Complexes simulation speciation models

Computer simulation is now used extensively as a tool to help to understand and predict the transport of radionuclides through environmental systems. Most models relate to waste disposal and are based on measured parameters such as water movements, salinity, suspended load and the radionuclide concentration in the solute, suspended particulate matter and bottom deposits. Comparatively few attempts appear to have been made to include chemical speciation into this type of model, presumably because of the added complexity involved. Some modellers have attempted to take into account the characteristics of the major chemical phases such as those present in different particles or coatings (e.g. Martinez-Aquirre et al., 1994). Others have noted the importance of including details of particular chemical species present in industrial waste releases when constructing models to predict dispersion (Abril and Fraga, 1996). 

The surface speciation in Model 3 simulations for systems equilibrated with air and 1% CO2 is shown in Fig. 4-11 and 4-12. The ternary carbonate complexes in Model 3 were of greater importance in comparison to Model 2. This emphasizes again the significance of collecting adsorption data as a function of the partial pressure of CO2, in order to accurately represent the effect of carbonate complexation on both aqueous and surface speciation. Model 3 speciation better represented the experimental data not only as a function of CO2, but also as a function of pH in the pH range from 5 to 7. 

A second obvious line of research for the future must be that related to the development and improvement of computer-based simulation of long-term environmental behaviour of radionuclides. Most currently available models are still comparatively simple compared with the physical, chemical and biological complexity of environments they purport to represent but, as noted in Section 13.5, our ability to construct ever more complex conceptual models for predicting the future behaviour of radionuclides is improving. However, the more complex the model, the more demands it places on the basic thermodynamic data and knowledge of likely speciation. The challenge for the future will therefore be to produce high-quality data for model construction and to devise realistic ways to validate those models once produced. 

In general, geochemical models can be divided according to their levels of complexity (Figure 2.3). Speciation-solubility models contain no spatial or temporal information and are sometimes called zero-dimension models. Reaction path models simulate the successive reaction steps of a system in response to the mass or energy flux. Some temporal information is included in terms of reaction progress, f, but no spatial information is contained. Coupled reactive mass transport models contain both temporal and spatial information about chemical reactions, a complexity that is desired for environmental applications, but these models are complex and expensive to use. 

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