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A B S T R AC T : Anisotropy and compositional and structural heterogeneity in clays are causes of considerable deviations from homogeneous diffusion, in particular in terms of direction-dependent transport rates and preferred transport zones. Conventional diffusion experiments, in which the sample is treated as a homogeneous black box in a concentration gradient, are interminable and insensitive to spatial effects. In contrast, tomographic imaging methods are capable of both reducing the amount of observation time required and revealing space-dependent features of the diffusion process.In the present study, positron-emission-tomography (PET) was applied as the most sensitive quantitative spatiotemporal tomographic modality for direct observation of positron-emitting radiotracers in opaque media at reasonable resolution (1 mm) on a laboratory scale (100 mm).Geoscientific applications of PET, or GeoPET, have revealed anisotropic and heterogeneous effects in diffusion experiments that have been conducted on Opalinus clay samples of different sizes, as well as on other rock types. Applying the Comsol Optimization Module to 2D-image sections of the PET tomograms, effective parameter values were derived, thereby quantifying the anisotropic diffusion.

Phenoxyalkanoic acids like the 4-chloro-2-methylphenoxyacetic acid (MCPA) are the second highest used xenobiotic herbicides worldwide after glyphosate because of their apparently favorable environmental properties. Experimental batch equilibration data suggested a reduced Cu adsorption efficiency with the soil mineral goethite below pH 6 in presence of MCPA. This has been verified by advanced surface complexation adsorption modelling involving dissolved Cu-MCPA complexation constants. Positron emission tomography is a non-invasive molecular imaging method for time-resolved three-dimensional information commonly applied on non-retarded tracers in soil core scale experiments. Mineral surface reactive tracers like Cu-64 are too immobile for the relatively short observation times available with this advanced imaging technique. However, Cu-64 radiolabeled Cu-MCPA complex migration could be observed in as long as 10-cm artificial soil test columns where break-through occurred within a few days. For the first time, time-lapse movies of Cu migration in the opaque soil columns were recorded using this novel reactive transport process tomography approach.

The transport of water and salt solutions in unsaturated clay and clay rock was measured using the positron emission tomography (PET). The experimental device is described. KF marked with 18 F was used as conservative hydrodynamic tracer to image the flow profiles at different times. Homogeneous and heterogeneous flow regimes were identified. Hydrodynamic model parameters could be determined for the homogeneous regime. The results demonstrate the advantage of PET measurements for investigations of transport processes in geological matrices. They yield quantitative values of the spatial distribution in regard to the flow pattern inside the samples which are important for the validation and parameter estimation of geochemical transport models.

Abstract. Clay plays a prominent role as barrier material in the geosphere. The small particle sizes cause extremely small pore sizes and induce low permeability and high sorption capacity. Transport of dissolved species by molecular diffusion, driven only by a concentration gradient, is less sensitive to the pore size. Heterogeneous structures on the centimetre scale could cause heterogeneous effects, like preferential transport zones, which are difficult to assess. Laboratory measurements with diffusion cells yield limited information on heterogeneity, and pore space imaging methods have to consider scale effects. We established positron emission tomography (PET), applying a high-resolution PET scanner as a spatially resolved quantitative method for direct laboratory observation of the molecular diffusion process of a PET tracer on the prominent scale of 1-100 mm. Although PET is rather insensitive to bulk effects, quantification required significant improvements of the image reconstruction procedure with respect to Compton scatter and attenuation. The experiments were conducted with 22 Na and 124 I over periods of 100 and 25 days, respectively. From the images we derived trustable anisotropic diffusion coefficients and, in addition, we identified indications of preferential transport zones. We thus demonstrated the unique potential of the PET imaging modality for geoscientific process monitoring under conditions where other methods fail, taking advantage of the extremely high detection sensitivity that is typical of radiotracer applications.

Abstract. Transport processes in geomaterials can be observed with input-output experiments, which yield no direct information on the impact of heterogeneities, or they can be assessed by model simulations based on structural imaging using µ-CT. Positron emission tomography (PET) provides an alternative experimental observation method which directly and quantitatively yields the spatio-temporal distribution of tracer concentration. Process observation with PET benefits from its extremely high sensitivity together with a resolution that is acceptable in relation to standard drill core sizes. We strongly recommend applying high-resolution PET scanners in order to achieve a resolution on the order of 1 mm.We discuss the particularities of PET applications in geoscientific experiments (GeoPET), which essentially are due to high material density. Although PET is rather insensitive to matrix effects, mass attenuation and Compton scattering have to be corrected thoroughly in order to derive quantitative values.Examples of process monitoring of advection and diffusion processes with GeoPET illustrate the procedure and the experimental conditions, as well as the benefits and limits of the method.

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