Understanding the Mechanism of CO Hydrogenation to Oxygenates
EMSL Project ID
50479
Abstract
The submitted proposal will enable a highly focused computational investigation of a novel CO hydrogenation molecular mechanism from first-principles using the state-of-the-art Cascade supercomputing cluster at EMSL. This research is complementary and integral to ongoing work on oxygenates formation via CO hydrogenation at WSU by the PI and our experimental collaborators. The members of our research group are veteran users of Cascade and are focused on both the application and science of heterogeneous catalysis for ensuring sustainable energy and materials solutions for the future. Specifically, as it relates to this work, syngas (CO/H2) is currently at the crossroads of many advanced chemical conversion routes and can be generated from renewable resources such as biogas. One example is hydroformylation which according to recent research has the potential of turning from an energy-demanding large-scale process of homogeneous catalysis into a 'one step - one pot' low-cost process of heterogeneous catalysis. Another example is the formation of short-chain alcohols which, in the case of syngas-out-of-biomass, could be turned entirely green. The submitted EMSL proposal will help lay the essential scientific basis by providing a detailed picture of the CO hydrogenation mechanism where the catalytically active surface phase is accounted for based on experimental evidence therefore enabling the targeted design of relevant catalyst formulations with the potential of an industrial implementation. The research we describe here is foundational to our integrated research approach in that the detailed mechanistic information we seek will require focused and intense computational investigations that few computational infrastructures around the world can handle. Our experience with Cascade at EMSL has shown us that this supercomputing cluster is the premier choice for this type of work. The results of this study will be fed into the productive feed-back loop we have developed with our experimental research collaborators at WSU with the ultimate goal of creating a predictive catalyst design enabling a large-scale industrial implementation. We advance the working hypothesis that the selective production of oxygenates versus hydrocarbons using the FT technology is the product of available surface intermediates/complexes, such as surface hydroxyl or formate, which are necessary for a repetitive CO insertion mechanism to take place so as to induce hydrocarbon growth and oxygenate production.
Project Details
Start Date
2018-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members