Computational Studies of Materials for Catalysis and Photocatalysis
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Authors
Curtis, Kevin
Issue Date
2024
Type
Dissertation
Language
en_US
Keywords
catalysis , chemistry , computational , invest , photocatalytic , zeolite
Alternative Title
Abstract
In this dissertation, ab-initio computational chemistry methods are used to studya variety of systems. First, systems with inverted singlet-to-triplet gaps are investigated
for the purpose of photocatalytic water splitting. In addition to designing
molecules for this purpose, a machine learning model is also presented, allowing for
large volume screening of molecules for required photophysical properties. Second,
copper-exchanged zeolites, specifically their active sites and neighboring atoms, are
investigated. These active sites are responsible for catalyzing methane-to-methanol
conversion, an important process needed for transport. Third, the complexation of
SO3 with pyridine and bipyridine is studied. This process allows for recapture of
SO3, preventing detrimental environment impact. Further, these complexes have
photochromatic properties that are useful in a wide range of applications.
In common, all of the content in this dissertation touches on the excited state
properties of molecules. In Chapters 2 and 3, materials with inverted S1 and T1
states are investigated for application in photocatalytic water splitting. This process
requires specific energies for low-lying excited states, as well as a correct ordering of
the S1 and T1 states. Chapter 4 uses excited states as reference values to contextualize
the accuracy of our !B88PTPSS density functional approximation (DFA). In Chapter
5, excited state spectra are calculated and compared to experimental data to identify
accurate computational methods for copper-exchanged zeolites. Lastly, Chapter 6
performs a similar analysis, but for pryridine and bipyridine complexes of SO3.