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PubMed2000

Nitric oxide up-regulates DNA-binding activity of nuclear factor-kappaB in macrophages stimulated with silica and inflammatory stimulants.

Nitric oxide (NO), a reactive nitrogen species, plays an important role in inflammatory lung damage. In the present study, we investigated the role of NO in DNA-binding activity of NF-kappaB in macrophages stimulated with silica or other inflammatory stimulants. Treatment of mouse macrophages (RAW264.7 cells) with a selective inhibitor of inducible nitric oxide synthase (iNOS), L-N6-(1-iminoethyl) lysine (L-NIL), or a nonselective iNOS inhibitor, N omega-nitro-L-arginine methylester (L-NAME), resulted in inhibition of silica-induced nitric oxide production as well as silica-induced NF-kappaB activation. L-NIL also effectively inhibited NF-kappaB activation induced by other inflammatory stimulants, such as lipopolysaccharide (LPS) or muramyl dipeptide (MDP). These inhibitory effects of L-NIL and L-NAME on silica- or LPS-induced NF-kappaB activation were also observed in primary rat alveolar macrophages. Furthermore, NO generating compounds, such as sodium nitroprusside (SNP) and 3-morpholinosydnonimine (SIN-1), caused a dose-dependent increase in NF-kappaB activation, which was positively correlated with the level of NO production. Specific inhibitors of protein tyrosine kinase, such as genistein and AG494, prevented NF-kappaB activation in SNP- or SIN-1 treated cells, suggesting involvement of tyrosine kinase in the NO signaling pathway leading to NF-kappaB activation. In contrast, inhibitors of protein kinase C or A, such as staurosporine or H89, had no inhibitory effect on SIN-1 induced NF-kappaB activation. Metalloporphyrins, such as tetrakis (N-methyl-4'-pyridyl) porphyrinato iron (III) (Fe-TMPyP) and Zn-TMPyP which are known to alter NO-dependent activity, markedly inhibited silica- and LPS-induced NF-kappaB activation. The results suggest that NF-kappaB activation in macrophages can be induced under certain conditions by nitric oxide and that nitric oxide produced by phagocytes exposed to inflammatory agents may up-regulate the activation of NF-kappaB.

Acetylmuramyl-Alanyl-Isoglutamine↗
PubMed1990

Requirement of tumour necrosis factor for development of silica-induced pulmonary fibrosis.

The deposition of silica particles in the lung of man or experimental animals leads to silicosis, a disease of progressive respiratory failure caused by a fibrotic reaction. It has long been suspected that the phagocytosis of silica by pulmonary macrophages induces the secretion of fibrogenic factors. Several potentially fibrogenic cytokines released by macrophages have been identified, including interleukin-1 (IL-1), tumour necrosis factor-alpha (TNF), platelet-derived growth factor, basic fibroblast growth factor and transforming growth factor-beta (TGF-beta). Here we show that TNF plays an important part in silica-induced pulmonary fibrosis in mice in that (1) a single instillation of silica leads to a marked increase in the level of lung TNF messenger RNA which lasts for greater than 70 days, while there are no obvious changes in the amounts of IL-1 alpha or TGF-beta mRNAs; and (2) silica-induced collagen deposition is almost completely prevented by anti-TNF antibody, but is significantly increased by continuous infusion of mouse recombinant TNF.

Animals↗
PubMed2000

Molecular imprinting of bulk, microporous silica

Molecular imprinting aims to create solid materials containing chemical functionalities that are spatially organized by covalent or non-covalent interactions with imprint (or template) molecules during the synthesis process. Subsequent removal of the imprint molecules leaves behind designed sites for the recognition of small molecules, making the material ideally suited for applications such as separations, chemical sensing and catalysis. Until now, the molecular imprinting of bulk polymers and polymer and silica surfaces has been reported, but the extension of these methods to a wider range of materials remains problematic. For example, the formation of substrate-specific cavities within bulk silica, while conceptually straightforward, has been difficult to accomplish experimentally. Here we describe the imprinting of bulk amorphous silicas with single aromatic rings carrying up to three 3-aminopropyltriethoxysilane side groups; this generates and occupies microporosity and attaches functional organic groups to the pore walls in a controlled fashion. The triethoxysilane part of the molecules' side groups is incorporated into the silica framework during sol-gel synthesis, and subsequent removal of the aromatic core creates a cavity with spatially organized aminopropyl groups covalently anchored to the pore walls. We find that the imprinted silicas act as shape-selective base catalysts. Our strategy can be extended to imprint other functional groups, which should give access to a wide range of functionalized materials.

Journal Article↗
PubMed2001

Fragile-to-strong transition and polyamorphism in the energy landscape of liquid silica.

Liquid silica is the archetypal glass former, and compounds based on silica are ubiquitous as natural and man-made amorphous materials. Liquid silica is also the extreme case of a 'strong' liquid, in that the variation of viscosity with temperature closely follows the Arrhenius law as the liquid is cooled toward its glass transition temperature. In contrast, most liquids are to some degree 'fragile', showing significantly faster increases in their viscosity as the glass transition temperature is approached. Recent studies have demonstrated the controlling influence of the potential energy hypersurface (or 'energy landscape') of the liquid on the transport properties near the glass transition. But the origin of strong liquid behaviour in terms of the energy landscape has not yet been resolved. Here we study the static and dynamic properties of liquid silica over a wide range of temperature and density using computer simulations. The results reveal a change in the energy landscape with decreasing temperature, which underlies a transition from a fragile liquid at high temperature to a strong liquid at low temperature. We also show that a specific heat anomaly is associated with this fragile-to-strong transition, and suggest that this anomaly is related to the polyamorphic behaviour of amorphous solid silica.

Journal Article↗
PubMed2001

Ultrafast holographic nanopatterning of biocatalytically formed silica.

Diatoms are of interest to the materials research community because of their ability to create highly complex and intricate silica structures under physiological conditions: what these single-cell organisms accomplish so elegantly in nature requires extreme laboratory conditions to duplicate-this is true for even the simplest of structures. Following the identification of polycationic peptides from the diatom Cylindrotheca fusiformis, simple silica nanospheres can now be synthesized in vitro from silanes at nearly neutral pH and at ambient temperatures and pressures. Here we describe a method for creating a hybrid organic/inorganic ordered nanostructure of silica spheres through the incorporation of a polycationic peptide (derived from the C. fusiformis silaffin-1 protein) into a polymer hologram created by two-photon-induced photopolymerization. When these peptide nanopatterned holographic structures are exposed to a silicic acid, an ordered array of silica nanospheres is deposited onto the clear polymer substrate. These structures exhibit a nearly fifty-fold increase in diffraction efficiency over a comparable polymer hologram without silica. This approach, combining the ease of processability of an organic polymer with the improved mechanical and optical properties of an inorganic material, could be of practical use for the fabrication of photonic devices.

Amino Acid Sequence↗
PubMed2004

Enzyme immobilization in a biomimetic silica support.

Robust immobilization techniques that preserve the activity of biomolecules have many potential applications. Silicates, primarily in the form of sol-gel composites or functionalized mesoporous silica, have been used to encapsulate a wide variety of biomolecules but the harsh conditions required for chemical synthesis limit their applicability. Silaffin polypeptides from diatoms catalyze the formation of silica in vitro at neutral pH and ambient temperature and pressure. Here we show that butyrylcholinesterase entrapped during the precipitation of silica nanospheres retained all of its activity. Ninety percent of the soluble enzyme was immobilized, and the immobilized enzyme was substantially more stable than the free enzyme. The mechanical properties of silica nanospheres facilitated application in a flow-through reactor. The use of biosilica for enzyme immobilization combines the excellent support properties of a silica matrix with a benign immobilization method that retains enzyme activity.

Adsorption↗
PubMed1988

Stimulation of surfactant phospholipid biosynthesis in the lungs of rats treated with silica.

The effects of intratracheally instilled silica (10 mg/rat) on the biosynthesis of surfactant phospholipids was investigated in the lungs of rats. The sizes of the intracellular and extracellular pools of surfactant phospholipids were measured 7, 14 and 28 days after silica exposure. The ability of lung slices to incorporate [14C]choline and [3H]palmitate into surfactant phosphatidylcholine (PC) and disaturated phosphatidylcholine (DSPC) was also investigated. Both intra- and extra-cellular pools of surfactant phospholipids were increased by silica treatment. The intracellular pool increased linearly over the 28-day time period, ultimately reaching a size 62-fold greater than controls. The extracellular pool also increased, but showed a pattern different from that of the intracellular pool. The extracellular pool increased non-linearly up to 14 days, and then declined. At its maximum, the extracellular pool was increased 16-fold over the control. The ability of lung slices to incorporate phospholipid precursors into surfactant-associated PC and DSPC was elevated at all time periods. The rate of incorporation of [14C]choline into surfactant PC and DSPC was maximal at 14 days and was nearly 3-fold greater than the rate in controls. The rate of incorporation of [3H]palmitate was also maximal at 14 days, approx. 5-fold above controls for PC and 3-fold for DSPC. At this same time point, the microsomal activity of cholinephosphate cytidylyltransferase was increased 4.5-fold above controls, but cytosolic activity was not significantly affected by silica treatment. These data indicate that biosynthesis of surfactant PC is elevated after treatment of lungs with silica and that this increased biosynthesis probably underlies the expansion of the intra- and extra-cellular pools of surfactant phospholipids.

Animals↗
PubMed1989

Characterization of phospholipids accumulated in pulmonary-surfactant compartments of rats intratracheally exposed to silica.

Phospholipids in the lung fractions, i.e. alveolar free cells, extracellular pulmonary surfactant, intracellular pulmonary surfactant (lamellar bodies) and microsomal fractions, of rats were examined 28 days after intratracheal injection of silica (40 mg/kg). Significant accumulations of phospholipids were observed in the extracellular- and intracellular-surfactant fractions of rats exposed to silica. The prominent phospholipid accumulated was phosphatidylcholine (PC), consisting mainly of the dipalmitoyl species. However, a compositional change in acidic phospholipids of surfactant fractions was produced by the silica treatment. The percentage of phosphatidylglycerol (PG) was significantly decreased; in contrast, that of phosphatidylinositol (PI) was increased. Thus the ratio PG/PI in the surfactant fractions was markedly decreased in response to silica. This compositional change in both acidic phospholipids occurred even in the early stages, i.e. before appreciable accumulations of alveolar phospholipids were noticed. The molecular-species profiles of both acidic phospholipids in the surfactant fractions were distinctly different from each other. The dipalmitoyl species accounted for more than 30% of PG and less than 6% of PI, respectively. These species patterns of PG and PI were similar in control and silica-treated rats. These findings suggest two possibilities that (1) PG and PI destined for pulmonary surfactant are synthesized from each specific CDP-diacylglycerol (DG) pool having different molecular species in the lung, or (2) individual enzymes responsible for synthesis of surfactant PG and PI have substrate specificities for molecular species of CDP-DG, thereby producing PG and PI having different molecular species in surfactant compartments.

Animals↗
PubMed2006

Effects of silica coating and silane surface conditioning on the bond strength of metal and ceramic brackets to enamel.

OBJECTIVE: To evaluate the effect of tribochemical silica coating and silane surface conditioning on the bond strength of metal and ceramic brackets bonded to enamel surfaces with light-cured composite resin. MATERIALS AND METHODS: Twenty metal and 20 ceramic brackets were divided into four groups (n = 10 for each group). The specimens were randomly assigned to one of the following treatment conditions of the metal and ceramic brackets' surface: (1) tribochemical silica coating combined with silane and (2) no treatment. Brackets were bonded to the enamel surface on the labial and lingual sides of human maxillary premolars (20 total) with a light-polymerized resin composite. All specimens were stored in water for 1 week at 37 degrees C and then thermocycled (5000 cycles, 5 degrees C to 55 degrees C, 30 seconds). The shear bond strength values were measured on a universal testing machine. Student's t-test was used to compare the data (alpha = 0.05). The types of failures were observed using a stereomicroscope. RESULTS: Metal and ceramic brackets treated with silica coating with silanization had significantly greater bond strength values (metal brackets: 14.2 +/- 1.7 MPa, P < .01; ceramic brackets: 25.9 +/- 4.4 MPa, P < .0001) than the control groups (metal brackets: 11.9 +/- 1.3 MPa; ceramic brackets: 15.6 +/- 4.2 MPa). Treated specimens of metal and ceramic exhibited cohesive failures in resin and adhesive failures at the enamel-adhesive interface, whereas control specimens showed mixed types of failures. CONCLUSIONS: Silica coating with aluminum trioxide particles coated with silica followed by silanization gave higher bond strengths in both metal and ceramic brackets than in the control group.

Adhesiveness↗
PubMed1999

Urinary retention in two male dromedaries due to silica uroliths.

Two cases of urinary retention in male dromedaries due to silica uroliths are presented. The animals were urethrostomized and one dromedary was euthanized 7 months later due to urethrostomy obstruction. The estimated daily intake of silica was 84.44 g. Silica, calcium, phosphorus and pH in urine were determined in healthy animals from the same farms, and the following values were obtained: 174.78 +/- 3.46 mg/l (silica), 41.48 +/- 4.82 mg/l (calcium), 20.4 +/- 3.6 mg/l (phosphorus) and pH 8.2, respectively. Possible causes of urolithiasis were the early castration of the animals and the fact that salt was not added to the diet. To our knowledge, this is the first description of silica urolithiasis in the dromedary camel.

Animal Feed↗
PubMed2004

Water-soluble silica-overcoated CdS:Mn/ZnS semiconductor quantum dots.

Highly luminescent and photostable CdS:Mn/ZnS core/shell quantum dots are not water soluble because of their hydrophobicity. To create water-soluble quantum dots by an appropriate surface functionalization, CdS:Mn/ZnS quantum dots synthesized in a water-in-oil (W/O) microemulsion system (reverse micelles) were consecutively overcoated with a very thin silica layer ( approximately 2.5 nm thick) within the same reverse micellar system. The water droplet serves as a nanosized reactor for the controlled hydrolysis and condensation of a silica precursor, tetraethyl orthosilicate (TEOS), using an ammonium hydroxide (NH4OH) catalyst. Structural characterizations with transmission electron microscopy (TEM) and x-ray photoelectron spectroscopy (XPS) indicate that the silica-quantum dot nanocomposites consist of a layered structure. Owing to the amorphous, porous nature of a silica layer, the optical and photophysical properties of silica-overcoated CdS:Mn/ZnS quantum dots are found to remain close to those of uncoated counterparts.

Journal Article↗
PubMed2005

Fractal dimensions of silica gels generated using reactive molecular dynamics simulations.

We have used molecular dynamics simulations based on a three-body potential with charge transfer to generate nanoporous silica aerogels. Care was taken to reproduce the sol-gel condensation reaction that forms the gel backbone as realistically as possible and to thereby produce credible gel structures. The self-similarity of aerogel structures was investigated by evaluating their fractal dimension from geometric correlations. For comparison, we have also generated porous silica glasses by rupturing dense silica and computed their fractal dimension. The fractal dimension of the porous silica structures was found to be process dependent. Finally, we have determined that the effect of supercritical drying on the fractal nature of condensed silica gels is not appreciable.

Journal Article↗
PubMed2006

Novel nanocomposites from spider silk-silica fusion (chimeric) proteins.

Silica skeletal architectures in diatoms are characterized by remarkable morphological and nanostructural details. Silk proteins from spiders and silkworms form strong and intricate self-assembling fibrous biomaterials in nature. We combined the features of silk with biosilica through the design, synthesis, and characterization of a novel family of chimeric proteins for subsequent use in model materials forming reactions. The domains from the major ampullate spidroin 1 (MaSp1) protein of Nephila clavipes spider dragline silk provide control over structural and morphological details because it can be self-assembled through diverse processing methods including film casting and fiber electrospinning. Biosilica nanostructures in diatoms are formed in aqueous ambient conditions at neutral pH and low temperatures. The R5 peptide derived from the silaffin protein of Cylindrotheca fusiformis induces and regulates silica precipitation in the chimeric protein designs under similar ambient conditions. Whereas mineralization reactions performed in the presence of R5 peptide alone form silica particles with a size distribution of 0.5-10 microm in diameter, reactions performed in the presence of the new fusion proteins generate nanocomposite materials containing silica particles with a narrower size distribution of 0.5-2 microm in diameter. Furthermore, we demonstrate that composite morphology and structure could be regulated by controlling processing conditions to produce films and fibers. These results suggest that the chimeric protein provides new options for processing and control over silica particle sizes, important benefits for biomedical and specialty materials, particularly in light of the all aqueous processing and the nanocomposite features of these new materials.

Amino Acid Sequence↗
PubMed1998

Atmospheric weathering and silica-coated feldspar: analogy with zeolite molecular sieves, granite weathering, soil formation, ornamental slabs, and ceramics.

Feldspar surfaces respond to chemical, biological, and mechanical weathering. The simplest termination is hydroxyl (OH), which interacts with any adsorption layer. Acid leaching of alkalis and aluminum generated a silica-rich, nanometers-thick skin on certain feldspars. Natural K, Na-feldspars develop fragile surfaces as etch pits expand into micrometer honeycombs, possibly colonized by lichens. Most crystals have various irregular coats. Based on surface-catalytic processes in molecular sieve zeolites, I proposed that some natural feldspars lose weakly bonded Al-OH (aluminol) to yield surfaces terminated by strongly bonded Si-OH (silanol). This might explain why some old feldspar-bearing rocks weather slower than predicted from brief laboratory dissolution. Lack of an Al-OH infrared frequency from a feldspar surface is consistent with such a silanol-dominated surface. Raman spectra of altered patches on acid-leached albite correspond with amorphous silica rather than hydroxylated silica-feldspar, but natural feldspar may respond differently. The crystal structure of H-exchanged feldspar provides atomic positions for computer modeling of complex ideas for silica-terminated feldspar surfaces. Natural weathering also depends on swings of temperature and hydration, plus transport of particles, molecules, and ionic complexes by rain and wind. Soil formation might be enhanced by crushing granitic outcrops to generate new Al-rich surfaces favorable for chemical and biological weathering. Ornamental slabs used by architects and monumental masons might last longer by minimizing mechanical abrasion during sawing and polishing and by silicifying the surface. Silica-terminated feldspar might be a promising ceramic surface.

Journal Article↗
PubMed2002

An evaluation of compliance with occupational exposure limits for crystalline silica (quartz) in ten Georgia granite sheds.

Since the 1920s, industrial hygiene studies have documented granite shed workers' exposures to crystalline silica, and the data from these studies have contributed to a better understanding of the relationship between silica exposures and adverse health effects, such as silicosis. The majority of these studies were conducted in the Barre, Vermont, granite sheds. However, a second major granite processing region is located in Elberton, Georgia, where approximately 1800 workers are employed in 150 granite sheds and 45 quarries. The current study reports the exposures of 40 workers in 10 granite sheds in Elberton, Georgia. The arithmetic mean exposure to silica for all monitored employees was 0.052 mg/m3. Employees were classified into one of seven job task groups. The job task group with the greatest exposure was the top polish group, which had a mean exposure of 0.085 mg/m3. Among the top polish workers, the greatest percentage of exposures above the Occupational Safety and Health Administration's permissible exposure limit (OSHA PEL) occurred among the workers who used dry grinders. Wet methods were effective in reducing these exposures to below the OSHA PEL. The mean exposure of Elberton granite shed workers was less than the OSHA PEL, but was not below the threshold limit value of the American Conference of Industrial Hygienists (ACGIH TLV), which was lowered in the year 2000 to 0.05 mg/m3. The Elberton granite shed workers provide a valuable cohort for research on the effects of exposure to crystalline silica at levels between the ACGIH TLV and the OSHA PEL. They are a relatively permanent worker population, are concentrated geographically, and have a quantitatively documented exposure to crystalline silica over the past twenty years.

Environmental Monitoring↗
PubMed1990

Role of free radicals in the mechanisms of hemolysis and lipid peroxidation by silica: comparative ESR and cytotoxicity studies.

Electron spin resonance (ESR) and cytotoxicity measurements were made on newly fractured silica to examine specifically the role of the fracture-induced, silicon-based radicals (Si. and SiO.) and silica-generated hydroxyl (.OH) radicals in the mechanism of the cell membrane damage by silica. The concentration of the Si. and SiO. radicals was controlled through decay processes, thermal annealing, and boiling, while that of the .OH radicals was varied by using catalase, superoxide dismutase, KMnO4, Na2SeO3, ascorbic acid, and metal ions, and monitored via ESR spectroscopy. The dust's cytotoxicity potential was evaluated by measuring the silica-induced hemolysis and also by determining lipid peroxidation (using linoleic acid). From the comparison of hemolysis and ESR results it is deduced that the radicals play little or no role in the silica-induced hemolysis. However, the lipid peroxidation data indicate that the radicals might be involved in the initiation of an oxidative chain reaction leading to the macrophage membrane damage through lipid peroxidation.

Animals↗
PubMed1992

Silica-induced pulmonary inflammation and fibrosis in mice is altered by acute exposure to nitrogen dioxide.

The biologic impact of consecutive exposures to two environmental pollutants was examined in mice exposed to silica crystals (SI) by intratracheal (IT) injection followed by an inhalation exposure to nitrogen dioxide (NO2). C57Bl/6 mice received an IT injection of 2 mg SI or sterile saline (SAL) followed by a 2-h inhalation exposure to NO2 at 20 ppm either within 2 h of or 24 h after SI instillation. During acute inflammation (d 3 postsilica), mice exposed to NO2 at either time showed a dramatic and significant reduction in the number of lavaged alveolar neutrophils (PMN) when compared to silica/air-exposed mice. Animals exposed to NO2 24 h after silica also evidenced significant decreases in levels of lavage albumin and lactate dehydrogenase (LDH) 3 d after silica, as well as significant decreases in hydroxyproline content of the lung 30 and 60 d postsilica injection when compared to silica/air-exposed animals. NO2 administration 24 h after silica appeared to shift the appearance of PMN in the lung from d 3 to d 14, but did not otherwise alter chronic cellular inflammation. These data suggest that the marked neutrophil response and collagen deposition induced by SI can be modulated by NO2 exposure and that the time of oxidant gas exposure after silica administration is critical to this modulation.

Acute Disease↗
PubMed1982

Evaluation of occupational exposure to free silica in Alberta foundries.

The Occupational Hygiene Branch of Alberta Workers' Health, Safety and Compensation conducted a comprehensive study of the foundry industry in Alberta. The surveys assessed both the degree of health hazards present and the effectiveness of existing control systems for airborne contaminants. All nine of Alberta's ferrous foundries were surveyed in the course of the project. The foundries varied from those which were small with limited mechanization to those which were large and highly automated. The concentrations of free silica in the work environment are correlated to the different attempts to control silica using substitution and various ventilation systems. The particular foundry processes evaluated for airborne free silica were sand preparation, shakeout, dry sand transport and sand molding. Workers' exposure to free airborne silica was evaluated by personal and area samples. The free silica content of the samples was determined by infra-red spectrophotometry. The results indicated most control systems were inadequate. Effective control methods are described to reduce the health hazard.

Alberta↗