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1.
NMR,XRD and IR study on microcrystalline opals   总被引：1，自引：0，他引：1  
Microcrystalline opal-CT and opal-C were investigated by 29Si MAS NMR and 29Si {1H} cross polarisation MAS NMR spectroscopy, X-ray small angle scattering, X-ray powder diffraction and infrared absorption spectroscopy. The results are compared with those for non-crystalline precious opal (opal-AG), non-crystalline hyalite (opal-AN), moderately disordered cristobalite and with well ordered low-cristobalite and low-tridymite. Opal-C is confirmed to be strongly stacking disordered low-cristobalite with about 20 to 30% probability for tridymitic stacking. More extensively stacking disordered opal-CT does not contain detectable domains of low-cristobalite or low-tridymite. The stacking sequence is close to 50% cristobalite and 50% tridymitic. The local order decreases with increasing stacking disorder, so that the structural state of microcrystalline opals lies between cristobalite, tridymite and non-crystalline opals.  相似文献   

2.
直至目前,我国相关欧泊的矿藏及其相应的矿物学特征鲜见报道,近期在浙江丽水缙云地区发现的蓝色类欧泊石引起了宝玉石科研工作者的广泛关注,但此矿物的相关研究至今尚未见论述。本文应用X射线荧光光谱(XRF)、场发射扫描电镜(FE-SEM)结合X射线粉晶衍射(XRD)与傅里叶变换红外光谱(FTIR)等多种综合检测技术首次对该类蓝色原矿的矿物学及光学变彩性质进行研究。结果表明:XRF分析显示蓝色原矿的主体化学组成为SiO2(质量含量95%),仅含极少量的Fe2O3与Al2O3等杂质。同时,蓝色原矿及其相应的热处理后样品局部区域具有明显的变彩特征,主体的化学组成与其光学特征与天然欧泊的组成及变彩效应类同。XRD分析显示原矿粉体的无机相的晶型为方石英相,衍射峰形锐化,该晶体的结构特征明显相异于天然欧泊即微晶类的蛋白石(Opal-CT)、Opal-C与非晶蛋白石类(Opal-A)。此外,样品的红外光谱与天然欧泊间存在一定的频率位移。鉴于此,初步将该类原矿归属为类欧泊,因蓝色原矿所在地丽水缙云地区属于中生代陆相火山岩的地质,因此进一步将该原矿命名为一类火山岩类的类欧泊石,而有关此类欧泊是否可以归属为广义上的欧泊有待再作商榷。同时基于对蓝色原矿有无变彩效应区域的FE-SEM测试结论,本文初步推测该类矿物的光学变彩特征与原矿表面的“叠瓦状”结构形貌有关。  相似文献   

3.
This paper reports the results of the study of hydrothermal precious opals. It was established that, in terms of their nanostructure and formation conditions, the hydrothermal opals differ from exogenic precious opals. They are made up of small globules and do not show any structuring of their nanoparticles on the basis of closest packing, which is typical of exogenic precious opals. During their formation, these opals were subjected to pneumatolytic annealing—they experienced the impact of a high-temperature vapor under elevated pressure. The influence of the thermal effect led to the formation of two-dimensional photonic band gaps in the chaotic opal matrix. These bands are composed of sheets whose cells were formed owing to the thermal effects according to the principle of “Benard cells.” Precisely these structured blocks and thin films are responsible for the spectral dispersion of light and iridescence.  相似文献   

4.
The decrease of the mean Si-O-Si angle in vitreous silica upon densification from 2.20 to 2.36 gcm-3 has been followed by oxygen and silicon K-edge XANES spectroscopy. Multiple scattering calculations using clusters of two shells around the oxygen and silicon atoms, respectively, are in good agreement with experimental absorption spectra and confirm mean Si-O-Si angles between 130 and 144° for these samples, and a decrease of the mean angle with densification. The experimental spectra also exhibit features due to scattering at outer (>2) shells around the photoabsorbers.  相似文献   

5.
Based on the idea that the X-ray emission of the knots in the kiloparsec-scale jet of 3C 273 located closest to the active nucleus is due to inverse Compton scattering on the quasar radiation, while the X-ray emission of knots further from the nucleus is due to inverse Compton scattering on the cosmic microwave background, we find that the angle of the jet to the line of sight is θ ≈ 30°. The magnetic field and electron density in the knots are estimated. It is concluded that there is a break in the electron-energy spectrum at a Lorentz factor of г ∼ 106. It is shown that the energy density of the relativistic electrons in the knots appreciably exceeds the energy density in the magnetic field.  相似文献   

6.
埃塞俄比亚WOLLO地区产出的欧泊品种丰富,但火欧泊和水欧泊不稳定,易因外界温度或水分变化形成较多裂纹,严重影响其稳定性及加工性能。因此,本实验对埃塞俄比亚WOLLO地区产出的多裂纹火欧泊、水欧泊样品进行了充填处理,并对充填前、后的样品进行了显微放大观察和红外光谱、相对密度、紫外荧光的测试及分析,总结出了有机充填欧泊的一些鉴定特征。测试及分析结果显示,在2800-3100cm叫范围内红外吸收峰为有机充填欧泊的主要鉴定特征,表面及内部显微充填特征、偏小的相对密度、裂隙处的蠕虫状及空洞缺陷处的斑块状强蓝白色荧光可作为辅助鉴定特征。从样品的充填及测试分析结果可见,埃塞俄比亚WOLLO地区产出欧泊的有机充填方案可行,比较明显的开放裂隙易被充填。  相似文献   

7.
The occurrence of water in natural opaline silicas has been studied by differential thermal analysis, thermogravimetric analysis, infra‐red analysis and nuclear magnetic resonance. The results show that in the “crystalline” opals studied, some 90 per cent or more of the total water is physically adsorbed whereas in “amorphous” opals, at least 20 per cent but perhaps much more of the total water is held as hydroxyl groups chemically bonded to the silica surface. The rate of water loss on heating is also different, being chiefly controlled by the pore structure in “crystalline” opals but to a significant extent by the surface structure in “amorphous”.  相似文献   

8.
Mineralogical and textural changes accompanying ageing of silica sinter   总被引：3，自引：0，他引：3  
Twenty nine samples of silica sinter, ranging in age from modern to Miocene, record temporal changes in both mineralogy and texture. When first deposited, sinters consist largely of noncrystalline spheres (<1–8 μm diameter) of opal-A exhibiting varying degrees of close-packing. Particle densities range from 1.5 to 2.1 g cm−3, total water 4–10 wt%, and porosities 35–60%. Changes over ∼10,000 years following deposition are slight although the spheres may be invested by an additional film of secondary silica. For the next 10,000 to ∼50,000 years, the silica incrementally crystallises to become poorly crystalline opal-CT and/or opal-C; spherical particles of thin-bladed crystals (lepispheres) replace opal-A particles and coalesce in microbotryoidal aggregates (∼10–30 μm diameter). Amygdaloidal fibrous clusters occur with lepispheres. As silica lattice ordering becomes enhanced, total water content drops to <7 wt%, particle density increases to ∼2.3 g cm−3, and porosity reduces to <30%. The change from opal-A to opal-C takes place over a briefer periods (∼50 years) in silica sinters that contain other materials (e.g. calcite, sulfur, alunite, plant remains). Sinters older than ∼50,000 years have recrystallised to microcrystalline quartz. With the onset of quartz crystallisation at ∼20,000 years, total water is <0.2 wt%, particle density approximates quartz (2.65 g cm−3), and porosity is <4%. The progressive changes in silica species and texture yield ageing profiles for sinters that may serve as guides to the paleohydrology of geothermal systems and/or epithermal ore deposits in areas where surface thermal activity has declined or ceased. Received: 18 November 1998 / Accepted: 6 July 1999  相似文献   

9.
Sedimentary biogenic silica from Redeyef in Gafsa basin (southern Tunisia) was analysed for its 29Si and 27Al magic angle spinning nuclear magnetic resonance (MAS NMR) spectra and complemented by X-ray diffraction and SEM observations. The 29Si MAS NMR spectrum is characterized by the abundance of hydroxylated silicon, displayed in resonance intensities and reflects a clear tendency towards dissolution of diatomaceous amorphous silica and the occurrence of the hydrated silica, which is the main component that ensures the diagenetic transition via the mechanism of dissolution–precipitation to other more crystalline silica phases, after the lost of its hydroxyls groups (water) by heating (burial). 27Al MAS NMR reveals two coordinations of Al; the octahedrally coordinated Al suggests the presence of clay relics trapped during crystal growth or a microcrystalline zeolite (clinoptilolite detected by SEM observations), while the tetrahedrally coordinated Al suggests the presence of minor quantities of minerals with tetrahedral Al, such as an Al-rich fluid and/or minerals such as feldspars.  相似文献   

10.
Agate/chalcedony samples of different origin were investigated by performing Raman, X-ray diffraction (using Rietveld refinement), and cathodoluminescence measurements. These analyses were performed to measure the content and spatial distribution of the silica polymorph moganite, which is considered to represent periodic Brazil-law twinning of α-quartz at the unit-cell scale in agate/chalcedonies. Homogeneous standard samples including the nearly α-quartz free moganite type material from Gran Canaria were analysed in order to compare results of the X-ray diffractometry and Raman spectroscopy techniques and to provide a calibration curve for the Raman results. However, due to the different length scales analysed by the two techniques, the “moganite content” in microcrystalline SiO2 samples measured by Raman spectroscopy (short-range order) was found to be considerably higher than the “moganite content” measured by X-ray diffractometry (long-range order). The difference is explained by the presence of moganite nanocrystals, nano-range moganite lamellae, and single Brazil-law twin-planes that are detected by vibrational spectroscopy but that are not large enough (in the sense of coherently scattering lattice domains) to be detected by X-ray diffractometry. High resolution Raman analysis provides a measure of the moganite content and its spatial variation in microcrystalline silica samples with a lateral resolution in the μm-range. Variations in the moganite-to-quartz ratio are revealed by varying intensity ratios of the main symmetric stretching-bending vibrations (A1 modes) of α-quartz (465 cm−1) and moganite (502 cm−1), respectively. Traces of Raman microprobe analyses perpendicular to the rhythmic zoning of agates revealed that the moganite-to-quartz ratio is often not uniform but shows a cyclic pattern that correlates with the observed cathodoluminescence pattern (colour and intensity). Data obtained from an agate sample from a fluorite deposit near Okorusu, Namibia and from a volcanic agate from Los Indios, Cuba were selected for detailed presentation. Variations of cathodoluminescence and Raman data between single bands in agates suggest alternating formation of fine-grained, highly defective chalcedony intergrown with moganite, and coarse-grained low-defect quartz. Multiple zones indicate dynamic internal growth during a self-organizational crystallization process from silica-rich fluids. Received: 4 December 1997 / Accepted 19 June 1998  相似文献   

11.
 The electrical properties of opal-CT are validated at temperatures from 600 to 840 °C and frequencies from 5 Hz to 10 MHz. The opals are hydrothermal, containing less than 11270 ppm total of Al, Fe, Ca, Na, and K, and from 1.17 to 17.63 wt% H2O interstitial and structural. Opal-CT shows fine crystallites, measuring from 19.4 to 22.7 μm, of an ordered tridymite-M stratification with high-cristobalite, embedded in a non-crystalline matrix. When heated to 600 °C, the non-crystalline phase devitrifies to the same stacked high-cristobalite-tridymite-M crystals. Opals containing less than 2070 ppm of cationic impurities are characterized by one single high-frequency complex impedance arc corresponding to the bulk polarization of the crystalline phase, of capacitances between 25 and 30×10−12 F and resistances from 132 to 890 ohm. Opals having over 6300 ppm of cationic impurities show two superimposed high- and low-frequency complex impedance arcs. The high-frequency arc corresponds to the bulk polarization of the crystalline phase, of capacitance between 8 and 15.7×10−12 F and resistance from 14 to 236 ohm, less than the capacitance of 0.25 to 0.53×10−9 F and resistance from 26 to 360 ohm of the non-crystalline minor intergranular material represented by the low-frequency impedance arc. The electric module shows one single vertex, ascribed to the bulk polarization of the crystalline phase. The conductivities are from 10−7 to 10−4 ohm−1cm−1, in the range of poor ionic conductors, essentially constant below 1.8 kHz, rapidly increasing at higher frequencies, due to ionic and electronic charge carriers. The activation energy changes between 0.905 and 1.003 eV for the conduction mechanism in the crystalline phase and from 0.924 to 1.087 eV in the non-crystaline phase. X-ray diffraction and impedance spectroscopy confirm that opal-CT is a crystalline stacked sequence of tridymite-M and cristobalite-high, in a non-crystalline matrix. Received October 20, 1995/Revised, accepted June 15, 1996  相似文献   

12.
Abstract

Black opal (opal-AG) owes its dark coloration to a fine-grained pigment commonly inferred to be mainly carbon, yet chemical compositions for black opals suggest there may be additional components. Here we search for such components in pigment concentrates prepared by dissolving black opal nodules (nobbies) from Lightning Ridge (NSW) in hydrofluoric acid, using electron microscopy (scanning electron microscopy, transmission electron microscopy), X-ray diffraction and laser-ablation ICP-MS. The results demonstrate the presence of sulfides—predominantly pyrite and chalcopyrite, with minor galena and Ti-oxide phases, as additional components of the pigment. ATR-FTIR analysis indicates the presence of C=O and C–H groups, consistent with an organic origin. Transmission electron microscopy images of pigment show variously deformed, originally spherical ～100?nm particles rich in sulfide and carbon, which are interpreted as thin coatings of pigment on now dissolved opaline silica spheres. Laser-ablation ICP-MS analysis identifies remnant silica in pigment concentrates, which may be interpreted as opaline silica surviving HF treatment protected as inclusions in sulfides. When examined within the context of petrographic observations from more than 1000 opal nodules (nobbies) at Lightning Ridge, these new results suggest that pigment carbon and sulfides in the nodules formed microbially under initially anoxic groundwater conditions, within pre-existing cavities concurrently being filled with silica sol ultimately derived from chemical weathering of feldspar-rich volcaniclastic sediment. Intensely black pigment layers observed at the floor of many nodules indicate settling of dark, high-density (sulfide–Ti-oxide-rich) pigment within cavities, with the implication that sulfate-reducing bacterial (SRB) activity commences early during the silica sol-gel ripening process. Microbial activity may persist until after the cavity has completely filled with the silica sol, as illustrated by abundant black opals with uniformly distributed pigment. Pigment formed at this stage may no longer be able to settle out within the ripening and increasingly viscous silica gel, thus forming pigmentation throughout the opal cavity. The existence of ‘amber’, pigment-poor opal with intensely black basal pigment layers is interpreted as signalling a lack of sulfate to sustain further SRB activity, or a change to more oxidising conditions, possibly related to interaction with surface waters within a downward-penetrating weathering front. A change in redox conditions would shut off activity of SRB and thus sulfide pigment production and allow development of aerobic microbial activity as described by others.  相似文献   

13.
This paper presents the results of the δ18O study of the precious opals from Primor’e (Raduzhnoe deposit), Australia, and Ethiopia and the modern opals from the hydrotherms of the Mendeleev Volcano (Kunashir Island, Kuril Islands). It is established that the oxygen isotope ratio in opals may serve as a criterion for the estimation of their formation temperature. The low-temperature sedimentary opals are relatively enriched in the heavy oxygen isotope independently of the sedimentary or volcanic host rocks. Examples are the Australian and Slovakian opals of the A-type. The hydrothermal opals are enriched in the light oxygen isotope, which depends on the precipitation temperature. The higher the temperature, the lighter the oxygen isotope ratio of the precipitating opal is and the closer it is to that of the hydrothermal fluid.  相似文献   

14.
Seventy-seven gem opals from ten countries were analyzed by inductively coupled plasma-mass spectrometry (ICP-MS) through a dilution process, in order to establish the nature of the impurities. The results are correlated to the mode of formation and physical properties and are instrumental in establishing the geographical origin of a gem opal. The geochemistry of an opal is shown to be dependant mostly on the host rock, at least for examples from Mexico and Brazil, even if modified by weathering processes. In order of decreasing concentration, the main impurities present are Al, Ca, Fe, K, Na, and Mg (more than 500 ppm). Other noticeable elements in lesser amounts are Ba, followed by Zr, Sr, Rb, U, and Pb. For the first time, geochemistry helps to discriminate some varieties of opals. The Ba content, as well as the chondrite-normalized REE pattern, are the keys to separating sedimentary opals (Ba > 110 ppm, Eu and Ce anomalies) from volcanic opals (Ba < 110 ppm, no Eu or Ce anomaly). The Ca content, and to a lesser extent that of Mg, Al, K and Nb, helps to distinguish gem opals from different volcanic environments. The limited range of concentrations for all elements in precious (play-of-color) compared to common opals, indicates that this variety must have very specific, or more restricted, conditions of formation. We tentatively interpreted the presence of impurities in terms of crystallochemistry, even if opal is a poorly crystallized or amorphous material. The main replacement is the substitution of Si4+ by Al3+ and Fe3+. The induced charge imbalance is compensated chiefly by Ca2+, Mg2+, Mn2+, Ba2+, K+, and Na+. In terms of origin of color, greater concentrations of iron induce darker colors (from yellow to “chocolate brown”). This element inhibits luminescence for concentrations above 1000 ppm, whereas already a low content in U (≤ 1 ppm) induces a green luminescence.  相似文献   

15.
《International Geology Review》2012,54(11):1750-1754
Examination of a large number of specimens of α-quartz, α-cristobalite, chalcedonies, opals, quartzines, and agates shows that the so-called amorphous forms of silica do not represent any particular specificities, but are simply amorphous mixtures, more often than not, for example, α-quartz with tridymite, on the α-quartz base (chalcedonies, opals). In chalcedonies the tridymitic constituent is somewhat larger than in opals. Another large group of opals is but an altered α-cristobalite, high in molecular water. The α-quartz opals characteristically contain far less water. — Authors.  相似文献   

16.
The dynamics of cyanobacterial silicification was investigated using synchrotron-based Fourier transform infrared micro-spectroscopy. The changes in exo-polymeric polysaccharide and silica vibrational characteristics of individual Calothrix sp. filaments was determined over time in a series of microcosms in which the microbially sorbed silica or silica and iron load was increased sequentially. The changes in intensity and integrated area of specific infrared spectral features were used to develop an empirical quantitative dynamic model and to derive silica load-dependent parameters for each quasi-equilibrium stage in the biomineralization process.The degree of change in spectral features was derived from the increase in integrated area of the combined silica/polysaccharide region (Si-O/C-O, at 1150-950 cm−1) and the Si-O band at 800 cm−1, the latter representing specific silica bonds corresponding to hydrated amorphous SiO4 tetrahedra. From the degree of change, a two-phase model with concurrent change in process was derived. In the first phase, a biologically controlled increase in thickness of the exo-polymeric polysaccharide sheath around the cell was observed. In phase two, a transition to an inorganically controlled accumulation of silica on the surface of the cyanobacterial cells was derived from the change in integrated area for the mixed Si-O/C-O spectral region. This second process is further corroborated by the synchronous formation of non-microbially associated inorganic SiO4 units indicated by the growth of the singular Si-O band at 800 cm−1. During silicification, silica accumulates (1) independently of the growth of the sheath polysaccharides and (2) via an increase in chain lengths of the silica polymers by expelling water from the siloxane bonds. IR evidence suggest that an inorganic, apparently surface catalyzed process, which leads to the accumulation of silica nanospheres on the cyanobacterial surfaces governs this second stage. In experiments where iron was present, the silicification followed similar pathways, but at low silica loads, the iron bound to the cell surfaces slightly enhanced the reaction dynamics.  相似文献   

17.
Activity coefficient for aqueous silica in saline waters and brines from the Paris Basin was calculated using Pitzer's specific interaction model. Quartz and chalcedony are the only reported authigenic silica minerals in the Dogger aquifer of the Paris Basin (France). However, the measured silica concentrations fall between those of these two phases. The silica concentrations measured in Dogger fluids seem to be controlled by a microcrystalline quartz phase with a grain size computed to be about 20 nm. Studies have shown that pressure can preserve small grain size for a long time at the geological scale. The effective mechanism of pressure action is probably linked to the fact that pressure simultaneously favours dissolution at the grain-contact inducing a quartz supersaturation and prohibits the increase in size of reprecipitated microcrystalline quartz grains. This hypothesis is supported by other studies reported in the literature. The proposed model, which incorporates silica mineralogy and a precise calculation of aqueous silica activity, allows us to explain measured silica concentrations in the deep sedimentary solutions of the Dogger aquifers. In the Keuper brines, silica solubility can in most cases be explained by an equilibrium with either chalcedony or quartz. Another application of the present work is shown by an example, where we examined the importance of precisely evaluating the activity coefficient in basin characterisation, as the goal of reservoir characterisation is to describe the spatial distribution of petrophysical parameters such as porosity, permeability, and saturations.  相似文献   

18.
The electron localization function, η, evaluated for first-principles geometry optimized model structures generated for quartz and coesite, reveals that the oxide anions are coordinated by two hemispherically shaped η-isosurfaces located along each of the SiO bond vectors comprising the SiOSi angles. With one exception, they are also coordinated by larger banana-shaped isosurfaces oriented perpendicular to the plane centered in the vicinity of the apex of each angle. The hemispherical isosurfaces, ascribed to domains of localized bond-pair electrons, are centered ～0.70 Å along the bond vectors from the oxide anions and the banana-shaped isosurfaces, ascribed to domains of localized nonbonding lone-pair electrons, are centered ～0.60 Å from the apex of the angle. The oxide anion comprising the straight SiOSi angle in coesite is the one exception in that the banana-shaped isosurface is missing; however, it is coordinated by two hemispherically shaped isosurfaces that lie along the bond vectors. In the case of a first-principles model structure generated for stishovite, the oxide anion is coordinated by five hemispherically shaped η-isosurfaces, one located along each of the three SiO bond vectors (ascribed to domains of bonding-electron pairs) that are linked to the anion with the remaining two (ascribed to domains of nonbonding-electron pairs) located on opposite sides of the plane defined by three vectors, each isosurface at a distance of ～0.5 Å from the anion. The distribution of the five isosurfaces is in a one-to-one correspondence with the distribution of the maxima displayed by experimental Δρ and theoretical ??2ρ maps. Isosurface η maps calculated for quartz and the (HO) 3 SiOSi(OH) 3 molecule also exhibit maxima that correspond with the (3,?3) maxima displayed by distributions of ??2ρ. Deformation maps observed for the SiOSi bridges for the silica polymorphs and a number of silicates are similar to that calculated for the molecule but, for the majority, the maxima ascribed to lone-pair features are absent. The domains of localized nonbonding-electron pair coordinating the oxide anions of quartz and coesite provide a basis for explaining the flexibility and the wide range of the SiOSi angles exhibited by the silica polymorphs with four-coordinate Si. They also provide a basis for explaining why the SiO bond length in coesite decreases with increasing angle. As found in studies of the interactions of solute molecules with a solvent, a mapping of η-isosurfaces for geometry-optimized silicates is expected to become a powerful tool for deducing potential sites of electrophilic attack and reactivity for Earth materials. The positions of the features ascribed to the lone pairs in coesite correspond with the positions of the H atoms recently reported for an H-doped coesite crystal.  相似文献   

19.
Diatomite, a type of biogenic mineral, is sourced from deposition and accumulation of diatom shell. Diatom shells are mainly composed of amorphous hydrated silica, which is categorized as non-crystalline opal-A according to the mineralogical classification. Diatomite has a characteristic macro/mesoporous structure and unique physical and chemical capabilities, such as high thermal stability, strong acid resistance, and high adsorption capacity, and thus is widely used as the filter aid, catalytic support, and adsorbent. However, the low surface area of diatomite shows disadvantage in adsorption. Moreover, the hydrophilic surface which contains abundant silanols is usually covered by adsorbed water, resulting in that the adsorption sites of diatomite were occupied and the adsorption capacity of hydrophobic guests decreased. In previous reports, zeolitization was employed to increase the specific surface area (SBET) and porosity of diatomite. However, the hydrophilic property of diatomite was not changed after zeolitization. It is due to that the zeolite formed on the surface area of diatomite contained some aluminum in its structure, which was highly hydrophilic. Therefore, it is significantly interesting to prepare the zeolitized diatomite with both large SBET and high hydrophobicity.  相似文献   

20.
Different polymorphs of silica and the opals exhibit significant variations in densities. The paper discusses and correlates the variations in the molar refraction with density. It emerges that in different polymorphs of silica, the increase in density involves a corresponding increase in the characteristic dispersion frequencies leading to a decrease in the molar refraction. The variation of the molar refraction with density can be represented in terms of an elementary formula. The variation of the molar refraction of opals with the water content in them is also accounted for.  相似文献   

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