We intend to rationally design dual-function heteropolymetalic molecular catalysts for desulfurization/denitrogenation and hydrocracking of bitumen under mild conditions. An understanding of the electronic structure level of the thermodynamic stability, the reactivity of the catalysts based on energetics and dynamics studies, as well as transition state optimization, will allow us to guide the development of the experimental exploratory catalyst. Understanding the cooperative involvement of multiple metal centers in bitumen fragment bond cleavage will be essential for us to design the dual-function catalysts.
We will use advanced multiscale modeling methods, including quantum mechanics/molecular dynamics, for cluster rearrangement and stability prediction. We will also employ the statistical mechanical 3D Reference Interaction Site Model (3D-RISM) for reaction path search and transition state optimization under external conditions (such as solvation, high temperature and pressure). From there, we'll analyze the reactivity preferences among series of catalysts and bitumen fragments using electron density derived functions, such as electrostatic potential and Fukui functions.
Principal Investigator: Andriy Kovalenko
Research Team: Stanislav R. Stoyanov, Sergey Gusarov
Project Number: COSI 2009-07
Projected Completion Date: March 31, 2012