Journal
EARTH AND PLANETARY SCIENCE LETTERS
Volume 457, Issue -, Pages 100-105Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.epsl.2016.10.019
Keywords
crystal surface reactivity; reaction rate mapping; porosity evolution.; rate spectra; kinetic Monte Carlo simulation
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Funding
- DFG [Fi 1212-7]
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A common assumption is that water rock reaction rates should converge to a mean value. There is, however, an emerging consensus on the genuine nature of reaction rate variations under identical chemical conditions. Thus, the further use of mean reaction rates for the prediction of material fluxes is environmentally and economically risky, manifest for example in the management of nuclear waste or the evolution of reservoir rocks. Surface-sensitive methods and resulting information about heterogeneous surface reactivity illustrate the inherent rate variability. Consequently, a statistical analysis was developed in order to quantify the heterogeneity of surface rates. We show how key components of the rate combine to give an overall rate and how the identification of those individual rate contributors provide mechanistic insight into complex heterogeneous reactions. This generates a paradigm change by proposing a new pathway to reaction model parameterization and for the prediction of reaction rates. (C) 2016 Elsevier B.V. All rights reserved.
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