Research Initiation Award: A Computational Study of Hydroformylation of Ethylene Over Heterogeneous Bimetallic Catalysts

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Research Initiation Awards provide support for junior and mid-career faculty at Historically Black Colleges and Universities who are building new research programs or redirecting and rebuilding existing research programs. It is expected that the award helps to further the faculty member's research capability and effectiveness, improve research and teaching at the home institution, and involves undergraduate students in research experiences. The award to Florida Agricultural and Mechanical University has potential to increase the understanding of hydroformylation which is an industrial process to produce aldehydes. The project will create undergraduate and graduate courses in materials modeling, provide research training in computational materials science and catalysis and create internal and external collaborations with local community colleges and high schools. Hydroformylation is a process to produce aldehydes by the reaction of synthesis gas with alkenes. Currently, hydroformylation is carried out using Rh and or Co-based transition metal complexes as a catalyst. The homogeneous nature of this reaction leads to difficulties in catalyst separation and recovery, active metal losses, metal species contamination, and corrosivity of catalytic solutions. The development of heterogeneous catalytic systems without sacrificing the activity and selectivity will avoid the drawbacks associated with homogeneous catalysts and be highly useful. This project employs computational methods such as first-principles density functional theory (DFT) calculations and kinetic Monte Carlo (KMC) simulations to gain a fundamental understanding of catalytic science of ethylene hydroformylation to C3-oxygenates on heterogeneous Rh and Rh-based bimetallic model catalysts. The DFT calculations will provide the energetics of the reaction network and KMC simulations will be employed to obtain the kinetics of the reaction at experimental reaction conditions. The theoretical calculations will provide atomistic insight into ethylene hydroformylation and help identify simple catalytic descriptors that can be used to screen potential bimetallic catalysts that are active and selective for ethylene conversion to C3-oxygenates. Moreover, the knowledge gained from this study will also shed light on the hydroformylation of other higher alkenes.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.