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Francesco Di Benedetto Francesco D’Acapito Gabriele Fornaciai Massimo Innocenti Giordano Montegrossi Luca A. Pardi Silvia Tesi Maurizio Romanelli 《Physics and Chemistry of Minerals》2010,37(5):283-289
An X-ray absorption spectroscopy (XAS) study of the Fe local environment in natural amethyst (a variety of α-quartz, SiO2) has been carried out. Room temperature measurements were performed at the Fe K-edge (7,112 eV), at both the X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) regions. Experimental results were then compared with DFT calculations. XANES experimental spectra suggest Fe to occur mainly in the trivalent state, although a fraction of Fe2+ is identified. EXAFS spectra, on the other hand, reveal an unusual short distance for the first coordination shell: = 1.78(2) Å, the coordination number being 2.7(5). These results allow to establish that Fe replaces Si in its tetrahedral site, and that numerous local distortions are occurring as a consequence of the presence of Fe3+ variably compensated by protons and/or alkaline ions, or uncompensated. The formal valence of Fe, on the basis of both experimental and DFT structural features, can be either 4+ or 3+. Taking into account the XANES evidences, we suggest that Fe mainly occurs in the trivalent state, compensated by protons, and that a minor fraction of Fe4+ is stabilised by the favourable local structural arrangement. 相似文献
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Franco Tassi Bruno Capaccioni Giorgio Caramanna Daniele Cinti Giordano Montegrossi Luca Pizzino Fedora Quattrocchi Orlando Vaselli 《Applied Geochemistry》2009
A geochemical survey of thermal waters collected from submarine vents at Panarea Island (Aeolian Islands, southern Italy) was carried out from December 2002 to March 2007, in order to investigate (i) the geochemical processes controlling the chemical composition of the hydrothermal fluids and (ii) the possible relations between the chemical features of the hydrothermal reservoir and the activity of the magmatic system. Compositional data of the thermal water samples were integrated in a hydrological conceptual model, which describes the formation of the vent fluid by mixing of seawater, seawater concentrated by boiling, and a deep, highly-saline end-member, whose composition is regulated by water-rock interactions at relatively high temperature and shows clear clues of magmatic-related inputs. The chemical composition of concentrated seawater was assumed to be represented by that of the water sample having the highest Mg content. The composition of the deep end-member was instead calculated by extrapolation assuming a zero-Mg end-member. The Na–K–Ca geothermometer, when applied to the thermal end-member composition, indicated an equilibrium temperature of approximately 300 °C, a temperature in agreement with the results obtained by gas-geothermometry. 相似文献
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Maurizio?Romanelli Francesco?Di BenedettoEmail author Laura?Bartali Massimo?Innocenti Gabriele?Fornaciai Giordano?Montegrossi Luca?A.?Pardi Alfonso?Zoleo Fabio?Capacci 《Physics and Chemistry of Minerals》2012,39(6):479-490
A set of raw industrial materials, that is, pure quartz and quartz-rich mixtures, were investigated through electron paramagnetic
resonance and electron spin echo-envelope modulation spectroscopies, with the aim of evaluating the effective role played
by defect centres and of assessing whether they can be used to monitor changes in the physical properties of quartz powders
with reference to their health effects. The obtained results point to two interactions of the Al defect centres with H+, hosted in sites within the channels parallel and perpendicular to the c axis of quartz, respectively. These two Al/H+ (hAl) centres exhibit a weak chemical bond, and their relative amounts appear to be modified/controlled by the thermo-mechanical
processes underwent by powders. Indeed, a mechanically promoted inter-conversion between the two kinds of site is suggested.
As a consequence, the hAl centres are effective in monitoring even modest activations of powders, through thermal or mechanical processes, and they
are also supposed to play a specific, relevant role in quartz reactivity during the considered industrial processes. 相似文献
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Francesco Di Benedetto Daniele Borrini Andrea Caneschi Gabriele Fornaciai Massimo Innocenti Alessandro Lavacchi Carlo Andrea Massa Giordano Montegrossi Werner Oberhauser Luca A. Pardi Maurizio Romanelli 《Physics and Chemistry of Minerals》2011,38(6):483-490
An extensive characterisation of the magnetic properties of synthetic powders of kuramite, with formal composition Cu3SnS4, was performed. Powders were investigated through superconducting quantum interference device (SQUID) magnetometry, electron paramagnetic resonance (EPR) spectroscopy, X-ray powder diffraction (XRPD), scanning and transmission electron microscopies (SEM and TEM) and microanalysis. SEM and TEM reveal the presence of nanodimensioned particles. XRPD clearly shows that Cu3SnS4 crystallised in a cubic sphalerite-type structural model, in spite of the stannite-type tetragonal structure described for the natural phase. This difference arises from a full random distribution of cations. Synthetic kuramite nanopowders exhibit a marked paramagnetism, originated by the presence of Cu(II), definitely assessed by EPR measurements. Moreover, the overall magnetic behaviour of the sample cannot be simply ascribed to diluted paramagnetism, and this suggests the presence of strong superexchange interactions among Cu(II) ions even at room temperature. The main consequences of these results are the definitive assessment of the chemical formula Cu(I)2Cu(II)SnS4 and of a random distribution of Cu(II), Cu(I) and Sn(IV) ions within the available tetrahedral sites. 相似文献
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Hydrogeochemistry and strontium isotopes in the Arno River Basin (Tuscany, Italy): Constraints on natural controls by statistical modeling 总被引:2,自引:0,他引:2
B. Nisi A. Buccianti O. Vaselli G. Perini F. Tassi A. Minissale G. Montegrossi 《Journal of Hydrology》2008,360(1-4):166-183
In this paper the chemistry of major and trace elements and, for the first time, strontium isotopic ratios measured in running waters from the Arno River Basin (Tuscany, central-northern Italy) and thermal springs discharging in the same hydrographic system are presented and discussed. Classical graphical methods (e.g. mixing diagrams) have here been improved to identify, in a correct statistical sample space, extreme chemical compositions attributable to the action of geochemical processes and/or inherited from specific lithologies (namely contributions or components 1, 2 and 3) to be used in inverse modeling procedures, due to the absence of clear end-members. A linear least squares problem, with non-negativity constraints and distances, as required for compositional data (convex linear mixing) was solved by considering the contribution of the most discriminant variables given by the 87Sr/86Sr isotopic ratios and the concentration of Ca2+, Mg2+, Sr and Rb. Following such approach, it can be assumed (p < 0.05) that component 1, characterized by a Ca2+(Mg2+)– radiogenic-rich (87Sr/86Sr = 0.71274; Rb/Sr = 0.039), represents a dominant feature at basin scale, with a weight ranging from 69% to 100%. Much lower percentages are related to component 2, represented by a Ca2+(Mg2+)– facies with intermediate 87Sr/86Sr (0.70874) and low Rb/Sr (2.8 × 10−4) ratios and component 3, identified by Ca2+– facies with less radiogenic 87Sr/86Sr (0.70827) and low Mg2+/Ca2+ (0.011) ratios. These components are mainly dominated by the dissolution of evaporitic rocks and/or mixing with thermal waters in the southern part of the Arno River Basin and by dissolution of the carbonatic fraction, kinetically favored with respect to that of the silicatic minerals, in the upper reaches of the main course and its tributaries, respectively. 相似文献
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Francesco Di Benedetto Ilaria Bencistà Francesco D’Acapito Silvia Frizzera Andrea Caneschi Massimo Innocenti Alessandro Lavacchi Giordano Montegrossi Werner Oberhauser Maurizio Romanelli Herbert Dittrich Luca A. Pardi Gerold Tippelt Georg Amthauer 《Physics and Chemistry of Minerals》2016,43(8):535-544
The successful synthesis of nanoparticles of Fe-bearing kuramite, (Cu,Fe)3SnS4, is reported in this study. Nanocrystalline powders were obtained through a mild, environmentally friendly and scalable solvothermal approach, in a single run. The sample was the object of a multidisciplinary investigation, including X-ray diffraction and absorption, scanning electron microscopy and microanalysis, electron paramagnetic resonance, diffuse reflectance and Mössbauer spectroscopy as well as SQUID magnetometry. The nanoparticles consist of pure Fe-bearing kuramite, exhibiting tetragonal structure. The valence state of the metal cations was assessed to be Cu+, Sn4+ and Fe3+. The material presents a band gap value of 1.6 eV, which is fully compatible with solar cell applications. The uptake of Fe by nanokuramite opens a compositional field where the physical properties can be tuned. We thus foster the application of Fe-bearing nanokuramite for photovoltaics and energy storage purposes. 相似文献
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Francesco Di Benedetto Francesco D’Acapito Fabio Capacci Gabriele Fornaciai Massimo Innocenti Giordano Montegrossi Werner Oberhauser Luca A. Pardi Maurizio Romanelli 《Physics and Chemistry of Minerals》2014,41(3):215-225
We investigated the speciation of Fe in bulk and in suspended respirable quartz dusts coming from ceramic and iron-casting industrial processes via X-ray absorption spectroscopy, with the aim of contributing to a better understanding of the variability of crystalline silica toxicity. Four different bulk industrial quartz powders, nominally pure quartz samples with Fe contents below 200 ppm, and three respirable dusts filters were selected. Fe speciation was determined in all samples through a coupled study of the X-ray absorption near-edge structure and extended X-ray absorption fine structure regions, operating at the Fe–K edge. Fe speciation revealed common features at the beginning of the different production processes, whereas significant differences were observed on both respirable dusts and bulk dusts exiting from the production process. Namely, a common pollution of the raw quartz dusts by elemental Fe was evidenced and attributed to residuals of the industrial production of quartz materials. Moreover, the respirable samples indicated that reactivity occurs after the suspension of the powders in air. The gravitational selection during the particle suspension consistently allowed us to clearly discriminate between suspended and bulk dusts. On the basis of the obtained results, we provide an apparent spectroscopic discrimination between the raw materials used in the considered industrial processes, and those that are effectively inhaled by workers. In particular, an amorphous FeIII oxide, with an unsaturated coordination sphere, can be related to silica reactivity (and health consequences). 相似文献
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F. Tassi O. Vaselli B. Capaccioni J. L. Macias A. Nencetti G. Montegrossi G. Magro 《Journal of Volcanology and Geothermal Research》2003,123(1-2):105
Since the March–April 1982 eruption of El Chichòn volcano, intense hydrothermal activity has characterised the 1-km-wide summit crater. This mainly consists of mud and boiling pools, fumaroles, which are mainly located in the northwestern bank of the crater lake. During the period 1998–2000, hot springs and fumaroles discharging inside the crater and from the southeastern outer flank (Agua Caliente) were collected for chemical analyses. The observed chemical fluctuations suggest that the physico-chemical boundary conditions regulating the thermodynamic equilibria of the deep rock/fluid interactions have changed with time. The chemical composition of the lake water, characterised in the period 1983–1997 by high Na+, Cl−, Ca2+ and SO42− contents, experienced a dramatic change in 1998–1999, turning from a Na+–Cl−- to a Ca2+–SO42−-rich composition. In June 2000, a relatively sharp increase in Na+ and Cl− contents was observed. At the same time, SO2/H2S ratios and H2 and CO contents in most gas discharges increased with respect to the previous two years of observations, suggesting either a new input of deep-seated fluids or local variations of the more surficial hydrothermal system. Migration of gas manifestations, enhanced number of emission spots and variations in both gas discharge flux and outlet temperatures of the main fluid manifestations were also recorded. The magmatic-hydrothermal system of El Chichòn is probably related to interaction processes between a deep magmatic source and a surficial cold aquifer; an important role may also be played by the interaction of the deep fluids with the volcanic rocks and the sedimentary (limestone and evaporites) basement. The chemical and physical changes recorded in 1998–2000 were possibly due to variations in the permeability of the conduit system feeding the fluid discharges at surface, as testified by the migration of gas and water emanations. Two different scenarios can be put forward for the volcanic evolution of El Chichòn: (1) build-up of an infra-crater dome that may imply a future eruption in terms of tens to hundreds of years; (2) minor phreatic–phreatomagmatic events whose prediction and timing is more difficult to constrain. This suggests that, unlike the diminished volcanic activity at El Chichòn after the 1982 paroxistic event, the volcano-hydrothermal fluid discharges need to be more constantly monitored with regular and more frequent geochemical sampling and, at the same time, a permanent network of seismic stations should be installed. 相似文献
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F. Di Benedetto G. Montegrossi A. Minissale M. Romanelli A. Delgado Huertas O. Vaselli D. Borrini 《Geochimica et cosmochimica acta》2011,75(16):4441-4455
A multidisciplinary characterization of an active thermal spring in central Italy has been undertaken with the aim of (i) ascertaining whether microbiological activity plays a relevant role in hot-depositing travertines and (ii) establishing an experimental protocol able to identify similar effects in fossil travertines. Water, gas, and travertine samples were investigated by chemical (ICP/MS, SEM/EDS), physical (DTA-DTG), isotopic (δ18O, δD, and δ13C), mineralogical (XRPD), and spectroscopic (EPR) techniques. Twenty-four samples (three for each phase) were collected every 5 °C temperature drop, along a ∼100 m long artificial channel near Viterbo (Bullicame 3, Latium, central Italy). A microbiological characterization was carried out in parallel, sampling the channel every 10 °C temperature drop.The Bullicame 3 system is revealed to be composed of two markedly different subsystems: a water/gas interface, where a kinetically fast exchange allows equilibrium of components both in water and in gases; a solid/water interface, where travertine precipitation occurs, influenced by microbiological activity. A peculiar lattice shrinking of calcite was identified, as well as an anomalous value of the zero-field splitting parameter from the EPR measurements. The interpretation of these anomalies is confirmed by the identification of calcifying cyanobacteria throughout the channel path.Our results point out that microbiological activity can play a significant role in travertine deposition from hot springs. Furthermore, the proposed approach, representing a tool to identify crystal chemical remnants of past microbiological activity, could be applicable to fossil travertines. 相似文献
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