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1.
《Applied Geochemistry》2000,15(7):1043-1051
This study presents and discusses groundwater colloid results from various geological formations ranging from crystalline to sedimentary, from organic rich to organic poor systems and from subsurface to very deep aquifers. Colloid presence and their potential mobility are justified on the basis of colloid stability properties in the investigated groundwaters. The colloid concentration is a function of pH, redox potential, concentrations of Na, K, Ca, Mg and organic carbon, as well as the status of the chemical and physical steady state of the hydrogeochemical system. The colloid properties are discussed with a non-site specific approach.  相似文献   

2.
Particle size distributions and the mineralogy of inorganic colloids in waters draining the adit of an abandoned mine (Goesdorf, Luxembourg) were quantified by single particle counting based on light scattering (100 nm–2 μm) combined with transmission electronic microscopy coupled with energy dispersive spectroscopy and selected area electron diffraction. This water system was chosen as a surrogate for groundwaters. The dependence of the colloid number concentration on colloid diameters can be described by a power-law distribution in all cases. Power-law slopes ranged from −3.30 to −4.44, depending on water ionic strength and flow conditions. The same main mineral types were found in the different samples: 2:1 phyllosilicates (illite and mica), chlorite, feldspars (albite and orthoclase), calcite and quartz; with a variable number of Fe oxide particles. The colloid mineralogical composition closely resembles the composition of the parent rock. Spatial variations in the structure and composition of the rock in contact with the waters, i.e. fissured rock versus shear joints, are reflected in the colloid composition. The properties of the study colloids, as well as the processes influencing them, can be considered as representative of the colloids present in groundwaters.  相似文献   

3.
The environmental behaviour of colloidal clay in aquatic systems is linked to the properties of their aggregates. Earlier investigations of clay colloids were performed with electron microscope techniques which caused de-hydration of the particles. Information on the structure of colloid aggregates is needed for understanding their sedimentation behaviour, as well as colloid contaminant transport properties in natural systems. Scanning transmission X-ray microspectroscopy successfully produced images of montmorillonite colloid aggregates in a pseudo-equilibrium state in 1 mM NaCl suspensions equilibrated for more than a year. These clay aggregates were revealed at photon energies below the O absorption edges of clay and water. They were spherical or ellipsoidal with diameters of the order of 100–800 nm. The aggregates are porous and gel like with lower densities than the clay mineral. These investigations are important for modelling the occurrence of clay aggregates in aqueous environments.  相似文献   

4.
The spread of radioactive contamination in the subsurface medium near Lake Karachai is considered. The complexity of this process requires a comprehensive approach to its study. The source of radioactive contamination is overviewed. The map of faults in subsurface medium is considered in order to determine the prevailing direction of contaminated groundwater flow. Photometry in observation wells has been used for structural geological estimation of transport properties of the shallow aquifer, where contaminated groundwater is moving. This study was carried out along with hydrochemical logging, which makes it possible to estimate the dynamics of contamination of subsurface medium and vertical distribution of groundwater contamination. Special attention is paid to transport of radionuclides in the form of radiocolloid particles. Groundwater samples were taken from various depths corresponding to different contamination levels near Lake Karachai. The depth intervals of sampling were determined from the data of hydrochemical logging. Ultrafiltration through membranes with a specific pore size in combination with gamma spectrometry was used to characterize radionuclide transfer with colloidal particles differing in size. The local elemental composition of the radiocolloid surface was studied by Auger spectroscopy. The chemical composition and structure of radiocolloid particles were determined by X-ray photoelectron spectroscopy with consecutive etching of the particle surface by argon ions for a certain depth. The data obtained indicate that radiocolloid particles are heterogeneous and an organic shell consisting of humic and fulvic acids and technogenic organic compounds coat their surface.  相似文献   

5.
《Applied Geochemistry》1991,6(5):565-574
Natural colloids (1–450 nm) and suspended particles (>450 nm) were characterized in groundwaters of the Whiteshell Research Area of southern Manitoba to evaluate their potential role in radionuclide transport through fractured granite. Data on particle concentrations, size distributions, compositions and natural radionuclide content were collected to predict radionuclide formation and to provide a database for future colloid migration studies. The concentrations of colloids between 10 and 450 nm ranged between 0.04 and 1 mg/l. The concentrations of suspended particles, which require higher groundwater velocities for transport, varied from 0.04 to 14 mg/l. Colloid (10–450 nm) concentrations as low as these observed in Whiteshell Research Area groundwater would have a minimal effect on radionuclide transport, assuming that radionuclide sorption on colloids is reversible. If radiocolloid formation is not reversible, and radionuclide-containing colloids cannot sorb onto fracture walls, the importance of natural colloids in radionuclide transport will depend upon particle migration properties.  相似文献   

6.
Natural colloids have a potential role in facilitating the transport of radionuclides in groundwater. To assess the role of mobile colloidal phases in radionuclide transport, characterization of colloids for size, size distribution, zeta potential, surface charge and elemental composition is required. Groundwater samples were collected from 12 borewells in the study area and were characterized with respect to physicochemical parameters. Water quality parameters such as pH, temperature, specific conductance, TDS and dissolved O2 were measured in situ. Based on salinity, two groundwater types were identified in the study area: (1) freshwater type and (2) brackish type. Laboratory and field-scale turbidity measurements in addition to quantitative analysis of major ions were carried out. It was observed that the colloid concentrations are reduced at higher salinity. Zetasizer, particle size analyzer, scanning electron microscopy, energy dispersive X-ray analysis and X-ray diffraction techniques were used to characterize the colloidal particles in groundwater. Colloids were present in all the groundwater samples, the concentration varying between 0.05 and 6 mg/L. Colloid concentration was greater in wells with low ionic strength and the number of colloidal particles varied between 3 × 109 and 4 × 1011 particles/L. The average colloid size varied between 200 and 350 nm for various samples. The zeta potential of the colloidal particles varied between −25.5 and –34.0 mV. SEM analysis of colloidal particles revealed the presence of clays particularly kaolinite and that the mineral composition of colloids reflects the mineralogy of the aquifer. For proper risk assessment and remediation studies, the role of colloids in radionuclide transport assumes greater importance. This study highlights the need for, and relevance of, detailed colloid characterization to assess its role in the migration of radionuclides from near surface disposal facilities.  相似文献   

7.
紫色土坡地泥岩裂隙潜流中的胶体迁移   总被引:1,自引:0,他引:1       下载免费PDF全文
为探求自然胶体迁移进入地下水的潜力,建立原位坡地径流观测场,研究了2013年夏季3场不同雨型降雨事件下,紫色土坡地(1 500 m2)泥岩裂隙潜流中自然胶体的迁移规律。结果表明:裂隙潜流中胶体对降雨的响应时间为30~90 min,比潜流对降雨的响应更迅速,且取决于坡地雨前干旱情况及降雨强度;胶体浓度峰早于潜流流量峰,峰值浓度相对背景浓度可增加1~2个数量级,最大雨强及雨型决定潜流流量和胶体浓度峰型。气液界面是胶体初始迁移响应的主要驱动因素,雨水混合土壤前期水对土壤介孔和大孔内壁胶体的剪切、裹携是胶体释放、分散与迁移的主要机制。因此,胶体辅助运移可能成为紫色土地区吸附性较强的污染物(如磷、疏水性农药等)的重要迁移方式。  相似文献   

8.
《Applied Geochemistry》2002,17(5):633-648
Acid rock drainage (ARD) solution from an abandoned ore mine (pH 2.7, SO2−4 concentration 411 mmol/l, Fe concentration 93.5 mmol/l) was investigated by photon correlation spectroscopy, centrifugation, filtration, ultrafiltration, scanning electron microscopy, ICP–MS, AAS, ion chromatography, TOC analysis, and extended X-ray absorption fine structure (EXAFS) spectroscopy. A colloid concentration of ⩾1 g/l was found. The prevailing particle size was <5 nm. Iron, As and Pb were the metal constituents of the colloidal particles. The most probable mineralogical composition of the particles is a mixture of hydronium jarosite and schwertmannite. A small amount of a relatively coarse precipitate was formed in the ARD solution during the months after sampling. The colloid particles are obviously an intermediate in the precipitate formation process. The results suggest that the arsenate is bound to the colloids by the formation of a bidentate binuclear inner-sphere surface complex. However, the transformation of the colloidal material to the more aggregated long-term precipitate results in the incorporation of the arsenate into the interior of the Fe hydroxy sulfate crystal structures. Lead seems to occur as anglesite.  相似文献   

9.
土体固化的核心问题之一就是使用适宜的固化剂固化黏土矿物。通过扫描电镜(SEM)、傅里叶红外光谱(FTIR)、X射线衍射(XRD)以及X射线光电子能谱(XPS)等试验方法,研究不同碱含量下碱激发地聚物固化的蒙脱石、伊利石和高岭土的微观结构、物质组成及物理化学反应过程,探究碱激发地聚物与黏土矿物之间的相互作用机理。研究结果表明:黏土矿物经碱激发地聚物固化后,由松散颗粒转变为块状致密结构;随着地聚物中碱含量的增加,Si、Al及Ca元素电子结合能下降;蒙脱石在衍射角为5°左右(001)峰形右移,层间距减小;蒙脱石吸附水含量减小,亲水能力下降,矿物活性被限制。  相似文献   

10.
《Applied Geochemistry》1995,10(2):119-131
In the framework of nuclear waste topics, the role of colloids is more and more emphasized in relation to the transport of radioelements in natural groundwaters. We attempt here to check if the nature and physico-chemical characteristics of the colloids from the granitic site of El Berrocal are closely related to the bedrock composition.The colloids are studied in three types of groundwaters (sulfate and carbonate waters in different redox conditions) as well as colloidal suspensions extracted from clayey materials present in the fractures. The particle size distributions are performed by photon correlation spectroscopy. Their chemical composition is obtained by X-ray microanalysis after transversal ultrafiltration.The main results deal with the chemical composition of colloids. They are mainly composed of silica, aluminosilicate phases, and Fe, Ti, Al oxyhydroxides. In the case of the carbonate and oxidized hydrofacies, traces of Mg, Cu, Zn, Ba, S as well as carbonate phases (Zn, Ca) occur. In the particular case of the sulfate hydrofacies, traces of S, Mg, Cu are identified. Finally in the less oxidized and carbonate groundwater, a lot of phases consist of sulphur with Cu, Zn, Fe as well as of carbonate with Cu, Zn, Fe, Ca and Mg. For the clayey suspensions, colloids are mainly composed of illite and silica.In conclusion, the contribution of the bedrock as well as the influence of the physico-chemical conditions are discussed in order to decipher the role of neoformation and dispersion processes in the colloid formation.  相似文献   

11.
We investigated Fe(III)-precipitates formed from Fe(II) oxidation in water at pH 7 as a function of dissolved Fe(II), As(III), phosphate, and silicate in the absence and presence of Ca. We used transmission electron microscopy (TEM), including selected area electron diffraction (SAED) and energy dispersive X-ray spectroscopy (EDX) to characterize the morphology, structure and elemental composition of the precipitates. Results from our companion X-ray absorption spectroscopy (XAS) study suggested that the oxidation of Fe(II) leads to the sequential formation of distinct polymeric units in the following order: Fe(III)-phosphate oligomers in the presence of phosphate, silicate-rich hydrous ferric oxide (HFO-Si) at high Si/Fe (>0.5) or 2-line ferrihydrite (2L-Fh) at lower Si/Fe (∼0.1-0.5), and lepidocrocite (Lp) in the absence of phosphate at low Si/Fe (<0.1). Results from this study show that the size of the polymeric units increased along the same sequence and that the aggregation of these polymeric units resulted in spherical particles with characteristic surface textures changing from smooth to coarse. The diameter of the spherical particles increased from 15 to 380 nm as the molar ratio (P + Si + As)/Fe(II) in the starting solution decreased and larger spherical particles precipitated from Ca-containing than from Ca-free solutions. These trends suggested that the size of the spherical particles was controlled by the charge of the polymeric units. Spherical particles coagulated into flocs whose size was larger in the presence than in the absence of Ca. Further observations pointed to the importance of Fe(II) oxidation and polymerization versus polymer aggregation and floc formation kinetics in controlling the spatial arrangement of the different polymeric units within Fe(III)-precipitates. The resulting structural and compositional heterogeneity of short-range-ordered Fe(III)-precipitates likely affects their colloidal stability and their chemical reactivity and needs to be considered when addressing the fate of co-transformed trace elements such as arsenic.  相似文献   

12.
The concentration and the role of colloids in the transport of elements in the vicinity of a fossil reactor at Bangombé, Gabon, were assessed. Colloid sampling was conducted in seven boreholes around and in the extinguished natural reactor. The ground waters are of Na–Mg–Ca–HCO3 type, with variable salinities, pH 4.6–6.8 and anaerobic Eh values. Filtered ground water and colloid samples were taken from the reactor and the surroundings. Filtered fluids and colloid samples collected on membranes and resuspended in solution were analysed by ICP-MS and ICP-AES in order to examine the element association in the colloid phase within the size range 3000 to 400 to 50 nm. The colloid concentrations for the size 400 to 50 nm range from 80 to 300 ng ml−1. They consist of silica particles associated with ferrihydrite coated with organics. Trace element results show that metals including Pb, Sc, Y, La, Ce, Pr, Nd, Bi, Th and U are associated to various degrees with the colloid phase. The distribution ratios of these trace elements between the water and the colloid phase (Kp) were experimentally determined. The high Pb distribution ratios of 10+7 ml g−1 are specifically discussed. Values range from 10+6 to 10+5 ml g−1for the trivalent elements (Sc, Y, La, Ce,  , Bi). For uranium, a Kp of the order of 10+5 ml g−1 may be calculated and compared with data gained using the surface complexation model. These Kp values suggest that the uranium is partially sorbed or associated with ground water colloids. Measurements from the reactor zone show that about 2–4% of the uranium is associated with the colloid phase, which contributes partially to the uranium transport. The rather low colloid concentrations are due to the relatively high concentrations of Ca, Mg and Na in these quasi-neutral waters. These soluble elements contribute to the attachment of the colloids, restricting their transport. This indicates that the colloid phase may not be an important transport medium for the radionuclides in the Bangombé system if their association is reversible. The Bangombé colloid results are compared with those studied for other systems.  相似文献   

13.
Data are presented on suspended particles and colloids in groundwaters from the Osamu Utsumi mine and the Morro do Ferro analogue study sites. Cross-flow ultrafiltration with membranes of different pore sizes (450 nm to 1.5 nm) was used to prepare colloid concentrates and ultrafiltrates for analyses of major and trace elements and U- and Th-isotopic compositions. Additional characterization of colloidal and particulate material was performed by ESCA, SEM and X-ray diffraction. The results indicate the presence of low concentrations of colloids in these waters (typically < 500 μg/l), composed mainly of iron/organic species. Minor portions of uranium and other trace elements, but significant fractions of the total concentrations of Th and REE in prefiltered waters (< 450 nm) were associated with these colloids.Suspended particles (> 450 nm), also composed mainly of hydrous ferric oxides and humic-like compounds, show the same trend as the colloids with respect to U, Th and REE associations, but elemental concentrations were typically higher by a factor of 1,000 or more. In waters of low pH and with high sulphate content, these associations are considerably lower. Due to the low concentrations of suspended particles in groundwaters from the Osamu Utsumi uranium mine (typically <0.5 mg/l), these particles carry only a minor fraction of U and the REE (<10% of the total concentrations in unfiltered groundwaters), but a significant, usually predominant fraction of Th (30–70%). The suspended particle load in groundwaters from the Morro do Ferro environment is typically higher than in those from the mine by a factor of 5 to 10. This suggests that U, Th and the REE could be transported predominantly by particulate matter. However, these particles and colloids seem to have a low capacity for migration.  相似文献   

14.
The colloidal fractions of various particle sizes were separated from the samples of groundwater in the area of radioactive contamination nearby Obninsk (Kaluga region, Russia). The primary component of the radioactive contamination is 90Sr isotope. The colloidal particles were separated from the samples of groundwater by means of ultrafiltration through membranes of 200, 100, and 25 nm pore sizes. The chemical composition of particle surfaces in each of the fractions was determined using X-ray photoelectron spectroscopy. The structure of particles was determined by the changes in the surface composition after the removal of outer layers of particles by etching with argon ions to a depth of 100 Å. It was found that the particles are constituted by inorganic cores mainly of montmorillonite and iron metahydroxide and a broken covering of humic acids. It was shown that about 50% of 90Sr is transferred by groundwater with colloidal particles of over 25 nm in size.  相似文献   

15.
《Applied Geochemistry》1993,8(6):605-616
The Cigar Lake U deposit is located in northern Saskatchewan in the eastern part of the Athabasca Sandstone Basin, and consists of a high-grade ore body (up to 55% U) located at a depth of ∼430 m. As part of a study to evaluate the analog features of this deposit with respect to a disposal vault for waste nuclear fuel, colloids (1–450 nm) and suspended particles (450nm) in groundwater have been investigated to evaluate their effect on element transport through the U deposit. Tangential-flow ultrafiltration was used to concentrate particles from 501 groundwater samples in order to characterize the size distribution, concentration, composition and natural radionuclide content of particles in representative parts of the U deposit. Although Cigar Lake groundwaters contain particles in all sizes ranging from 10 nm to slightly larger than 20 μm, most samples contained a relatively high concentration of colloids in the 100–400 nm size range. Particle compositions are similar to the composition of minerals in the sandstones and ore body, suggesting that particles in groundwater are generated by the erosion of fracture-lining minerals. As a result, particle concentrations in groundwater are affected by the integrity of the host rock. In some piezometers the high initial concentrations of suspended particles, which may have been drilling artifacts, decreased during the collection of the first 350 1. Although colloid concentrations fluctuated during sampling, there are no indications that these concentrations will be permanently reduced by continued groundwater pumping. The observed colloid and suspended particle concentrations in the deep groundwaters are too low to have a significant impact on radionuclide migration, provided that radionuclide sorption is reversible. If radionuclides are irreversibly sorbed to particles they cannot sorb to the host rock and their migration can only be evaluated with an understanding of particle mobility. The data for dissolved and particulate U, Th and Ra were used to calculate field-derived distribution ratios (Rd) between particles and groundwater. The wide range of observed Rd values indicates that these radionuclides in particulate form are not in equilibrium with groundwater. U-series isotope data indicated that most of the U and Ra on particles was derived from groundwater. Some particles could have retained their U for as long as 8000 a. The U and Ra contents of particles in the ore and surrounding clay zones are significantly higher than in particles from sandstone, suggesting that the clay has been an effective barrier to particle migration.  相似文献   

16.
选取8例乳腺纤维腺瘤的钙化样品,利用光学显微镜(OM)、环境扫描电镜(ESEM)、高分辨透射电镜(HR-TEM)、显微红外光谱仪(FTIR)、微区X射线衍射等矿物学方法对样品进行了原位和分离后形貌、结构及成分的测试分析,探讨了病灶中钙化的矿物学特征,初步探讨了钙化的组成及形成机理。研究结果表明,乳腺纤维腺瘤中的钙化是由病变后期玻璃样变性胶原中的羟基和羧基为钙化提供了成核位点,伴随病情发展最后形成OM下可见的以羟磷灰石为主要成分的坏死钙化。  相似文献   

17.
This paper discusses the formation of whiting events, drifting milky clouds of water, and their role in the formation of recent aragonite sediments in a semi-enclosed, karstic, marine lake on the island of Mljet (Adriatic Sea). This study is based on detailed structural, morphological and sedimentological characterization of, and strontium distribution in, particles originating from suspended matter and sediments. The particles were examined by X-ray diffraction and electron diffraction analyses, scanning and transmission electron microscopy, as well as electron microprobe energy dispersive X-ray analyses and atomic absorption spectroscopy. Morphological features, granulometric characteristics, strontium enrichment and characteristic details of the aragonite structure in the needle-like particles were identical in both the suspended matter collected during whiting events and in the bottom sediments. The whiting events, which occasionally occurred in surface waters, were found to be sites of short-term active authigenic aragonite precipitation and the main source of fine-grained aragonite mud. This study exemplifies the role of biologically induced inorganic precipitation processes in the formation of recent aragonite mud in a restricted Mediterranean environment.  相似文献   

18.
We used X-ray absorption spectroscopy at the Al K-edge to investigate the atomic structure of biogenic silica and to assess the effect of Al on its crystal chemistry. Our study provides the first direct evidence for a structural association of Al and Si in biogenic silica. In samples of cultured diatoms, Al is present exclusively in fourfold coordination. The location and relative intensity of X-ray absorption near-edge structure (XANES) features suggests the structural insertion of tetrahedral Al inside the silica framework synthesized by the organism. In diatom samples collected in the marine environment, Al is present in mixed six- and fourfold coordination. The relative intensity of XANES structures indicates the coexistence of structural Al with a clay component, which most likely reflects sample contamination by adhering mineral particles. Extended X-ray absorption fine structure spectroscopy has been used to get Al-O distances in biogenic silica of cultured diatoms, confirming a tetrahedral coordination. Because of its effect on solubility and reaction kinetics of biogenic silica, the structural association between Al and biogenic silica at the stage of biosynthesis has consequences for the use of sedimentary biogenic silica as an indicator of past environmental conditions.  相似文献   

19.
Monoclinic and hexagonal pyrrhotites leached in 1 mol/L HCl and exposed to the air at 100% and ∼10% relative humidity for up to 5 months were studied using X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), X-ray emission spectroscopy, Mössbauer spectroscopy, and electron paramagnetic resonance (EPR). The amorphous, nonequilibrium, iron-depleted layer (NL) produced by the leaching amounted to half of the residue mass and was composed of predominantly low-spin ferrous iron and polysulfide anions. Elemental sulfur and goethite were the only crystalline products of the NL decomposition. FTIR spectroscopy and XPS also revealed several sulfoxy species and, at low humidity, a small amount of ferric oxide. Neither alterations of the underlying pyrrhotite nor new iron sulfide phases (pyrite, pyrrhotite, etc.) crystallized from the amorphous NL were found. The NL decomposition was faster in the wet environment than in the dry one, and the oxidation of the NL was much more rapid than that of starting pyrrhotites. The intensity and quadruple split of the Mössbauer signal from the product (an isomer shift of 0.36 mm/s) were found to increase over the aging, indicating that the NL structure becomes more rigid and the singlet Fe(II) gradually converts to Fe(III). X-ray Fe Lα,β emission spectra showed the formation of intermediate, high-spin Fe(II) within the NL oxidized in the humid environment, but not in the dry air. No unpaired electron spins were detected by EPR; lines of paramagnetic Fe3+ appeared after the samples were aged in the dry air for 49 d and even later in the humid atmosphere. These phenomena are explained in terms of the formation of defects with negative correlation energy, similar to noncrystalline semiconductor chalcogenides, and of the fast electron exchange between the iron species, respectively. Mechanisms for reactions involved with the weathering of iron sulfides, which take into consideration the NL lattice elasticity, S-S and S-O bonding, oxygen incorporation, and oxidative and spin state of iron, are discussed. It is suggested in particular that the surface layer, strongly enriched in sulfur, as well as elemental sulfur and ferric oxyhydroxides, do not inhibit sulfide oxidation and acid production under weathering conditions, but the partially oxidized, disordered, nonstoichiometric layer may be passive.  相似文献   

20.
A deep “parent” composition for bonanza oreforming fluids at the Sleeper deposit was calculated by the computer program SOLVEQ using fluid-inclusion microthermometric and gas data, and by assuming equilibrium with the following minerals present in vein samples below the bonanza zones: gold, chalcedony, adularia, pyrite, chalcopyrite, and acanthite. The calculated dissolved gold content of 295 ppb is approximately 2 orders of magnitude higher than that assumed for typical geothermal systems. Thus, a gold-enriched fluid appears to have been a principal factor in the genesis of bonanza Au-Ag ores at the Sleeper deposit. Geochemical modelling of possible ore-forming processes using the computer program CHILLER, with the reconstructed ore-forming solution as a starting composition, indicates that boiling most closely reproduces observed minerals and their relative abundances in bonanza ores. The constraint imposed by the association of amorphous silica with gold precludes all of the mixing scenarios modelled, such as mixing with cold and steam-heated groundwaters (acid-sulfate, CO2-rich). Modelling indicates that boiling of a gold-rich deep solution leads to rapid gold precipitation, and that the amount of gold precipitated initially is large relative to other minerals. These factors apparently led to nucleation of colloidal gold particles instead of in-situ gold deposition or coprecipitation with other phases. Gold colloids apparently were entrained in the upward-flowing hydrothermal solutions and grew as they travelled. Upon reaching a critical size (10–100 nm?), they were deposited due to orthokinetic aggregation at an elevation and temperature at which amorphous silica was nucleating and aggregating.  相似文献   

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