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Mario Villalobos Brandy Toner Garrison Sposito 《Geochimica et cosmochimica acta》2003,67(14):2649-2662
Manganese oxides form typically in natural aqueous environments via Mn(II) oxidation catalyzed by microorganisms, primarily bacteria, but little is known about the structure of the incipient solid-phase products. The Mn oxide produced by a Pseudomonas species representative of soils and freshwaters was characterized as to composition, average Mn oxidation number, and N2 specific surface area. Electron microscopy, X-ray diffraction, and X-ray absorption near edge structure spectroscopy were applied to complement the physicochemical data with morphological and structural information. A series of synthetic Mn oxides also was analyzed by the same methods to gain better comparative understanding of the structure of the biogenic oxide. The latter was found to be a poorly crystalline layer type Mn(IV) oxide with hexagonal symmetry, significant negative structural charge arising from cation vacancies, and a relatively small number of randomly stacked octahedral sheets per particle. Its properties were comparable to those of δ-MnO2 (vernadite) and a poorly crystalline hexagonal birnessite (“acid birnessite”) synthesized by reduction of permanganate with HCl, but they were very different from those of crystalline triclinic birnessite. Overall, the structure and composition of the Mn oxide produced by P. putida were similar to what has been reported for other freshly precipitated Mn oxides in natural weathering environments, yielding further support to the predominance of biological oxidation as the pathway for Mn oxide formation. Despite variations in the degree of sheet stacking and Mn(III) content, all poorly crystalline oxides studied showed hexagonal symmetry. Thus, there is a need to distinguish layer type Mn oxides with structures similar to those of natural birnessites from the synthetic triclinic variety. We propose designating the unit cell symmetry as an addition to the current nomenclature for these minerals. 相似文献
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University faculty partners from the Departments of Geography and Instruction and Teacher Education at a large, public university collaborated with K-12 teachers and the leadership of a rural school district in order to investigate the crosscutting content of science, mathematics, and geography through the integration of web-based GIS technologies. The project explored the critical connections among technology, pedagogy, and content with a particular emphasis on developing technology-enhanced, inquiry-based lessons in which the teachers and their students used GIS technologies to analyze, visualize, and present data in real-world contexts. The findings highlight the importance of well-structured professional development that builds community, integrates diverse content and pedagogical expertise, provides feedback and coaching, and is of sufficient duration to effect change. 相似文献
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Mark Brenner Thomas J. Whitmore Melanie A. Riedinger-Whitmore Brandy DeArmond Douglas A. Leeper William F. Kenney Jason H. Curtis Byron Shumate 《Journal of Paleolimnology》2006,36(4):371-383
We studied sediment cores from four Florida (USA) lakes that have received groundwater hydrologic supplements (augmentation) for >30 years to maintain lake stage. Top samples (0–4 cm) from sediment cores taken in Lakes Charles, Saddleback, Little Hobbs, and Crystal had 226Ra activities of 44.9, 17.5, 7.6, and 8.5 dpm g−1, respectively, about an order of magnitude greater than values in deeper, older deposits. The surface sample from Lake Charles yielded the highest 226Ra activity yet reported from a Florida lake core. Several lines of evidence suggest that groundwater augmentation is responsible for the high 226Ra activities in recent sediments: (1) 226Ra activity in cores increased recently, (2) the Charles, Crystal, and Saddleback cores display 226Ra/210Pb disequilibrium at several shallow depths, suggesting 226Ra entered the lakes in dissolved form, (3) cores show recent increases in Ca, which, like 226Ra, is abundant in augmentation groundwater, and (4) greater Sr concentrations are associated with higher 226Ra activities in recent Charles and Saddleback sediments. Sr concentrations in Eocene limestones of the deep Floridan Aquifer are high relative to Sr concentrations in surficial quartz sands around the lakes. Historical water quality inferences for the lakes were based on diatom assemblages in sediments. Recent alkalization in Lakes Charles, Saddleback, Little Hobbs, and Crystal was inferred from weighted-averaging calibration (WACALIB). The lakes also show recent trophic state increases based on WACALIB-derived estimates for limnetic total P. Although residential and agricultural sources might contribute to increased P loading, P in augmentation waters probably has had significant influence on eutrophication. Dystrophic diatoms were abundant in the early history of Lakes Saddleback, Little Hobbs, and Crystal, which suggests that these lakes contained more tannic waters during the past than at present, perhaps as a consequence of greater inflows from surrounding wetlands. Ionic content of lake waters increased, as indicated by diatom autecological analysis. Recent geochemical and biological changes detected in cores from these lakes probably are a result of deliberate groundwater augmentation, although inputs of groundwater pumped for agricultural and residential development in the watersheds also might have contributed to limnological changes. 相似文献
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Brandy M. Toner Cara M. Santelli Richard Wirth Thomas McCollom Katrina J. Edwards 《Geochimica et cosmochimica acta》2009,73(2):388-994
Here we examine Fe speciation within Fe-encrusted biofilms formed during 2-month seafloor incubations of sulfide mineral assemblages at the Main Endeavor Segment of the Juan de Fuca Ridge. The biofilms were distributed heterogeneously across the surface of the incubated sulfide and composed primarily of particles with a twisted stalk morphology resembling those produced by some aerobic Fe-oxidizing microorganisms. Our objectives were to determine the form of biofilm-associated Fe, and identify the sulfide minerals associated with microbial growth. We used micro-focused synchrotron-radiation X-ray fluorescence mapping (μXRF), X-ray absorption spectroscopy (μΕXAFS), and X-ray diffraction (μXRD) in conjunction with focused ion beam (FIB) sectioning, and high resolution transmission electron microscopy (HRTEM). The chemical and mineralogical composition of an Fe-encrusted biofilm was queried at different spatial scales, and the spatial relationship between primary sulfide and secondary oxyhydroxide minerals was resolved. The Fe-encrusted biofilms formed preferentially at pyrrhotite-rich (Fe1−xS, 0 ? x ? 0.2) regions of the incubated chimney sulfide. At the nanometer spatial scale, particles within the biofilm exhibiting lattice fringing and diffraction patterns consistent with 2-line ferrihydrite were identified infrequently. At the micron spatial scale, Fe μEXAFS spectroscopy and μXRD measurements indicate that the dominant form of biofilm Fe is a short-range ordered Fe oxyhydroxide characterized by pervasive edge-sharing Fe-O6 octahedral linkages. Double corner-sharing Fe-O6 linkages, which are common to Fe oxyhydroxide mineral structures of 2-line ferrihydrite, 6-line ferrihydrite, and goethite, were not detected in the biogenic iron oxyhydroxide (BIO). The suspended development of the BIO mineral structure is consistent with Fe(III) hydrolysis and polymerization in the presence of high concentrations of Fe-complexing ligands. We hypothesize that microbiologically produced Fe-complexing ligands may play critical roles in both the delivery of Fe(II) to oxidases, and the limited Fe(III) oxyhydroxide crystallinity observed within the biofilm. Our research provides insight into the structure and formation of naturally occurring, microbiologically produced Fe oxyhydroxide minerals in the deep-sea. We describe the initiation of microbial seafloor weathering, and the morphological and mineralogical signals that result from that process. Our observations provide a starting point from which progressively older and more extensively weathered seafloor sulfide minerals may be examined, with the ultimate goal of improved interpretation of ancient microbial processes and associated biological signatures. 相似文献
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Zinc sorption to biogenic hexagonal-birnessite particles within a hydrated bacterial biofilm 总被引：3，自引：0，他引：3
Biofilm-embedded Mn oxides exert important controls on trace metal cycling in aquatic and soil environments. The speciation and mobility of Zn in particular has been linked to Mn oxides found in streams, wetlands, soils, and aquifers. We investigated the mechanisms of Zn sorption to a biogenic Mn oxide within a biofilm produced by model soil and freshwater MnII-oxidizing bacteria Pseudomonas putida. The biogenic Mn oxide is a c-disordered birnessite with hexagonal layer symmetry. Zinc adsorption isotherm and Zn and Mn K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy experiments were conducted at pH 6.9 to characterize Zn sorption to this biogenic Mn oxide, and to determine whether the bioorganic components of the biofilm affect metal sorption properties. The EXAFS data were analyzed by spectral fitting, principal component analysis, and linear least-squares fitting with reference spectra. Zinc speciation was found to change as Zn loading to the biosorbent [bacterial cells, extracellular polymeric substances (EPS), and biogenic Mn oxide] increased. At low Zn loading (0.13 ± 0.04 mol Zn kg−1 biosorbent), Zn was sorbed to crystallographically well-defined sites on the biogenic oxide layers in tetrahedral coordination to structural O atoms. The fit to the EXAFS spectrum was consistent with Zn sorption above and below the MnIV vacancy sites of the oxide layers. As Zn loading increased to 0.72 ± 0.04 mol Zn kg−1 biosorbent, Zn was also detected in octahedral coordination to these sites. Overall, our results indicate that the biofilm did not intervene in Zn sorption by the Mn-oxide because sorption to the organic material was observed only after all Mn vacancy sites were capped by Zn. The organic functional groups present in the biofilm contributed significantly to Zn removal from solution when Zn concentrations exceeded the sorption capacity of the biooxide. At the highest Zn loading studied, 1.50 ± 0.36 mol Zn kg−1 biosorbent, the proportion of total Zn sorption attributed to bioorganic material was 38 mol%. The maximum Zn loading to the biogenic oxide that we observed was 4.1 mol Zn kg−1 biogenic Mn oxide, corresponding to 0.37 ± 0.02 mol Zn mol−1 Mn. This loading is in excellent agreement with previous estimates of the content of cation vacancies in the biogenic oxide. The results of this study improve our knowledge of Zn speciation in natural systems and are consistent with those of Zn speciation in mineral soil fractions and ferromanganese nodules where the Mn oxides present are possibly biogenic. 相似文献
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