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Research ArticleArticles

Crystal surface reactivity analysis using a combined approach of X-ray micro-computed tomography and vertical scanning interferometry

Wolf-Achim Kahl, Tao Yuan, Till Bollermann, Wolfgang Bach and Cornelius Fischer
American Journal of Science January 2020, 320 (1) 27-52; DOI: https://doi.org/10.2475/01.2020.03
Wolf-Achim Kahl
* Department of Geosciences, University of Bremen, Bremen, Germany
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  • For correspondence: wakahl@uni-bremen.de c.fischer@hzdr.de
Tao Yuan
** Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Institut für Ressourcenökologie, Abteilung Reaktiver Transport, Permoserstrasse 15, D-04318 Leipzig, Germany
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Till Bollermann
** Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Institut für Ressourcenökologie, Abteilung Reaktiver Transport, Permoserstrasse 15, D-04318 Leipzig, Germany
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Wolfgang Bach
* Department of Geosciences, University of Bremen, Bremen, Germany
*** MARUM Center for Marine Environmental Sciences, University of Bremen, Bremen, Germany
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Cornelius Fischer
** Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Institut für Ressourcenökologie, Abteilung Reaktiver Transport, Permoserstrasse 15, D-04318 Leipzig, Germany
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  • For correspondence: wakahl@uni-bremen.de c.fischer@hzdr.de
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Abstract

Dissolution rates of porous crystalline materials reflect the superposition of transport and surface control, mainly via the parameters saturation of the ambient fluid and distribution of surface energy. As a result, reacting surfaces evolve over time showing a heterogeneous distribution of surface rates. The spatiotemporal heterogeneity of surface reaction rates is analyzed using the rate map and rate spectra concept. Here, we quantify the dissolution rate variability covering the nm- to mm-scale of dissolving single-crystal and polycrystalline calcite samples, using a combined approach of X-ray micro-computed tomography (μ-CT) and vertical scanning interferometry (VSI). The dissolution experiments cover reaction periods from 15 minutes up to 54 days. The observed rate ranges are remarkably consistent over the entire reaction period but include a variability of about two orders of magnitude (10−9 − 3 × 10−7 mol m−2 s−1). The rate map data underscore the concurrent and superimposing impact of surface- vs. fluid flow controlled rate portions. The impact of fluid flow on reactivity at the mm-scale in the transport-controlled system is confirmed by 2-D reactive transport modeling. The sub-mm spatial heterogeneity of low vs. high reactivity surface portions of polycrystalline calcite is clearly below the mean crystal size. This suggests the dominant impact of highly reactive surface portions irrespective of the orientation of larger crystals on the overall surface reactivity. Correspondingly, the overall range of intrinsic reactivity heterogeneity as observed using singly crystal material is not further expanded for polycrystalline material. As a general conclusion, numerical reactive transport concepts would benefit from the implementation of a reactivity term resembling the experimentally observed existence of multiple rate components.

  • crystal surface reactivity
  • rate map
  • dissolution rate variability
  • X-ray micro-computed tomography (μ-CT)
  • vertical scanning interferometry (VSI)
  • reactive transport
  • fluid-rock interaction
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American Journal of Science: 320 (1)
American Journal of Science
Vol. 320, Issue 1
1 Jan 2020
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Crystal surface reactivity analysis using a combined approach of X-ray micro-computed tomography and vertical scanning interferometry
Wolf-Achim Kahl, Tao Yuan, Till Bollermann, Wolfgang Bach, Cornelius Fischer
American Journal of Science Jan 2020, 320 (1) 27-52; DOI: 10.2475/01.2020.03

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Crystal surface reactivity analysis using a combined approach of X-ray micro-computed tomography and vertical scanning interferometry
Wolf-Achim Kahl, Tao Yuan, Till Bollermann, Wolfgang Bach, Cornelius Fischer
American Journal of Science Jan 2020, 320 (1) 27-52; DOI: 10.2475/01.2020.03
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Keywords

  • crystal surface reactivity
  • rate map
  • dissolution rate variability
  • X-ray micro-computed tomography (μ-CT)
  • vertical scanning interferometry (VSI)
  • reactive transport
  • fluid-rock interaction

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