54 research outputs found
Reaction of Water-Saturated Supercritical CO2 with Forsterite: Evidence for Magnesite Formation at Low Temperatures
Recommended from our members
Protein–Mineral Interactions: Molecular Dynamics Simulations Capture Importance of Variations in Mineral Surface Composition and Structure
Molecular dynamics simulations, conventional and metadynamics, were performed to determine the interaction of model protein Gb1 over kaolinite (001), Na⁺-montmorillonite (001), Ca²⁺-montmorillonite (001), goethite (100), and Na⁺-birnessite (001) mineral surfaces. Gb1, a small (56 residue) protein with a well-characterized solution-state nuclear magnetic resonance (NMR) structure and having α-helix, 4-fold β-sheet, and hydrophobic core features, is used as a model protein to study protein soil mineral interactions and gain insights on structural changes and potential degradation of protein. From our simulations, we observe little change to the hydrated Gb1 structure over the kaolinite, montmorillonite, and goethite surfaces relative to its solvated structure without these mineral surfaces present. Over the Na⁺ -birnessite basal surface, however, the Gb1 structure is highly disturbed as a result of interaction with this birnessite surface. Unraveling of the Gb1 β-sheet at specific turns and a partial unraveling of the α-helix is observed over birnessite, which suggests specific vulnerable residue sites for oxidation or hydrolysis possibly leading to fragmentation
Uranium in Hanford Site 300 Area: Extraction Data on Borehole Sediments
In this study, sediments collected from boreholes drilled in 2010 and 2011 as part of a remedial investigation/feasibility study were characterized. The wells, located within or around two process ponds and one process trench waste site, were characterized in terms of total uranium concentration, mobile fraction of uranium, particle size, and moisture content along the borehole depth. In general, the gravel-dominated sediments of the vadose zone Hanford formation in all investigated boreholes had low moisture contents. Based on total uranium content, a total of 48 vadose zone and periodically rewetted zone sediment samples were selected for more detailed characterization, including measuring the concentration of uranium extracted with 8 M nitric acid, and leached using bicarbonate mixed solutions to determine the liable uranium (U(VI)) contents. In addition, water extraction was conducted on 17 selected sediments. Results from the sediment acid and bicarbonate extractions indicated the total concentrations of anthropogenic labile uranium in the sediments varied among the investigated boreholes. The peak uranium concentration (114.84 µg/g, acid extract) in <2-mm size fractions was found in borehole 399 1-55, which was drilled directly in the southwest corner of the North Process Pond. Lower uranium concentrations (~0.3–2.5 µg/g, acid extract) in <2-mm size fractions were found in boreholes 399-1-57, 399-1-58, and 399-1-59, which were drilled either near the Columbia River or inland and upgradient of any waste process ponds or trenches. A general trend of “total” uranium concentrations was observed that increased as the particle size decreased when relating the sediment particle size and acid extractable uranium concentrations in two selected sediment samples. The labile uranium bicarbonate leaching kinetic experiments on three selected sediments indicated a two-step leaching rate: an initial rapid release, followed by a slow continual release of uranium from the sediment. Based on the uranium leaching kinetic results, quasi equilibrium can be assumed after 1000-h batch reaction time in this study
Recommended from our members
Kinetic Controls on the Desorption/Dissolution of Sorbed U(VI) and Their Influence on Reactive Transport
Elemental Composition of Natural Nanoparticles and Fine Colloids in European Forest Stream Waters and Their Role as Phosphorus Carriers
"This is the peer reviewed version of the following article: Gottselig, N., W. Amelung, J. W. Kirchner, R. Bol, W. Eugster, S. J. Granger, C. Hernández-Crespo, et al. 2017. Elemental Composition of Natural Nanoparticles and Fine Colloids in European Forest Stream Waters and Their Role as Phosphorus Carriers. Global Biogeochemical Cycles 31 (10). American Geophysical Union (AGU): 1592 1607. doi:10.1002/2017gb005657, which has been published in final form at https://doi.org/10.1002/2017GB005657. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving."[EN] Biogeochemical cycling of elements largely occurs in dissolved state, but many elements may also be bound to natural nanoparticles (NNP, 1-100 nm) and fine colloids (100-450 nm). We examined the hypothesis that the size and composition of stream water NNP and colloids vary systematically across Europe. To test this hypothesis, 96 stream water samples were simultaneously collected in 26 forested headwater catchments along two transects across Europe. Three size fractions (similar to 1-20 nm, >20-60 nm, and >60 nm) of NNP and fine colloids were identified with Field Flow Fractionation coupled to inductively coupled plasma mass spectrometry and an organic carbon detector. The results showed that NNP and fine colloids constituted between 2 +/- 5% (Si) and 53 +/- 21% (Fe; mean +/- SD) of total element concentrations, indicating a substantial contribution of particles to element transport in these European streams, especially for P and Fe. The particulate contents of Fe, Al, and organic C were correlated to their total element concentrations, but those of particulate Si, Mn, P, and Ca were not. The fine colloidal fractions >60 nm were dominated by clay minerals across all sites. The resulting element patterns of NNP <60 nm changed from North to South Europe from Fe-to Ca-dominated particles, along with associated changes in acidity, forest type, and dominant lithology.The authors gratefully acknowledge the assistance of the following people in locating suitable sampling sites, contacting site operators, performing the sampling, and providing data: A. Avila Castells (Autonomous University of Barcelona), R. Batalla (University of Lleida), P. Blomkvist (Swedish University of Agricultural Sciences), H. Bogena (Julich Research Center), A.K. Boulet (University of Aveiro), D. Estany (University of Lleida), F. Garnier (French National Institute of Agricultural Research), H.J. Hendricks-Franssen (Research Center Julich), L. JacksonBlake (James Hutton Institute, NIVA), T. Laurila (Finnish Meteorological Institute), A. Lindroth (Lund University), M.M. Monerris (Universitat Politecnica de Valencia), M. Ottosson Lofvenius (Swedish University of Agricultural Sciences), I. Taberman (Swedish University of Agricultural Sciences), F. Wendland (Research Center Julich), T. Zetterberg (Swedish University of Agricultural Sciences and The Swedish Environmental Research Institute, IVL) and further unnamed contributors. The Swedish Infrastructure for Ecosystem Science (SITES) and the Swedish Integrated Monitoring, the latter financed by the Swedish Environmental Protection Agency, and ICOS Sweden have supported sampling and provided data for the Swedish sites. J.J.K. gratefully acknowledges the support from CESAM (UID/AMB/50017/2013), funded by the FCT/MCTES (PIDDAC) with cofunding by FEDER through COMPETE. N.G. gratefully acknowledges all those who contributed to organizing and implementing the continental sampling. The raw data can be found at http://hdl.handle.net/2128/14937. This project was partly funded by the German Research Foundation (DFG KL2495/1-1).Gottselig, N.; Amelung, W.; Kirchner, J.; Bol, R.; Eugster, W.; Granger, S.; Hernández Crespo, C.... (2017). Elemental Composition of Natural Nanoparticles and Fine Colloids in European Forest Stream Waters and Their Role as Phosphorus Carriers. Global Biogeochemical Cycles. 31(10):1592-1607. https://doi.org/10.1002/2017GB005657S159216073110Baken, S., Moens, C., van der Grift, B., & Smolders, E. (2016). Phosphate binding by natural iron-rich colloids in streams. Water Research, 98, 326-333. doi:10.1016/j.watres.2016.04.032Baken, S., Regelink, I. C., Comans, R. N. J., Smolders, E., & Koopmans, G. F. (2016). Iron-rich colloids as carriers of phosphorus in streams: A field-flow fractionation study. Water Research, 99, 83-90. doi:10.1016/j.watres.2016.04.060Benedetti, M. F., Van Riemsdijk, W. H., Koopal, L. K., Kinniburgh, D. G., Gooddy, D. C., & Milne, C. J. (1996). Metal ion binding by natural organic matter: From the model to the field. Geochimica et Cosmochimica Acta, 60(14), 2503-2513. doi:10.1016/0016-7037(96)00113-5Binkley, D., Ice, G. G., Kaye, J., & Williams, C. A. (2004). NITROGEN AND PHOSPHORUS CONCENTRATIONS IN FOREST STREAMS OF THE UNITED STATES. Journal of the American Water Resources Association, 40(5), 1277-1291. doi:10.1111/j.1752-1688.2004.tb01586.xBishop, K., Buffam, I., Erlandsson, M., Fölster, J., Laudon, H., Seibert, J., & Temnerud, J. (2008). Aqua Incognita: the unknown headwaters. Hydrological Processes, 22(8), 1239-1242. doi:10.1002/hyp.7049Bol, R., Julich, D., Brödlin, D., Siemens, J., Kaiser, K., Dippold, M. A., … Hagedorn, F. (2016). Dissolved and colloidal phosphorus fluxes in forest ecosystems-an almost blind spot in ecosystem research. Journal of Plant Nutrition and Soil Science, 179(4), 425-438. doi:10.1002/jpln.201600079Buffle, J., & Leppard, G. G. (1995). Characterization of Aquatic Colloids and Macromolecules. 2. Key Role of Physical Structures on Analytical Results. Environmental Science & Technology, 29(9), 2176-2184. doi:10.1021/es00009a005Celi, L., & Barberis, E. (s. f.). Abiotic stabilization of organic phosphorus in the environment. Organic phosphorus in the environment, 113-132. doi:10.1079/9780851998220.0113Dahlqvist, R., Benedetti, M. F., Andersson, K., Turner, D., Larsson, T., Stolpe, B., & Ingri, J. (2004). Association of calcium with colloidal particles and speciation of calcium in the Kalix and Amazon rivers. Geochimica et Cosmochimica Acta, 68(20), 4059-4075. doi:10.1016/j.gca.2004.04.007Darch, T., Blackwell, M. S. A., Hawkins, J. M. B., Haygarth, P. M., & Chadwick, D. (2014). A Meta-Analysis of Organic and Inorganic Phosphorus in Organic Fertilizers, Soils, and Water: Implications for Water Quality. Critical Reviews in Environmental Science and Technology, 44(19), 2172-2202. doi:10.1080/10643389.2013.790752Dynesius, M., & Nilsson, C. (1994). Fragmentation and Flow Regulation of River Systems in the Northern Third of the World. Science, 266(5186), 753-762. doi:10.1126/science.266.5186.753Erickson, H. P. (2009). Size and Shape of Protein Molecules at the Nanometer Level Determined by Sedimentation, Gel Filtration, and Electron Microscopy. Biological Procedures Online, 11(1), 32-51. doi:10.1007/s12575-009-9008-xEspinosa, M., Turner, B. L., & Haygarth, P. M. (1999). Preconcentration and Separation of Trace Phosphorus Compounds in Soil Leachate. Journal of Environmental Quality, 28(5), 1497-1504. doi:10.2134/jeq1999.00472425002800050015xFernández-Martínez, M., Vicca, S., Janssens, I. A., Sardans, J., Luyssaert, S., Campioli, M., … Peñuelas, J. (2014). Nutrient availability as the key regulator of global forest carbon balance. Nature Climate Change, 4(6), 471-476. doi:10.1038/nclimate2177Giddings, J., Yang, F., & Myers, M. (1976). Flow-field-flow fractionation: a versatile new separation method. Science, 193(4259), 1244-1245. doi:10.1126/science.959835Gimbert, L. J., Andrew, K. N., Haygarth, P. M., & Worsfold, P. J. (2003). Environmental applications of flow field-flow fractionation (FIFFF). TrAC Trends in Analytical Chemistry, 22(9), 615-633. doi:10.1016/s0165-9936(03)01103-8Gottselig, N., Bol, R., Nischwitz, V., Vereecken, H., Amelung, W., & Klumpp, E. (2014). Distribution of Phosphorus-Containing Fine Colloids and Nanoparticles in Stream Water of a Forest Catchment. Vadose Zone Journal, 13(7), vzj2014.01.0005. doi:10.2136/vzj2014.01.0005Gottselig, N., Nischwitz, V., Meyn, T., Amelung, W., Bol, R., Halle, C., … Klumpp, E. (2017). Phosphorus Binding to Nanoparticles and Colloids in Forest Stream Waters. Vadose Zone Journal, 16(3), vzj2016.07.0064. doi:10.2136/vzj2016.07.0064Hagedorn , A. G. 2006 EG-Sicherheitsdatenblatt (Gemäß 2001/58/EG)Hart, B. T., Douglas, G. B., Beckett, R., Van Put, A., & Van Grieken, R. E. (1993). Characterization of colloidal and particulate matter transported by the magela creek system, Northern Australia. Hydrological Processes, 7(1), 105-118. doi:10.1002/hyp.3360070111Hassellöv, M., Lyvén, B., Haraldsson, C., & Sirinawin, W. (1999). Determination of Continuous Size and Trace Element Distribution of Colloidal Material in Natural Water by On-Line Coupling of Flow Field-Flow Fractionation with ICPMS. Analytical Chemistry, 71(16), 3497-3502. doi:10.1021/ac981455yHassellov, M., & von der Kammer, F. (2008). Iron Oxides as Geochemical Nanovectors for Metal Transport in Soil-River Systems. Elements, 4(6), 401-406. doi:10.2113/gselements.4.6.401Hens, M., & Merckx, R. (2001). Functional Characterization of Colloidal Phosphorus Species in the Soil Solution of Sandy Soils. Environmental Science & Technology, 35(3), 493-500. doi:10.1021/es0013576Hill, D. M., & Aplin, A. C. (2001). Role of colloids and fine particles in the transport of metals in rivers draining carbonate and silicate terrains. Limnology and Oceanography, 46(2), 331-344. doi:10.4319/lo.2001.46.2.0331Jarvie, H. P., Neal, C., Rowland, A. P., Neal, M., Morris, P. N., Lead, J. R., … Hockenhull, K. (2012). Role of riverine colloids in macronutrient and metal partitioning and transport, along an upland–lowland land-use continuum, under low-flow conditions. Science of The Total Environment, 434, 171-185. doi:10.1016/j.scitotenv.2011.11.061Jiang, X., Bol, R., Nischwitz, V., Siebers, N., Willbold, S., Vereecken, H., … Klumpp, E. (2015). Phosphorus Containing Water Dispersible Nanoparticles in Arable Soil. Journal of Environmental Quality, 44(6), 1772-1781. doi:10.2134/jeq2015.02.0085Kögel-Knabner, I., & Amelung, W. (2014). Dynamics, Chemistry, and Preservation of Organic Matter in Soils. Treatise on Geochemistry, 157-215. doi:10.1016/b978-0-08-095975-7.01012-3Krám, P., Hruška, J., & Shanley, J. B. (2012). Streamwater chemistry in three contrasting monolithologic Czech catchments. Applied Geochemistry, 27(9), 1854-1863. doi:10.1016/j.apgeochem.2012.02.020Lyvén, B., Hassellöv, M., Turner, D. R., Haraldsson, C., & Andersson, K. (2003). Competition between iron- and carbon-based colloidal carriers for trace metals in a freshwater assessed using flow field-flow fractionation coupled to ICPMS. Geochimica et Cosmochimica Acta, 67(20), 3791-3802. doi:10.1016/s0016-7037(03)00087-5Marschner, B., & Kalbitz, K. (2003). Controls of bioavailability and biodegradability of dissolved organic matter in soils. Geoderma, 113(3-4), 211-235. doi:10.1016/s0016-7061(02)00362-2Martin, J.-M., Dai, M.-H., & Cauwet, G. (1995). Significance of colloids in the biogeochemical cycling of organic carbon and trace metals in the Venice Lagoon (Italy). Limnology and Oceanography, 40(1), 119-131. doi:10.4319/lo.1995.40.1.0119Mattsson, T., Kortelainen, P., Laubel, A., Evans, D., Pujo-Pay, M., Räike, A., & Conan, P. (2009). Export of dissolved organic matter in relation to land use along a European climatic gradient. Science of The Total Environment, 407(6), 1967-1976. doi:10.1016/j.scitotenv.2008.11.014Missong, A., Bol, R., Willbold, S., Siemens, J., & Klumpp, E. (2016). Phosphorus forms in forest soil colloids as revealed by liquid-state31P-NMR. Journal of Plant Nutrition and Soil Science, 179(2), 159-167. doi:10.1002/jpln.201500119Montalvo, D., Degryse, F., & McLaughlin, M. J. (2015). Natural Colloidal P and Its Contribution to Plant P Uptake. Environmental Science & Technology, 49(6), 3427-3434. doi:10.1021/es504643fNeubauer, E., Köhler, S. J., von der Kammer, F., Laudon, H., & Hofmann, T. (2013). Effect of pH and Stream Order on Iron and Arsenic Speciation in Boreal Catchments. Environmental Science & Technology, 47(13), 7120-7128. doi:10.1021/es401193jNeubauer, E., v.d. Kammer, F., & Hofmann, T. (2011). Influence of carrier solution ionic strength and injected sample load on retention and recovery of natural nanoparticles using Flow Field-Flow Fractionation. Journal of Chromatography A, 1218(38), 6763-6773. doi:10.1016/j.chroma.2011.07.010Nischwitz, V., & Goenaga-Infante, H. (2012). Improved sample preparation and quality control for the characterisation of titanium dioxide nanoparticles in sunscreens using flow field flow fractionation on-line with inductively coupled plasma mass spectrometry. Journal of Analytical Atomic Spectrometry, 27(7), 1084. doi:10.1039/c2ja10387gRan, Y., Fu, J. ., Sheng, G. ., Beckett, R., & Hart, B. . (2000). Fractionation and composition of colloidal and suspended particulate materials in rivers. Chemosphere, 41(1-2), 33-43. doi:10.1016/s0045-6535(99)00387-2Regelink, I. C., Koopmans, G. F., van der Salm, C., Weng, L., & van Riemsdijk, W. H. (2013). Characterization of Colloidal Phosphorus Species in Drainage Waters from a Clay Soil Using Asymmetric Flow Field-Flow Fractionation. Journal of Environmental Quality, 42(2), 464-473. doi:10.2134/jeq2012.0322Regelink, I. C., Voegelin, A., Weng, L., Koopmans, G. F., & Comans, R. N. J. (2014). Characterization of Colloidal Fe from Soils Using Field-Flow Fractionation and Fe K-Edge X-ray Absorption Spectroscopy. Environmental Science & Technology, 48(8), 4307-4316. doi:10.1021/es405330xRegelink, I. C., Weng, L., & van Riemsdijk, W. H. (2011). The contribution of organic and mineral colloidal nanoparticles to element transport in a podzol soil. Applied Geochemistry, 26, S241-S244. doi:10.1016/j.apgeochem.2011.03.114RICHARDSON, C. J. (1985). Mechanisms Controlling Phosphorus Retention Capacity in Freshwater Wetlands. Science, 228(4706), 1424-1427. doi:10.1126/science.228.4706.1424Roth , C. 2011 Sicherheitsdatenblatt Gemäß Verordnung (EG) Nr. 1907/2006 RepSchmitt, D., Taylor, H. E., Aiken, G. R., Roth, D. A., & Frimmel, F. H. (2002). Influence of Natural Organic Matter on the Adsorption of Metal Ions onto Clay Minerals. Environmental Science & Technology, 36(13), 2932-2938. doi:10.1021/es010271pSix, J., Elliott, E. T., & Paustian, K. (1999). Aggregate and Soil Organic Matter Dynamics under Conventional and No-Tillage Systems. Soil Science Society of America Journal, 63(5), 1350-1358. doi:10.2136/sssaj1999.6351350xStolpe, B., Guo, L., Shiller, A. M., & Hassellöv, M. (2010). Size and composition of colloidal organic matter and trace elements in the Mississippi River, Pearl River and the northern Gulf of Mexico, as characterized by flow field-flow fractionation. Marine Chemistry, 118(3-4), 119-128. doi:10.1016/j.marchem.2009.11.007Tipping, E., & Hurley, M. . (1992). A unifying model of cation binding by humic substances. Geochimica et Cosmochimica Acta, 56(10), 3627-3641. doi:10.1016/0016-7037(92)90158-fTombácz, E., Libor, Z., Illés, E., Majzik, A., & Klumpp, E. (2004). The role of reactive surface sites and complexation by humic acids in the interaction of clay mineral and iron oxide particles. Organic Geochemistry, 35(3), 257-267. doi:10.1016/j.orggeochem.2003.11.002Trostle, K. D., Ray Runyon, J., Pohlmann, M. A., Redfield, S. E., Pelletier, J., McIntosh, J., & Chorover, J. (2016). Colloids and organic matter complexation control trace metal concentration-discharge relationships in Marshall Gulch stream waters. Water Resources Research, 52(10), 7931-7944. doi:10.1002/2016wr019072U.S. Department of Agriculture 1993 Soil survey manual, chapter 3. Selected chemical propertiesVitousek, P. (1982). Nutrient Cycling and Nutrient Use Efficiency. The American Naturalist, 119(4), 553-572. doi:10.1086/283931Wells, M. L., & Goldberg, E. D. (1991). Occurrence of small colloids in sea water. Nature, 353(6342), 342-344. doi:10.1038/353342a0Wen, L.-S., Santschi, P., Gill, G., & Paternostro, C. (1999). Estuarine trace metal distributions in Galveston Bay: importance of colloidal forms in the speciation of the dissolved phase. Marine Chemistry, 63(3-4), 185-212. doi:10.1016/s0304-4203(98)00062-0Zirkler, D., Lang, F., & Kaupenjohann, M. (2012). «Lost in filtration»—The separation of soil colloids from larger particles. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 399, 35-40. doi:10.1016/j.colsurfa.2012.02.02
Advective Removal of Intraparticle Uranium from Contaminated Vadose Zone Sediments, Hanford, U.S.
420,000 year assessment of fault leakage rates shows geological carbon storage is secure
Carbon capture and storage (CCS) technology is routinely cited as a cost effective tool for climate change mitigation. CCS can directly reduce industrial CO2 emissions and is essential for the retention of CO2 extracted from the atmosphere. To be effective as a climate change mitigation tool, CO2 must be securely retained for 10,000 years (10 ka) with a leakage rate of below 0.01% per year of the total amount of CO2 injected. Migration of CO2 back to the atmosphere via leakage through geological faults is a potential high impact risk to CO2 storage integrity. Here, we calculate for the first time natural leakage rates from a 420 ka paleo-record of CO2 leakage above a naturally occurring, faulted, CO2 reservoir in Arizona, USA. Surface travertine (CaCO3) deposits provide evidence of vertical CO2 leakage linked to known faults. U-Th dating of travertine deposits shows leakage varies along a single fault and that individual seeps have lifespans of up to 200 ka. Whilst the total volumes of CO2 required to form the travertine deposits are high, time-averaged leakage equates to a linear rate of less than 0.01%/yr. Hence, even this natural geological storage site, which would be deemed to be of too high risk to be selected for engineered geologic storage, is adequate to store CO2 for climate mitigation purposes
Mineralização e nitrificação do nitrogênio proveniente da cama de aves aplicada ao solo
Strontium and Cesium Release Mechanisms during Unsaturated Flow through Waste-Weathered Hanford Sediments
- …