Long-Term 13C Uptake by 12C-Enriched Calcite
Abstract
Knowledge of the exchange of carbon isotopes between dissolved inorganic carbon and calcite minerals is of long-standing importance for the interpretation of sedimentary paleoclimate records and 14C transport in the geosphere. To assess the mechanism and rates of carbon isotope exchange, we equilibrated 12C-pure synthetic calcite particles in water, first in a glovebox and then in contact with atmospheric PCO2 and 13C/12C ratio, at two different temperatures. Cavity ring-down infrared spectroscopy δ13C measurements of the solid revealed sustained 13C incorporation for over a period of 500 days (21 °C) and 125 days (50 °C). We developed a quantitative model for recrystallization and isotope exchange, assuming that the interfacial free energy provides a thermodynamic driving force for the growth of larger particles at the expense of smaller ones. Furthermore, this Ostwald ripening model did not reproduce the kinetics of 13C uptake and required greater coarsening than observed. Rather, the data were best explained by a mechanism involving surface exchange and solid-phase diffusion of 13C into the particles with an inferred effective diffusion constant at 21 °C of about 10–25 m2/s. Although this work cannot rule out the possibility that structural or chemical aspects of the synthetic particles enabled faster 13C uptakemore »
- Authors:
-
- Univ. Grenoble Alpes and CNRS (France)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. Grenoble Alpes and CNRS (France); Kanchrapara College, West Bengal (India)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Agence Nationale pour la Gestion des Déchets Radioactifs (ANDRA), Chatenay-Malabry (France)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1832706
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Earth and Space Chemistry
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2472-3452
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbonate sediments; carbon isotope exchange; recrystallization; cavity ring-down spectroscopy; diffusion; carbon; calcite; inorganic carbon compounds; carbon isotopes
Citation Formats
Géhin, Antoine, Gilbert, Benjamin, Chakraborty, Sudipta, Stack, Andrew G., Allard, Lawrence F., Robinet, Jean-Charles, and Charlet, Laurent. Long-Term 13C Uptake by 12C-Enriched Calcite. United States: N. p., 2021.
Web. doi:10.1021/acsearthspacechem.0c00122.
Géhin, Antoine, Gilbert, Benjamin, Chakraborty, Sudipta, Stack, Andrew G., Allard, Lawrence F., Robinet, Jean-Charles, & Charlet, Laurent. Long-Term 13C Uptake by 12C-Enriched Calcite. United States. https://doi.org/10.1021/acsearthspacechem.0c00122
Géhin, Antoine, Gilbert, Benjamin, Chakraborty, Sudipta, Stack, Andrew G., Allard, Lawrence F., Robinet, Jean-Charles, and Charlet, Laurent. Wed .
"Long-Term 13C Uptake by 12C-Enriched Calcite". United States. https://doi.org/10.1021/acsearthspacechem.0c00122. https://www.osti.gov/servlets/purl/1832706.
@article{osti_1832706,
title = {Long-Term 13C Uptake by 12C-Enriched Calcite},
author = {Géhin, Antoine and Gilbert, Benjamin and Chakraborty, Sudipta and Stack, Andrew G. and Allard, Lawrence F. and Robinet, Jean-Charles and Charlet, Laurent},
abstractNote = {Knowledge of the exchange of carbon isotopes between dissolved inorganic carbon and calcite minerals is of long-standing importance for the interpretation of sedimentary paleoclimate records and 14C transport in the geosphere. To assess the mechanism and rates of carbon isotope exchange, we equilibrated 12C-pure synthetic calcite particles in water, first in a glovebox and then in contact with atmospheric PCO2 and 13C/12C ratio, at two different temperatures. Cavity ring-down infrared spectroscopy δ13C measurements of the solid revealed sustained 13C incorporation for over a period of 500 days (21 °C) and 125 days (50 °C). We developed a quantitative model for recrystallization and isotope exchange, assuming that the interfacial free energy provides a thermodynamic driving force for the growth of larger particles at the expense of smaller ones. Furthermore, this Ostwald ripening model did not reproduce the kinetics of 13C uptake and required greater coarsening than observed. Rather, the data were best explained by a mechanism involving surface exchange and solid-phase diffusion of 13C into the particles with an inferred effective diffusion constant at 21 °C of about 10–25 m2/s. Although this work cannot rule out the possibility that structural or chemical aspects of the synthetic particles enabled faster 13C uptake than could be observed in natural systems, this study adds to the body of the recent work, suggesting that fast exchange processes are possible, likely through grain boundaries and other defects.},
doi = {10.1021/acsearthspacechem.0c00122},
journal = {ACS Earth and Space Chemistry},
number = 5,
volume = 5,
place = {United States},
year = {Wed Apr 28 00:00:00 EDT 2021},
month = {Wed Apr 28 00:00:00 EDT 2021}
}
Works referenced in this record:
A new kinetic approach to modeling water-rock interaction: The role of nucleation, precursors, and Ostwald ripening
journal, October 1990
- Steefel, Carl I.; Van Cappellen, Philippe
- Geochimica et Cosmochimica Acta, Vol. 54, Issue 10
Retardation of dissolved radiocarbon through a carbonated matrix
journal, March 1985
- Garnier, Jean-Marie
- Geochimica et Cosmochimica Acta, Vol. 49, Issue 3
Sr isotopes and pore fluid chemistry in carbonate sediment of the Ontong Java Plateau: Calcite recrystallization rates and evidence for a rapid rise in seawater Mg over the last 10 million years
journal, August 2006
- Fantle, Matthew S.; DePaolo, Donald J.
- Geochimica et Cosmochimica Acta, Vol. 70, Issue 15
Sorption of inorganic 14C on to calcite, montmorillonite and soil
journal, January 1998
- Sheppard, S. C.; Ticknor, K. V.; Evenden, W. G.
- Applied Geochemistry, Vol. 13, Issue 1
Diffusion of Ca and Mg in calcite
journal, September 1999
- Fisler, Diana K.; Cygan, Randall T.
- American Mineralogist, Vol. 84, Issue 9
Isotopic approaches for quantifying the rates of marine burial diagenesis
journal, January 2010
- Fantle, M. S.; Maher, K. M.; DePaolo, D. J.
- Reviews of Geophysics, Vol. 48, Issue 3
A novel determination of calcite dissolution kinetics in seawater
journal, December 2015
- Subhas, Adam V.; Rollins, Nick E.; Berelson, William M.
- Geochimica et Cosmochimica Acta, Vol. 170
Precipitation of calcium carbonate
journal, December 1982
- Söhnel, O.; Mullin, J. W.
- Journal of Crystal Growth, Vol. 60, Issue 2
Biomineralization by particle attachment in early animals
journal, August 2019
- Gilbert, Pupa U. P. A.; Porter, Susannah M.; Sun, Chang-Yu
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 36
An experimental study of the diffusion of C and O in calcite in mixed CO2-H2O fluid
journal, August 2011
- Labotka, T. C.; Cole, D. R.; Fayek, M. J.
- American Mineralogist, Vol. 96, Issue 8-9
SELF-DIFFUSION OF Ca45 INTO CERTAIN CARBONATES
journal, January 1964
- Lahav, N.; Bolt, G. H.
- Soil Science, Vol. 97, Issue 5
Relationship between surface structure, growth mechanism, and trace element incorporation in calcite
journal, February 1995
- Paquette, Jeanne; Reeder, Richard J.
- Geochimica et Cosmochimica Acta, Vol. 59, Issue 4
Growth of Nanosized Calcite through Gas−Solid Carbonation of Nanosized Portlandite under Anisobaric Conditions
journal, September 2010
- Montes-Hernandez, G.; Daval, D.; Chiriac, R.
- Crystal Growth & Design, Vol. 10, Issue 11
Low temperature stable mineral recrystallization of foraminiferal tests and implications for the fidelity of geochemical proxies
journal, January 2019
- Chanda, Piyali; Gorski, Christopher A.; Oakes, Rosie L.
- Earth and Planetary Science Letters, Vol. 506
Overview of CAST project
journal, December 2018
- Norris, Simon; Capouet, Manuel
- Radiocarbon, Vol. 60, Issue 6
Ca isotopes in carbonate sediment and pore fluid from ODP Site 807A: The Ca2+(aq)–calcite equilibrium fractionation factor and calcite recrystallization rates in Pleistocene sediments
journal, May 2007
- Fantle, Matthew S.; DePaolo, Donald J.
- Geochimica et Cosmochimica Acta, Vol. 71, Issue 10
Diffusion of C and O in calcite from 0.1 to 200 MPa
journal, May 2004
- Labotka, Theodore C.; Cole, David R.; Riciputi, Lee R.
- American Mineralogist, Vol. 89, Issue 5-6
Effects of mineral distribution at mesoscopic scale on solute diffusion in a clay-rich rock: Example of the Callovo-Oxfordian mudstone (Bure, France): EFFECTS OF MINERAL DISTRIBUTION
journal, May 2012
- Robinet, Jean-Charles; Sardini, Paul; Coelho, Daniel
- Water Resources Research, Vol. 48, Issue 5
Controls of Microstructure and Chemical Reactivity on the Replacement of Limestone by Fluorite Studied Using Spatially Resolved Small Angle X-ray and Neutron Scattering
journal, July 2019
- Weber, Juliane; Cheshire, Michael C.; Distefano, Victoria H.
- ACS Earth and Space Chemistry, Vol. 3, Issue 9
Neptunium(V) Coprecipitation with Calcite
journal, January 2008
- Heberling, Frank; Denecke, Melissa A.; Bosbach, Dirk
- Environmental Science & Technology, Vol. 42, Issue 2
The widespread occurrence of coupled carbonate dissolution/reprecipitation in surface sediments on the Bahamas Bank
journal, June 2010
- Burdige, D. J.; Hu, X.; Zimmerman, R. C.
- American Journal of Science, Vol. 310, Issue 6
Rare Earth element (REE) incorporation in natural calcite: Upper limits for actinide uptake in a secondary phase
journal, November 2006
- Stipp, S. L. S.; Christensen, J. T.; Lakshtanov, L. Z.
- Radiochimica Acta, Vol. 94, Issue 9-11
Using a laser-based CO2 carbon isotope analyser to investigate gas transfer in geological media
journal, March 2012
- Guillon, S.; Pili, E.; Agrinier, P.
- Applied Physics B, Vol. 107, Issue 2
Next generation models of carbonate mineral growth and dissolution: Modeling and Analysis: Next generation models of carbonate mineral growth and dissolution
journal, January 2014
- Stack, Andrew G.
- Greenhouse Gases: Science and Technology, Vol. 4, Issue 3
Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D)
journal, February 2018
- Cao, Bo; Stack, Andrew G.; Steefel, Carl I.
- Geochimica et Cosmochimica Acta, Vol. 222
The surface chemistry of divalent metal carbonate minerals; a critical assessment of surface charge and potential data using the charge distribution multi-site ion complexation model
journal, October 2008
- Wolthers, M.; Charlet, L.; Van Cappellen, P.
- American Journal of Science, Vol. 308, Issue 8
On the equilibrium of coexisting sedimentary carbonates
journal, February 1972
- Brätter, P.; Möller, P.; Rösick, U.
- Earth and Planetary Science Letters, Vol. 14, Issue 1
13C in atmospheric CO2
journal, August 1986
- Mook, W. G.
- Netherlands Journal of Sea Research, Vol. 20, Issue 2-3, p. 211-223
Carbon isotope exchange rate of DIC in karst groundwater
journal, June 2003
- Gonfiantini, Roberto; Zuppi, Gian Maria
- Chemical Geology, Vol. 197, Issue 1-4
Deducing growth mechanisms for minerals from the shapes of crystal size distributions
journal, June 1998
- Eberl, D. D.; Drits, V. A.; Srodon, J.
- American Journal of Science, Vol. 298, Issue 6
Experimental observations on carbon isotope exchange in carbonate-water systems
journal, March 1984
- Mozeto, A. A.; Fritz, P.; Reardon, E. J.
- Geochimica et Cosmochimica Acta, Vol. 48, Issue 3
Carbon Isotope Exchange During Calcite Interaction With Brine: Implications for 14 C Dating of Hypersaline Groundwater
journal, January 2013
- Avrahamov, Naama; Sivan, Orit; Yechieli, Yoseph
- Radiocarbon, Vol. 55, Issue 1
Catalysis and chemical mechanisms of calcite dissolution in seawater
journal, July 2017
- Subhas, Adam V.; Adkins, Jess F.; Rollins, Nick E.
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 31
Nanostructured calcite precipitated under hydrothermal conditions in the presence of organic and inorganic selenium
journal, November 2011
- Montes-Hernandez, G.; Sarret, G.; Hellmann, R.
- Chemical Geology, Vol. 290, Issue 3-4
Annual Variations of the 14 C Content of Soil CO 2
journal, January 1986
- Dörr, Helmut; Münnich, K. O.
- Radiocarbon, Vol. 28, Issue 2A
Applications of cavity ring-down spectroscopy to high precision isotope ratio measurement of 13 C/ 12 C in carbon dioxide
journal, March 2006
- Wahl, Ed H.; Fidric, Bernard; Rella, Chris W.
- Isotopes in Environmental and Health Studies, Vol. 42, Issue 1
Rate of radiocarbon retention onto calcite by isotope exchange
journal, May 2016
- Lempinen, Janne; Lehto, Jukka
- Radiochimica Acta, Vol. 104, Issue 9
Can bottom-up ocean CO2 fluxes be reconciled with atmospheric 13C observations?
journal, January 2010
- Alden, Caroline; Miller, John; White, James
- Tellus B: Chemical and Physical Meteorology, Vol. 62, Issue 5, p. 369-388
An assessment of calcite crystal growth mechanisms based on crystal size distributions
journal, September 2000
- Kile, D. E.; Eberl, D. D.; Hoch, A. R.
- Geochimica et Cosmochimica Acta, Vol. 64, Issue 17
The rapid resetting of the Ca isotopic signatures of calcite at ambient temperature during its congruent dissolution, precipitation, and at equilibrium
journal, May 2019
- Oelkers, Eric H.; Pogge von Strandmann, Philip A. E.; Mavromatis, Vasileios
- Chemical Geology, Vol. 512
Stable mineral recrystallization in low temperature aqueous systems: A critical review
journal, February 2017
- Gorski, Christopher A.; Fantle, Matthew S.
- Geochimica et Cosmochimica Acta, Vol. 198
Linear growth rate of nanosized calcite synthesized via gas–solid carbonation of Ca(OH)2 particles in a static bed reactor
journal, January 2012
- Montes-Hernandez, G.; Daval, D.; Findling, N.
- Chemical Engineering Journal, Vol. 180
Burial-induced oxygen-isotope re-equilibration of fossil foraminifera explains ocean paleotemperature paradoxes
journal, October 2017
- Bernard, S.; Daval, D.; Ackerer, P.
- Nature Communications, Vol. 8, Issue 1
Measurement of Paleotemperatures and Temperatures of the Upper Cretaceous of England, Denmark, and the Southeastern United States
journal, January 1951
- Urey, H. C.; Lowenstam, H. A.; Epstein, S.
- Geological Society of America Bulletin, Vol. 62, Issue 4