As our nation's supply of fossil fuels dwindles over the next century, low-quality �dirty� petroleum feedstocks (from tar sands, oil shales, etc.)  will serve as a bridge to alternative energy sources. However, these feedstocks typically contain N and S-containing hydrocarbons as impurities, and must be �cleaned� prior to burning via hydrodenitrogenation (HDN) and hydrodesulfurization (HDS).                                           In this project, DFT calculations are performed for the actinide systems Cp2An(Ph)2 (An = Th, U). Experimentally, these systems exhibit a rich chemistry towards heterocyclic substrates (C-H/C-N activation, ring-opening, dearomatization). Recently at LANL, Cp2Th(Ph)2 was found to catalyze the ring opening and C-C coupling of two thiophene molecules to form a novel dimeric Th complex. In addition to calculating a mechanism for this dimerization, we perform time-dependent DFT (TDDFT) and natural transition orbital (NTO) calculations to elucidate the nature of the transitions and excited states in the experimental absorption spectrum of the Th dimer.

DFT study of Cp<sub>2</sub>An(Ph)<sub>2</sub> as catalysts for thiophene hydrodesulfurization (HDS): A novel dimerization

243rd National Meeting (2012)

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DFT study of Cp2An(Ph)2 as catalysts for thiophene hydrodesulfurization (HDS): A novel dimerization

DFT study of Cp₂An(Ph)₂ as catalysts for thiophene hydrodesulfurization (HDS): A novel dimerization