Surface evolution of dissolving minerals investigated with a kinetic Ising model

Joel Z. Bandstra, Susan Louise Brantley

Research output: Contribution to journalArticle

34 Citations (Scopus)

Abstract

In natural weathering systems, both the chemistry and the topography of mineral surfaces change as rocks and minerals equilibrate to surface conditions. Most geochemical research has focused on changes in solution chemistry over time; however, temporal changes in surface topography may also yield information about rates and mechanisms of dissolution. We use stochastic dissolution simulations of a regular 2-D lattice with reaction mechanisms defined in terms of nearest neighbor interactions to elucidate how the surface area and reactivity of a crystal evolve during dissolution. Despite the simplicity of the model, it reproduces key features observed or inferred for mineral dissolution. Our model results indicate that: (i) dissolving surfaces reach a steady-state conformation after sufficient dissolution time, (ii) linear defects cause surface area and dissolution rate to vary in concert with one another, (iii) sigmoidal and non-sigmoidal rate vs. free-energy of reaction (ΔGrxn) behavior can be rationalized in terms of the multiple steps occurring during dissolution, and (iv) surface roughness as a function of ΔGrxn is highly sensitive to the reaction mechanism. When simulated times to reach steady-state are compared to published time series rate data using suitable scaling, good agreement is found for silicate minerals while the model significantly over-predicts the duration of the transient for Fe and Al oxides. The implication of our simple model is that many aspects of mineral dissolution behavior, including approach to steady-state, sigmoidal vs. non-sigmoidal rate vs. ΔGrxn behavior, and development of rougher surfaces in conditions further from equilibrium can be explained by nearest neighbor interactions and simple Kossel-type models where reactivity of a surface is defined in terms of perfect surface, step, and kink sites.

Original languageEnglish (US)
Pages (from-to)2587-2600
Number of pages14
JournalGeochimica et Cosmochimica Acta
Volume72
Issue number11
DOIs
StatePublished - Jun 1 2008

Fingerprint

Ising model
Minerals
Dissolution
dissolution
kinetics
Kinetics
mineral
surface area
topography
Silicate minerals
silicate mineral
Surface defects
Surface topography
Weathering
surface roughness
Oxides
Topography
Free energy
defect
Conformations

All Science Journal Classification (ASJC) codes

  • Geochemistry and Petrology

Cite this

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Surface evolution of dissolving minerals investigated with a kinetic Ising model. / Bandstra, Joel Z.; Brantley, Susan Louise.

In: Geochimica et Cosmochimica Acta, Vol. 72, No. 11, 01.06.2008, p. 2587-2600.

Research output: Contribution to journalArticle

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