Solving difficult problems with automated technology : new tools to understand complex chemical and physical processes

The desire for cheaper, faster, energy-conscious, and more sustainable chemical processes often necessitates the design and development of new catalytic methods. Once a catalytic transformation is conceived, the reaction conditions must be optimized to maximize yield and selectivity. Traditional optimization protocols stipulate the correlation of these end-metrics at a fixed time point to variable reaction parameters such as temperature, time, concentration, stoichiometry, etc. By systematically varying these parameters, researchers hope to develop empirical trends relating properties of the chemical species involved to the observed reactivity. What underpins these efforts is an attempt to account for and control the complex, dynamic, and numerous chemical equilibria within a catalytic environment. However, while idealized catalytic mechanisms can be easily envisioned, the reality is that these processes are often plagued by off-cycle equilibria and decomposition pathways that lead to reduced yield and efficiency. In order to rapidly assess what inhibits productive chemistry, focus must be redirected towards scrutinizing the mechanisms within a catalytic environment. To facilitate this, the acquisition of high-density, trustworthy, and time-resolved reaction progress information for all observable species present within a chemical transformation (starting reagents, intermediates, by-products, products, etc.) by modern in situ reaction monitoring tools offers unmatched opportunities for mechanistic understanding. Ultimately, these time-course profiles provide temporal signatures of dynamic processes active during the chemical transformation that inform process development. This Thesis reports on case studies in which the construction and application of automated technology enabled the solution to difficult problems in complex chemical and physical processes.Science, Faculty ofChemistry, Department ofGraduat