant (1/epsilon(k)) and the electrostatic energy change through the Pauling bond strength to bond length ratio (s/r) of the oxide. I address here why inclusion of the solid's dielectric constant brings silica into the same correlation as other oxides like TiO2, Al2O3, and Fe2O3. The solvation and electrostatic contributions are interpreted in terms of classical concepts such as chemical hardness, polarizability, ionicity, electronegativity, and local charge densities. Silica is acidic (PZC < 7), not because of its small dielectric constant, its tetrahedral coordination, or its high bond strength alone. Surface acidity depends largely on high values of the s/r ratio. The dielectric constant of the solid affects acidity mainly by reflecting the nature of water-surface interactions. Solids with large values of epsilon(k) are interpreted as being less polarizable and more ionic so that water, a hard polar solvent, interacts favorably with such surfaces and scales similar to water-water interactions regardless of whether the metal-oxide bond is in the solid or in the aqueous state. For these oxides, pKa(s) = pKa(aq) +/- 1. Silica, with a small dielectric constant, is interpreted as being more polarizable and more covalent so that water-SiO2 interactions scale differently than for the more ionic oxides. Such an interpretation when combined with the Partial Charge Model for metal hydrolysis suggests that the surfaces of RuO2, W03, Sb2O5, and Ta2O5 should be acidic similar to silica. But, unlike silica, they would lie on the pKa correlation defined by the other oxides because of their larger dielectric constants. The mixed oxide, AlPO4, is predicted to behave like silica.

Hydrogen-Ion Concentration↗

PubMed2002

IR and theoretical studies of monocarbonyl Ni complexes formed by adsorption of CO at low pressure on silica-supported Ni(II) ions.

This work reports on the reactivity of coordination vacancies of Ni(II) ions grafted onto the tridentate silica support (Ni(II)(3c) ions) with respect to CO used as a probe molecule. The adsorption of CO at 77 K in the 0.3 to 3.5 Pa CO pressure range is studied by FTIR on two samples differing in the dispersion of nickel. Quantum chemical calculations by the DFT method are performed to investigate, using a cluster approach, the binding of Ni to silica and, after CO adsorption, the geometry of the resulting carbonyl Ni complexes. Silica is modeled by using clusters composed of three types of monodentate ligands, SiO(-), SiOSi and/or SiOH, found on the surface of silica. This work is devoted to the monocarbonyl complexes. Whatever the sample, only one type of monocarbonyl is formed from Ni(II)(3c) ions. It is shown that the charge of the silica cluster is the major parameter influencing the CO IR frequency whereas the nature and the size of the silica cluster do not affect the CO bond length, confirming that local electrostatic interactions predominate. Only the 1- charged silica cluster Si(5)O(3)(-), composed of SiO(-), 2SiOSi fragments, respectively, reproduces the Ni[bond]O distances derived from EXAFS for the Ni(II)(3c) grafted site and gives CO frequencies in good agreement with the experimental values. It is shown that CO is stabilized by a magnetic transition from the (3)Ni(2+) triplet to the (1)Ni(2+) singlet state occurring upon adsorption.

Journal Article↗

PubMed2005

MCM-48-like large mesoporous silicas with tailored pore structure: facile synthesis domain in a ternary triblock copolymer-butanol-water system.

Assembly of mesostructured silica using Pluronic P123 triblock copolymer (EO(20)-PO(70)-EO(20)) and n-butanol mixture is a facile synthesis route to the MCM-48-like ordered large mesoporous silicas with the cubic Iad mesostructure. The cubic phase domain is remarkably extended by controlling the amounts of butanol and silica source correspondingly. The extended phase domain allows synthesis of the mesoporous silicas with various structural characteristics. Characterization by powder X-ray diffraction, nitrogen physisorption, scanning electron microscopy, and transmission electron microscopy reveals that the cubic Iad materials possess high specific surface areas, high pore volumes, and readily tunable pore diameters in narrow distribution of sizes ranging from 4 to 12 nm. Moreover, generation of complementary pores between the two chiral channels in the gyroid Iad structure can be controlled systematically depending on synthesis conditions. Carbon replicas, using sucrose as the carbon precursor, are obtained with either the same Iad structure or I4(1)/a (or lower symmetry), depending on the controlled synthesis conditions for silica. Thus, the present discovery of the extended phase domain leads to facile synthesis of the cubic Iad silica with precise structure control, offering vast prospects for future applications of large-pore silica materials with three-dimensional pore interconnectivity.

Journal Article↗

PubMed2005

Polypeptide-templated synthesis of hexagonal silica platelets.

Several studies have demonstrated the use of biomimetic approaches in the synthesis of a variety of inorganic materials. Poly-L-lysine (PLL) promotes the precipitation of silica from a silicic acid solution within minutes. The molecular weight of PLL was found to affect the morphology of the resulting silica precipitate. Larger-molecular weight PLL produced hexagonal silica platelets, whereas spherical silica particles were obtained using low-molecular weight PLL. Here we report on the polypeptide secondary-structure transition that occurs during the silicification reaction. The formation of the hexagonal silica platelets is attributed to the PLL helical chains that are formed in the presence of monosilicic acid and phosphate ions. Hexagonal PLL crystals can also serve as templates in directing the growth of the silica in a manner that generates a largely mesoporous silica phase that is oriented with respect to the protein crystal template.

Microscopy, Electron, Scanning↗

PubMed2005

Synthesis of mesoporous carbons using ordered and disordered mesoporous silica templates and polyacrylonitrile as carbon precursor.

Mesoporous carbons were synthesized from polyacrylonitrile (PAN) using ordered and disordered mesoporous silica templates and were characterized using transmission electron microscopy (TEM), powder X-ray diffraction, nitrogen adsorption, and thermogravimetry. The pores of the silica templates were infiltrated with carbon precursor (PAN) via polymerization of acrylonitrile from initiation sites chemically bonded to the silica surface. This polymerization method is expected to allow for a uniform filling of the template with PAN and to minimize the introduction of nontemplated PAN, thus mitigating the formation of nontemplated carbon. PAN was stabilized by heating to 573 K under air and carbonized under N2 at 1073 K. The resulting carbons exhibited high total pore volumes (1.5-1.8 cm3 g(-1)), with a primary contribution of the mesopore volume and with relatively low microporosity. The carbons synthesized using mesoporous templates with a 2-dimensional hexagonal structure (SBA-15 silica) and a face-centered cubic structure (FDU-1 silica) exhibited narrow pore size distributions (PSDs), whereas the carbon synthesized using disordered silica gel template had broader PSD. TEM showed that the SBA-15-templated carbon was composed of arrays of long, straight, or curved nanorods aligned in 2-D hexagonal arrays. The carbon replica of FDU-1 silica appeared to be composed of ordered arrays of spheres. XRD provided evidence of some degree of ordering of graphene sheets in the carbon frameworks. Elemental analysis showed that the carbons contain an appreciable amount of nitrogen. The use of our novel infiltration method and PAN as a carbon precursor allowed us to obtain ordered mesoporous carbons (OMCs) with (i) very high mesopore volume, (ii) low microporosity, (iii) low secondary mesoporosity, (iv) large pore diameter (8-12 nm), and (v) semi-graphitic framework, which represent a desirable combination of features that has not been realized before for OMCs.

Acrylic Resins↗