Abstract
Mechanistic understanding and prediction of solute transport and surface reactions in the pore space of rocks and soils is critical for a variety of processes, including sediment diagenesis, contaminant remediation, and long-term waste storage strategies. Positron emission tomography (PET) using β+-emitting radiotracers is an established and reliable method for investigating advective flow and diffusive flux in porous geomaterials. Here we present a conceptual strategy for spatially resolved quantification of crystal surface reactivity for sorption reactions based on PET techniques. The deconvolution of tracer breakthrough curves quantifies the sorption of F− tracer on calcite crystal surfaces and identifies the varying surface reactivity in the complex porous material. Using an artificial sediment as a model system, we demonstrate the quantifiability of sorption effects down to 10 pmol/mm3. The proposed strategy outlines how spatially resolved surface reactivities and their temporal changes over time can generally be determined using PET.
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