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Title: Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba x,Sr 1-x )SO 4 from undersaturated solution

Abstract

Sr-bearing marine barite [(Ba x, Sr 1-x)SO 4] cycling has been widely used to reconstruct geochemical evolutions of paleoenvironments. However, an understanding of barite precipitation in the ocean, which is globally undersaturated with respect to barite, is missing. Moreover, the reason for the occurrence of higher Sr content in marine barites than expected for classical crystal growth processes remains unknown. Field data analyses suggested that organic molecules may regulate the formation and composition of marine barites; however, the specific organic–mineral interactions are unclear. Using in situ grazing incidence small-angle X-ray scattering (GISAXS), size and total volume evolutions of barite precipitates on organic films were characterized. The results show that barite forms on organic films from undersaturated solutions. Moreover, from a single supersaturated solution with respect to barite, Sr-rich barite nanoparticles formed on organics, while micrometer-size Sr-poor barites formed in bulk solutions. Ion adsorption experiments showed that organic films can enrich cation concentrations in the adjacent solution, thus increasing the local supersaturation and promoting barite nucleation on organic films, even when the bulk solution was undersaturated. The Sr enrichment in barites formed on organic films was found to be controlled by solid-solution nucleation rates; instead, the Sr-poor barite formation in bulkmore » solution was found to be controlled by solid-solution growth rates. This study provides a mechanistic explanation for Sr-rich marine barite formation and offers insights for understanding and controlling the compositions of solid solutions by separately tuning their nucleation and growth rates via the unique chemistry of solution–organic interfaces.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [1];  [3]; ORCiD logo [1]
  1. Univ. of Houston, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1546500
Alternate Identifier(s):
OSTI ID: 1542993
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 116; Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Deng, Ning, Stack, Andrew G., Weber, Juliane, Cao, Bo, De Yoreo, James, and Hu, Yandi. Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax,Sr1-x )SO4 from undersaturated solution. United States: N. p., 2019. Web. doi:10.1073/pnas.1821065116.
Deng, Ning, Stack, Andrew G., Weber, Juliane, Cao, Bo, De Yoreo, James, & Hu, Yandi. Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax,Sr1-x )SO4 from undersaturated solution. United States. doi:10.1073/pnas.1821065116.
Deng, Ning, Stack, Andrew G., Weber, Juliane, Cao, Bo, De Yoreo, James, and Hu, Yandi. Tue . "Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax,Sr1-x )SO4 from undersaturated solution". United States. doi:10.1073/pnas.1821065116.
@article{osti_1546500,
title = {Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax,Sr1-x )SO4 from undersaturated solution},
author = {Deng, Ning and Stack, Andrew G. and Weber, Juliane and Cao, Bo and De Yoreo, James and Hu, Yandi},
abstractNote = {Sr-bearing marine barite [(Bax, Sr1-x)SO4] cycling has been widely used to reconstruct geochemical evolutions of paleoenvironments. However, an understanding of barite precipitation in the ocean, which is globally undersaturated with respect to barite, is missing. Moreover, the reason for the occurrence of higher Sr content in marine barites than expected for classical crystal growth processes remains unknown. Field data analyses suggested that organic molecules may regulate the formation and composition of marine barites; however, the specific organic–mineral interactions are unclear. Using in situ grazing incidence small-angle X-ray scattering (GISAXS), size and total volume evolutions of barite precipitates on organic films were characterized. The results show that barite forms on organic films from undersaturated solutions. Moreover, from a single supersaturated solution with respect to barite, Sr-rich barite nanoparticles formed on organics, while micrometer-size Sr-poor barites formed in bulk solutions. Ion adsorption experiments showed that organic films can enrich cation concentrations in the adjacent solution, thus increasing the local supersaturation and promoting barite nucleation on organic films, even when the bulk solution was undersaturated. The Sr enrichment in barites formed on organic films was found to be controlled by solid-solution nucleation rates; instead, the Sr-poor barite formation in bulk solution was found to be controlled by solid-solution growth rates. This study provides a mechanistic explanation for Sr-rich marine barite formation and offers insights for understanding and controlling the compositions of solid solutions by separately tuning their nucleation and growth rates via the unique chemistry of solution–organic interfaces.},
doi = {10.1073/pnas.1821065116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 27,
volume = 116,
place = {United States},
year = {2019},
month = {5}
}

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    Works referencing / citing this record:

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    journal, July 1993

    • Henke, B. L.; Gullikson, E. M.; Davis, J. C.
    • Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342
    • DOI: 10.1006/adnd.1993.1013

    Celestine in a sulfidic spring barite deposit - A potential biomarker?
    journal, November 2016


    The saturation state of the world’s ocean with respect to (Ba,Sr)SO4 solid solutions
    journal, July 2006


    Stable strontium isotope fractionation in synthetic barite
    journal, December 2014

    • Widanagamage, Inoka H.; Schauble, Edwin A.; Scher, Howie D.
    • Geochimica et Cosmochimica Acta, Vol. 147
    • DOI: 10.1016/j.gca.2014.10.004

    Inner- and outer-sphere complexation of ions at the goethite–solution interface
    journal, May 2006

    • Rahnemaie, Rasoul; Hiemstra, Tjisse; van Riemsdijk, Willem H.
    • Journal of Colloid and Interface Science, Vol. 297, Issue 2
    • DOI: 10.1016/j.jcis.2005.11.003

    Determination of thiol functional groups on bacteria and natural organic matter in environmental systems
    journal, February 2014


    Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging
    journal, July 2018

    • Weber, Juliane; Bracco, Jacquelyn N.; Poplawsky, Jonathan D.
    • Crystal Growth & Design, Vol. 18, Issue 9
    • DOI: 10.1021/acs.cgd.8b00839

    Small Angle X-ray Scattering for Nanoparticle Research
    journal, April 2016


    Homogeneous and Heterogeneous (Fe x , Cr 1– x )(OH) 3 Precipitation: Implications for Cr Sequestration
    journal, January 2016

    • Dai, Chong; Zuo, Xiaobing; Cao, Bo
    • Environmental Science & Technology, Vol. 50, Issue 4
    • DOI: 10.1021/acs.est.5b04319

    Heterogeneous Ni- and Cd-Bearing Ferrihydrite Precipitation and Recrystallization on Quartz under Acidic pH Condition
    journal, November 2017


    Heterogeneous Lead Phosphate Nucleation at Organic–Water Interfaces: Implications for Lead Immobilization
    journal, July 2018


    In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping
    journal, June 2012

    • Fernandez-Martinez, Alejandro; Hu, Yandi; Lee, Byeongdu
    • Environmental Science & Technology, Vol. 47, Issue 1
    • DOI: 10.1021/es3014826

    Control of Heterogeneous Fe(III) (Hydr)oxide Nucleation and Growth by Interfacial Energies and Local Saturations
    journal, August 2013

    • Hu, Yandi; Neil, Chelsea; Lee, Byeongdu
    • Environmental Science & Technology, Vol. 47, Issue 16
    • DOI: 10.1021/es401160g

    Aluminum Affects Heterogeneous Fe(III) (Hydr)oxide Nucleation, Growth, and Ostwald Ripening
    journal, December 2013

    • Hu, Yandi; Li, Qingyun; Lee, Byeongdu
    • Environmental Science & Technology, Vol. 48, Issue 1
    • DOI: 10.1021/es403777w

    Fe(III) Hydroxide Nucleation and Growth on Quartz in the Presence of Cu(II), Pb(II), and Cr(III): Metal Hydrolysis and Adsorption
    journal, December 2014

    • Dai, Chong; Hu, Yandi
    • Environmental Science & Technology, Vol. 49, Issue 1
    • DOI: 10.1021/es504140k

    Dynamics and Structure of Hydration Water on Rutile and Cassiterite Nanopowders Studied by Quasielastic Neutron Scattering and Molecular Dynamics Simulations
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    • Mamontov, E.; Vlcek, L.; Wesolowski, D. J.
    • The Journal of Physical Chemistry C, Vol. 111, Issue 11
    • DOI: 10.1021/jp067242r

    Environmentally Abundant Anions Influence the Nucleation, Growth, Ostwald Ripening, and Aggregation of Hydrous Fe(III) Oxides
    journal, May 2012

    • Hu, Yandi; Lee, Byeongdu; Bell, Christopher
    • Langmuir, Vol. 28, Issue 20
    • DOI: 10.1021/la300791w

    Marine barite as a monitor of seawater strontium isotope composition
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    • Paytan, A.; Kastner, M.; Martin, E. E.
    • Nature, Vol. 366, Issue 6454
    • DOI: 10.1038/366445a0

    Sponge-associated bacteria mineralize arsenic and barium on intracellular vesicles
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    • Keren, Ray; Mayzel, Boaz; Lavy, Adi
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14393

    Calcium carbonate nucleation driven by ion binding in a biomimetic matrix revealed by in situ electron microscopy
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    • Smeets, Paul J. M.; Cho, Kang Rae; Kempen, Ralph G. E.
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    • DOI: 10.1038/nmat4193

    Pelagic barite precipitation at micromolar ambient sulfate
    journal, November 2017


    Barium bioaccumulation by bacterial biofilms and implications for Ba cycling and use of Ba proxies
    journal, April 2018


    Preparation of homodisperse solids
    journal, January 1986


    Anomalous grazing incidence small-angle x-ray scattering studies of platinum nanoparticles formed by cluster deposition
    journal, August 2005

    • Lee, Byeongdu; Seifert, Sönke; Riley, Stephen J.
    • The Journal of Chemical Physics, Vol. 123, Issue 7
    • DOI: 10.1063/1.1999627

    Carboxylated molecules regulate magnesium content of amorphous calcium carbonates during calcification
    journal, December 2009

    • Wang, D.; Wallace, A. F.; De Yoreo, J. J.
    • Proceedings of the National Academy of Sciences, Vol. 106, Issue 51
    • DOI: 10.1073/pnas.0906741106

    Initial stages of calcium uptake and mineral deposition in sea urchin embryos
    journal, December 2013

    • Vidavsky, N.; Addadi, S.; Mahamid, J.
    • Proceedings of the National Academy of Sciences, Vol. 111, Issue 1
    • DOI: 10.1073/pnas.1312833110

    Nanometer-Scale Chemistry of a Calcite Biomineralization Template: Implications for Skeletal Composition and Nucleation
    journal, October 2016

    • Branson, Oscar; Bonnin, Elisa A.; Perea, Daniel E.
    • Proceedings of the National Academy of Sciences, Vol. 113, Issue 46
    • DOI: 10.1073/pnas.1522864113

    Directed nucleation and growth by balancing local supersaturation and substrate/nucleus lattice mismatch
    journal, March 2018

    • Li, L.; Fijneman, A. J.; Kaandorp, J. A.
    • Proceedings of the National Academy of Sciences, Vol. 115, Issue 14
    • DOI: 10.1073/pnas.1712911115

    Barite in the ocean - occurrence, geochemistry and palaeoceanographic applications
    journal, March 2012


    How well suited are current thermodynamic models to predict or interpret the composition of (Ba,Sr)SO4 solid-solutions in geothermal scalings?
    journal, June 2017


    Morphological and compositional evidence for biotic precipitation of marine barite
    journal, May 1997


    The Organic-Mineral Interface in Biominerals
    journal, January 2005

    • Gilbert, P. U. P. A.
    • Reviews in Mineralogy and Geochemistry, Vol. 59, Issue 1
    • DOI: 10.2138/rmg.2005.59.7

    Thermodynamics of Solid Solution-Aqueous Solution Systems
    journal, January 2009


    Organic interfaces enhance strontium content of marine barite
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    • Wallace, Adam F.
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 27
    • DOI: 10.1073/pnas.1908013116