Heterogeneous catalyst design for plastics upcycling and energy conversion processes
EMSL Project ID
51711
Abstract
The overall goal of this project is to develop, implement, and apply a set of computational, multiscale techniques for the design of heterogeneous catalysts that are relevant in addressing the nation’s energy and environmental challenges. The proposed work involves two different projects in which we apply our computational strategy to identify suitable catalysts for (i) the hydrogenolysis and ?-alkyl elimination reactions of n-alkanes to understand the deconstruction mechanism of polyolefins and (ii) for the selective conversion of propane to propene, a key intermediate in the petrochemical industry. The central objective of the first project is to significantly enhance our scientific understanding of the catalytic phenomena at the interface of molecular-scale chemistry and mesoscale materials science that will enable the selective catalytic conversion of the environmentally disruptive plastic waste into more valuable products. Here, we propose to target catalytic reactions of hydrocarbon polymers, such as C-C bond hydrogenolysis catalyzed by noble metal nanoparticles or metal hydrides that will enable the selective conversion of these materials into value-added chemicals and materials (upcycling). In particular, we propose to investigate the hydrogenolysis mechanism of n-hexane and n-octane over various active site models of Pt catalyst and also the ?-alkyl elimination reaction over ZrO2 surface models under experimental reaction conditions. This study will help us understand the experimental results observed by our collaborators that the Pt/SrTiO3 and ZrO2 catalysts are active for the selective transformation of polyethylene into value-added products and identify the responsible active sites and reaction mechanism over these catalysts. The second project focuses on the selective and efficient conversion of propane to propene using economic and environmentally friendly catalysts. Specifically, we will investigate the non-oxidative propane dehydrogenation (PDH) pathway over Pt-Sn bimetallic catalysts using DFT and microkinetic modeling techniques to understand the reaction mechanism, identify the active sites and rate/selectivity controlling steps with the aim of guiding the design of improved catalysts. Overall, the results obtained from these projects?together with the experimental results from our collaborators?will provide useful design principles for catalysts discovery for sustainable energy.
Project Details
Start Date
2020-10-12
End Date
2021-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Asif J. Chowdhury, Andreas Heyden, Gabriel A. Terejanu, Wenqiang Yang. 2021. "Comparative Study on the Machine Learning-Based Prediction of Adsorption Energies for Ring and Chain Species on Metal Catalyst Surfaces." The Journal of Physical Chemistry C 125 (32):17742-17748. https://doi.org/10.1021/acs.jpcc.1c05470
Charles Fricke, Andreas Heyden, Subrata Kumar Kundu, Biplab Rajbanshi, Wenqiang Yang, Adam Yonge. 2021. "Computational Investigation of the Catalytic Hydrodeoxygenation of Propanoic Acid over a Cu(111) Surface." The Journal of Physical Chemistry C 125 (35):19276-19293. https://doi.org/10.1021/acs.jpcc.1c05240
Jesse Q. Bond, Andreas Heyden, Subrata Kumar Kundu, Osman Mamun, Rajadurai Vijay Solomon, Eric Walker, Wenqiang Yang. 2021. "Surface structure sensitivity of hydrodeoxygenation of biomass-derived organic acids over palladium catalysts: a microkinetic modeling approach." Catalysis Science & Technology 11 (18):6163-6181. https://doi.org/10.1039/D1CY01029H