Mineralogical, magnetic and geochemical data constrain the pathways and extent of weathering of mineralized sedimentary rocks

Carrero, Sergio; Slotznick, Sarah P.; Fakra, Sirine C.; Sitar, M. Cole; Bone, Sharon E.; Mauk, Jeffrey L.; Manning, Andrew H.; Swanson-Hysell, Nicholas L.; Williams, Kenneth H.; Banfield, Jillian F.; Gilbert, Benjamin

doi:10.1016/j.gca.2022.11.005

Mineralogical, magnetic and geochemical data constrain the pathways and extent of weathering of mineralized sedimentary rocks

Journal Article · Fri Nov 11 00:00:00 EST 2022 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2022.11.005· OSTI ID:2282492

Carrero, Sergio ^[1]; Slotznick, Sarah P. ^[2]; Fakra, Sirine C. ^[3]; Sitar, M. Cole ^[4]; Bone, Sharon E. ^[5]; Mauk, Jeffrey L. ^[6]; Manning, Andrew H. ^[6]; Swanson-Hysell, Nicholas L. ^[7]; Williams, Kenneth H. ^[8]; Banfield, Jillian F. ^[9]; Gilbert, Benjamin ^[9]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Energy Geoscience Division; University of California, Berkeley, CA (United States); Institute of Environmental Assessment and Water Research, (IDAEA-CSIC), Barcelona (Spain)
University of California, Berkeley, CA (United States); Dartmouth College, Hanover, NH (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Energy Geoscience Division
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
US Geological Survey, Denver, CO (United States)
University of California, Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Energy Geoscience Division; Rocky Mountain Biological Laboratory, Gothic, CO (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Energy Geoscience Division; University of California, Berkeley, CA (United States)

The oxidative weathering of sulfidic rock can profoundly impact watersheds through the resulting export of acidity and metals. Weathering leaves a record of mineral transformation, particularly involving minor redox-sensitive phases, that can inform the development of conceptual and quantitative models. In sulfidic sedimentary rocks, however, variations in depositional history, diagenesis and mineralization can change or overprint the distributions of these trace minerals, complicating the interpretation of weathering signatures. Here we show that a combination of bulk mineralogical and geochemical techniques, micrometer-resolution X-ray fluorescence microprobe analysis and rock magnetic measurements, applied to drill core samples and single weathered fractures, can provide data that enable the development of a geochemically consistent weathering model. This work focused on one watershed in the Upper Colorado River Basin sitting within the Mesaverde Formation, a sedimentary sandstone bedrock with disseminated sulfide minerals, including pyrite and sphalerite, that were introduced during diagenesis and subsequent magmatic-hydrothermal mineralization. Combined analytical methods revealed the pathways of iron (Fe), carbonate and silicate mineral weathering and showed how pH controls element retention or release from the actively weathering fractured sandstone. Drill core logging, whole rock X-ray diffraction, and geochemical measurements document the progression from unweathered rock at depth to weathered rock at the surface. X-ray microprobe analyses of a 1-cm size weathering profile along a fracture surface are consistent with the mobilization of Fe(II) and Fe(III) into acidic pore water from the dissolution of primary pyrite, Fe-sphalerite, chlorite, and minor siderite and pyrrhotite. These reactions are followed by the precipitation of secondary minerals such as of goethite and jarosite, a Fe-(oxyhydr)oxide and hydrous Fe(III) sulfate, respectively. Microscale analyses also helped explain the weathering reactions responsible for the mineralogical transformations observed in the top and most weathered section of the drill core. For example, dissolution of feldspar and chlorite neutralizes the acidity generated by Fe and sulfide mineral oxidation, oversaturating the solution in both Fe-oxides. The combination of X-ray spectromicroscopy and magnetic measurements show that the Fe(III) product is goethite, mainly present either as a coating on fracture surfaces in the actively weathering region of the core or more homogeneously contained within the unconsolidated regolith at the top of the core. Low-temperature magnetic data reveal the presence of ferromagnetic Fe-sulfide pyrrhotite that, although it occurs at trace concentrations, could provide a qualitative proxy for unweathered sulfide minerals because the loss of pyrrhotite is associated with the onset of oxidative weathering. Pyrrhotite loss and goethite formation are detectable through room-temperature magnetic coercivity changes, suggesting that rock magnetic measurements can determine weathering intensity in rock samples at many scales. In conclusion, this work contributes evidence that the weathering of sulfidic sedimentary rocks follows a geochemical pattern in which the abundance of sulfide minerals controls the generation of acidity and dissolved elements, and the pH-dependent mobility of these elements controls their export to the ground- and surface-water.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 2282492

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Vol. 343; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Constraints on Neoproterozoic paleogeography and Paleozoic orogenesis from paleomagnetic records of the Bitter Springs Formation, Amadeus Basin, central Australia Swanson-Hysell, N. L.; Maloof, A. C.; Kirschvink, J. L. American Journal of Science, Vol. 312, Issue 8 https://doi.org/10.2475/08.2012.01	journal	October 2012
Oxidative dissolution under the channel leads geomorphological evolution at the Shale Hills catchment Sullivan, Pamela L.; Hynek, Scott A.; Gu, Xin American Journal of Science, Vol. 316, Issue 10 https://doi.org/10.2475/10.2016.02	journal	December 2016
Global chemical weathering of surficial rocks estimated from river dissolved loads Meybeck, M. American Journal of Science, Vol. 287, Issue 5 https://doi.org/10.2475/ajs.287.5.401	journal	May 1987
A New Tool for Separating the Magnetic Mineralogy of Complex Mineral Assemblages from Low Temperature Magnetic Behavior Lagroix, France; Guyodo, Yohan Frontiers in Earth Science, Vol. 5 https://doi.org/10.3389/feart.2017.00061	journal	July 2017
Iron Transformation Pathways and Redox Micro-Environments in Seafloor Sulfide-Mineral Deposits: Spatially Resolved Fe XAS and δ57/54Fe Observations Toner, Brandy M.; Rouxel, Olivier J.; Santelli, Cara M. Frontiers in Microbiology, Vol. 7 https://doi.org/10.3389/fmicb.2016.00648	journal	May 2016
Spatio-Temporal Shifts in Magmatism and Mineralization in Northern Colorado Beginning in the Late Eocene Rosera, Joshua M.; Gaynor, Sean P.; Coleman, Drew S. Economic Geology, Vol. 116, Issue 4 https://doi.org/10.5382/econgeo.4815	journal	June 2021

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58 GEOSCIENCES
High-resolution X-ray fluorescence
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