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A surface complexation model of the carbonate mineral-aqueous solution interface

Journal Article · · Geochimica et Cosmochimica Acta; (United States)
 [1];  [2];  [3];  [4]
  1. Georgia Inst. of Technology, Atlanta (United States)
  2. Univ. of Bern (Switzerland)
  3. Swiss Federal Inst. of Technology, Duebendorf (Switzerland)
  4. Stanford Univ., CA (United States)

A surface complexation model for the chemical structure and reactivity of the carbonate-water interface is presented. The model postulates the formation of the hydration species >CO[sub 3]H[sup 0] and >MeOH[sup 0] at the surface of a divalent metal carbonate MeCO[sub 3] (Me = Ca, Mn, Fe, etc.). The existence of these primary hydration species is supported by spectroscopic data. The following reactions are proposed to govern surface speciation in the MeCO[sub 3](s)-H[sub 2]O-CO[sub 2] system: >CO[sub 3]H[sup 0] [Leftrightarrow] >CO[sub 3][sup [minus]] + H[sup +]; >CO[sub 3]H[sup 0] + Me[sup 2+] [Leftrightarrow] >CO[sub 3]Me[sup +] + H[sup +]; >MeOH[sub 2][sup +] [Leftrightarrow] >MeOH[sup 0] + H[sup +]; >MeOH[sup 0] [Leftrightarrow] >MeO[sup [minus]] + H[sup +]; >MeOH[sup -] + CO[sub 2] [Leftrightarrow] >MeHCO[sub 3][sup 0]; and >MeOH[sup 0] + CO[sub 2] [Leftrightarrow] >MeCO[sub 3][sup [minus]] + H[sup +]. It is shown in this paper that the surface complexation model provides a systematic explanation of surface charge development and dissolution kinetics of carbonate minerals. The intrinsic stability constants of the surface complexation reactions agree well with the equilibrium constants of the corresponding complexation reactions in homogeneous solution. 61 refs., 11 figs., 3 tabs.

OSTI ID:
6064462
Journal Information:
Geochimica et Cosmochimica Acta; (United States), Journal Name: Geochimica et Cosmochimica Acta; (United States) Vol. 57:15; ISSN GCACAK; ISSN 0016-7037
Country of Publication:
United States
Language:
English