Structure and reactivity of the dolomite (104) water interface: New insights into the dolomite problem

Details Structure and reactivity of the dolomite (104) water interface: New insights into the dolomite problem Structure and reactivity of the dolomite (104) water interface: New insights into the dolomite problem

Feb 2007

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2007gecoa..71..566f&link_type=abstract

Geochimica et Cosmochimica Acta, Volume 71, Issue 3, p. 566-579.

Computer Science

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Scientific paper

The structure and reactivity of the dolomite (104) water interface was probed in situ with high resolution X-ray reflectivity and surface force microscopy at room temperature. Measurements in stoichiometric solutions alternating between saturated and supersaturated (log IAP/K = 2.3) conditions show that the dolomite surface termination readily changes in response to solution composition, but these changes are self-limiting and partially irreversible. The freshly cleaved dolomite (104) surface in contact with the saturated solution has a stoichiometric termination, a distinct surface hydration layer and small surface structural displacements, similar to those observed previously at the calcite water interface. After reaction with supersaturated solutions dolomite is terminated by a two-layer thick Ca-rich film with substantial structural displacements of the cations. With subsequent exposure to a saturated solution this surface was transformed to an interfacial structure different from the freshly cleaved surface, having a reduced density of the outermost surface layer and a Ca-rich second layer. These results provide new insight into the lack of dolomite growth in modern carbonate environments (i.e., the “dolomite problem”), suggesting that this behavior is associated with a combination of thermodynamic and kinetic factors, including (1) growth of compositionally modified epitaxial CaXMg2-X(CO3)2 layers having thicknesses limited by lattice strain, (2) slow incorporation of Mg during layer growth, and (3) partial irreversibility of surface reactions.

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