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Formation of Diagenetic Siderite in Modern Ferruginous Sediments Aurèle Vuillemin1,2*, Richard Wirth1, Helga Kemnitz1, Anja M

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Formation of Diagenetic Siderite in Modern Ferruginous Sediments Aurèle Vuillemin1,2*, Richard Wirth1, Helga Kemnitz1, Anja M https://doi.org/10.1130/G46100.1 Manuscript received 25 September 2018 Revised manuscript received 26 March 2019 Manuscript accepted 27 March 2019 © 2019 The Authors. Gold Open Access: This paper is published under the terms of the CC-BY license. Published online XX Month 2019 Formation of diagenetic siderite in modern ferruginous sediments Aurèle Vuillemin1,2*, Richard Wirth1, Helga Kemnitz1, Anja M. Schleicher1, André Friese1, Kohen W. Bauer3, Rachel Simister3, Sulung Nomosatryo1,4, Luis Ordoñez5, Daniel Ariztegui5, Cynthia Henny4, Sean A. Crowe3, Liane G. Benning1,6,7, Jens Kallmeyer1, James M. Russell8, Satria Bijaksana9, Hendrik Vogel10 and the Towuti Drilling Project Science Team† 1GFZ German Research Centre for Geosciences, Helmholtz Centre Potsdam, Telegrafenberg, 14473 Potsdam, Germany 2Present address: Department of Earth and Environmental Sciences, Paleontology and Geobiology, Ludwig-Maximilians-Universität, Richard-Wagner-Str. 10, 80333 Munich, Germany 3Department of Earth, Ocean, and Atmospheric Sciences, and of Microbiology and Immunology, University of British Columbia, 2350 Health Sciences Mall, Vancouver, BC V6T 1Z4, Canada 4Research Center for Limnology, Indonesian Institute of Sciences (LIPI), Jl. Raya Bogor, Cibinong, Bogor, West Java 16911, Indonesia 5Department of Earth Sciences, University of Geneva, rue des Maraîchers 13, 1205 Geneva, Switzerland 6Department of Earth Sciences, Free University of Berlin, 12249 Berlin, Germany 7School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK 8Department of Earth, Environmental, and Planetary Sciences, Brown University, 324 Brook Street, Providence, Rhode Island 02912, USA 9Faculty of Mining and Petroleum Engineering, Institut Teknologi Bandung, Jl. Ganesha 10, 40132 Bandung, Jawa Barat, Indonesia 10Institute of Geological Sciences & Oeschger Centre for Climate Change Research, University of Bern, Baltzerstrasse 1-3, 3012 Bern, Switzerland ABSTRACT and lateritic soils in the Malili Lakes catch- Ferruginous conditions prevailed in the world’s deep oceans during the Archean and ment supplies considerable amounts of iron Proterozoic Eons. Sedimentary iron formations deposited at that time may provide an impor- (oxyhydr)oxides but little sulfate to the lakes tant record of environmental conditions, yet linking the chemistry and mineralogy of these (Crowe et al., 2004; Morlock et al., 2019). Lake sedimentary rocks to depositional conditions remains a challenge due to a dearth of information Towuti (2°45′0″S, 121°30′0″E) is currently about the processes by which minerals form in analogous modern environments. We identified stratified with anoxic conditions below 130 m siderites in ferruginous Lake Towuti, Indonesia, which we characterized using high-resolution (Costa et al., 2015; Vuillemin et al., 2016). In microscopic and spectroscopic imaging combined with microchemical and geochemical analy- nearby Lake Matano (2°29′7″S, 121°20′0″E), ses. We infer early diagenetic growth of siderite crystals as a response to sedimentary organic carbonate green rust (GR) forms below the carbon degradation and the accumulation of dissolved inorganic carbon in pore waters. We chemo cline, likely via the reduction of ferri- suggest that siderite formation proceeds through syntaxial growth on preexisting siderite crys- hydrite or via its reaction with dissolved Fe2+ tals, or possibly through aging of precursor carbonate green rust. Crystal growth ultimately and bicarbonate (Zegeye et al., 2012), but the leads to spar-sized (>50 μm) mosaic single siderite crystals that form twins, bundles, and fate of this GR is not known. Although carbonate spheroidal aggregates during burial. Early-formed carbonate was detectable through micro- GR has been proposed as a precursor to other chemical zonation and the possible presence of residual phases trapped in siderite interstices. diagenetic mineral phases in banded iron forma- This suggests that such microchemical zonation and mineral inclusions may be used to infer tions (Halevy et al., 2017), its transformation to siderite growth histories in ancient sedimentary rocks including sedimentary iron formations. these phases has not been observed in nature. Prior studies suggested that iron phases in Lake INTRODUCTION ker et al., 2014), and their mineralogy has been Towuti sediments undergo dissolution during Ancient sedimentary iron formations (IFs) used to infer atmospheric and oceanic conditions reductive diagenesis, with secondary growth of are composed of diverse iron oxides, silicates, on early Earth (Holland, 2006). The interpre- diagenetic phases such as magnetite and siderite and carbonates that are thought to form through tation of IFs and their depositional conditions (Tamuntuan et al., 2015). However, siderite was diagenesis and subsequent metamorphism of depends on our knowledge of their mineral ori- not explicitly documented in that study, nor is primary ferric-ferrous (Fe3+-Fe2+) iron (oxyhydr) gins and formation pathways (Ohmoto et al., it clear where in the lake and sediment these oxide precipitates (Gole, 1980; Raiswell et al., 2004), which is limited in part due to scarcity minerals form. 2011). Yet iron carbonate minerals such as sider- of analogous ferruginous (Fe-rich, SO4-poor) We discovered spar-sized aggregates ite (FeCO3) are also thought to form as primary environments on Earth today (Konhauser et al., (>50 μm) of diagenetic siderite crystals in Lake pelagic precipitates (Canfield et al., 2008; Bek- 2005; Posth et al., 2014). Towuti sediments, and used detailed geochemi- Ferruginous sediments are deposited in the cal and mineralogical information to describe *E-mail: a.vuillemin@ lrz .uni -muenchen.de Malili Lakes, a chain of five interconnected tec- their features and infer pathways of formation. †University of Minnesota, https:// csdco .umn .edu tonic lakes on Sulawesi Island, Indonesia (Haff- We suggest that this siderite forms during dia- /project /lake -towuti -drilling -project -tdp. ner et al., 2001). Erosion of ultramafic rocks genesis through growth on preexisting primary CITATION: Vuilemin, A., et al., 2019, Formation of diagenetic siderite in modern ferruginous sediments: Geology, v. 47, p. 1–5, https:// doi .org /10 .1130 /G46100.1 Geological Society of America | GEOLOGY | Volume 47 | Number 6 | www.gsapubs.org 1 Downloaded from https://pubs.geoscienceworld.org/gsa/geology/article-pdf/doi/10.1130/G46100.1/4678804/g46100.pdf by Universitaetsbibliothek Bern user on 18 April 2019 6.2 m 82.6 m A B C 4 E 2 1 F 3 B A twinning 200 nm 200 nm 200 nm Figure 1. Top: Scanning merged D E F transmission electron crystals D 6 microscope (TEM) images C of siderite crystals from 6.2 m and 82.6 m 5 sediment depth with 2 μm 2 μm 200 nm 250200 nm 250200 nm close-ups of crystal pores (A–F); indexed selected 1 2 2020 3 4 5 6 111 020 1120 2110 022 151 1123 3.71 1011 area electron diffraction 18 1011 4. 0 2 2 (SAED) patterns for amor- 5 6 1102 7 0 . 7 .78 . 1 2 3 2 4 131 1010 3.5 3.55 4 0111 phous iron oxide (1), green 1344 1213 2.58 2.13 111 8 rust (2), siderite (3, 5) and 3.8 0111 magnetite (4, 6), and high- resolution SAED pattern amorphous green rust siderite rim magnetite siderite rim magnetite entire siderite obtained for the entire mosaic monocrystal of 6.2 m B siderite from 82.6 m depth. B amo g.r. Bottom: Bright-field TEM g.r. images of a siderite crystal g.r. from 6.2 m depth in scatter- ing intensity after siderite A sid subtraction. Close-ups 200 nm 5 nm 2 nm of crystal pores with the C corresponding images of C sid lattice fringes (A–D) illus- g.r. trate the interface between D g.r. amorphous iron oxide (amo), green rust (g.r.), siderite (sid) and nano- sid magnetite (mgt). Arrows 2 μm 200 nm 5 nm 2 nm point at interphases g.r. between phases. A D g.r. g.r. sid g.r. mgt g.r. mgt sid 200 nm 5 nm 2 nm 100 nm 5 nm 2 nm phases, including siderite and possibly carbonate trations, with some contribution of fluvially de- ing out the non-magnetic fraction with deionized GR. We hypothesize that the chemical and min- rived material (Hasberg et al., 2019; Morlock water. Siderite imaging and elemental analysis eralogical features of these siderites, and their ir- et al., 2019). were performed on a Zeiss Ultra 55 Plus field regular distribution down core, reflect changes in Here we focus on material recovered from emission scanning electron microscope (SEM) redox conditions in the pore water and sediment core catchers. In the field, core catchers were equipped with an energy-dispersive X-ray spec- over time, including non-steady-state diagenesis, packed into gas-tight aluminum foil bags flushed trometer (EDX). Electron-transparent foils were which likely results from variability in the burial with nitrogen gas and heat-sealed to keep them prepared with a FEI focused ion beam, imaged fluxes of ferric iron and organic matter. under anoxic conditions until mineral extraction. and analyzed on a FEI Tecnai G2 F20 X-Twin Pore water was retrieved on site using hydraulic transmission electron microscope (TEM). Struc- METHODS squeezers. Alkalinity, pH, and Fe2+ concentra- tural information was obtained via selected area Sediments were recovered using the Inter- tions were determined in the field via colorimet- electron diffraction (SAED) patterns or calcu- national Continental Scientific Drilling Pro- ric titration, potentiometry, and spectrophotom- lated from high-resolution lattice fringe im- gram Deep Lakes Drilling System (https:// etry, respectively. Major ions were analyzed at ages (HR-TEM). Freeze-dried powdered bulk www .icdp -online .org). Cores from the 113-m- GFZ Potsdam by ion chromatography. Dissolved sediments and siderite extracts were analyzed deep TDP-TOW15- 1A hole (https://csdco .umn inorganic carbon (DIC) was calculated from pH in glycerol using a PANalytical Empyrean X-ray .edu /project /lake -towuti -drilling -project -tdp), and alkalinity. Siderite crystals were retrieved diffractometer in a theta-theta configuration. A drilled in 156 m water depth, were split and via density separation and sorted by placing a complete description of all methods is available imaged at the Limnological Research Center neodymium magnet under the beaker and rins- in the GSA Data Repository1.
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