Measurement of the vapor-liquid equilibrium (VLE) of fluid mixtures with many components presents a challenge. Data describing such mixtures, like fuels, are important for the development of alternative energy sources and to support forensic science, but there is a lack of suitable instrumentation to provide data with reasonable uncertainty for mixtures with many components. In this thesis, three different techniques for fluid characterization are explored: the advanced distillation curve (ADC), the advanced distillation curve with reflux (ADCR), and PLOT-cryoadsorption. Two pyrolysis fuels similar to gasoline and diesel fuel made from polypropylene were studied with respect to volatility, composition, and energy content using the advanced distillation curve. The diesel fuel demonstrated volatility very similar to previously measured diesel fuels. The gasoline was less volatile than petroleum-derived counterparts and did not meet specifications.
Two pyrolysis crude oils made from ponderosa pine and dairy manure were assessed using the ADC coupled to an approach for characterizing fluids with multiple, immiscible liquid phases. Both oils contained high water levels and would require further refinement before use. The organic phases of each oil contained components indicative of the feedstock used.
A modification of the ADC method, the advanced distillation curve with reflux, was introduced as an approach to measuring the VLE of fluids with many components. The ADCR additionally approximates the weathering of an ignitable liquid that occurs during an arson fire and measures VLE across a range of weathered conditions. The method was demonstrated using two simple mixtures. The measurements agreed well with models, indicating that ADCR is a suitable VLE metrology.
Vapor-liquid equilibrium data are crucial for interpreting the results of headspace characterization used often in forensic science. One headspace method, portable PLOT-cryoadsorption, was tested in a series of experiments in the laboratory and then deployed for the first time in a field environment that simulated a cargo container. The technology was found to be rapid and sensitive to a variety of compounds of interest to forensic science. Each of the three techniques described in this thesis contribute valuable property data for multicomponent mixtures, towards the development of high-quality predictive models.
|Commitee:||Huber, Marcia, Lovestead, Tara, Ziemann, Paul, de Gouw, Joost|
|School:||University of Colorado at Boulder|
|School Location:||United States -- Colorado|
|Source:||DAI-B 80/02(E), Dissertation Abstracts International|
|Subjects:||Alternative Energy, Analytical chemistry, Environmental science|
|Keywords:||Distillation, Forensic science, Headspace analysis, Pyrolysis fuels, Thermodynamics, Vapor-liquid equilibrium|
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