Heterogeneous catalyst design for biorefining and energy conversion processes
EMSL Project ID
50576
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 (i) investigate chemical reactions at the solid-liquid interface relevant for biomass conversion processes and (ii) identify suitable catalysts for 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 molecular level understanding of heterogeneous catalysis at the solid-liquid interface that is generally relevant for biomass conversion processes in the liquid phase. In particular, we propose to use our own implicit and explicit solvation models to investigate the hydrodeoxygenation (HDO) mechanism of succinic acid, a top ten biomass derivative, in aqueous media on various mono- and bimetallic catalysts in order to understand the specific effect of solvents on the reaction mechanism and to help identify activity, selectivity, and stability descriptors that can be used to design and evaluate tailored bimetallic catalysts. Our multiscale strategy for investigating reactions at the solid-liquid interface involves gas phase computations of the reaction mechanism on metal surfaces, developing microkinetic models to determine rate-limiting steps and activity descriptors, examining the effect of solvents, properly considering the amount of uncertainty in computational predictions (and their correlation structure) and finally screening a number of mono- and multimetallic catalysts for optimal performance. 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 and the oxidative dehydrogenation (ODH) pathway over boron nitride nanoribbon 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 proposed work will provide fundamental insights into heterogeneous catalysis at solid-liquid and solid-gas interfaces. These results?together with the experimental results from our collaborators?will provide useful design principles for catalysts discovery for sustainable energy.
Project Details
Start Date
2018-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Ammal S., and A. Heyden. 2019. "Understanding the Nature and Activity of Supported Platinum Catalysts for the Water-Gas Shift Reaction: From Metallic Nanoclusters to Alkali-Stabilized Single-Atom Cations." ACS Catalysis 9, no. 9:7721-7740. doi:10.1021/acscatal.9b01560
Andreas Heyden, Osman Mamun, Mohammad Saleheen, Mehdi Zare. 2021. "Aqueous-phase effects on ethanol decomposition over Ru-based catalysts." Catalysis Science & Technology https://doi.org/10.1039/D1CY01057C
Celik G., R.M. Kennedy, R.A. Hackler, M.S. Ferrandon, A. Tennakoon, S. Patnaik, and A. LaPointe, et al. 2019. "Upcycling Single-Use Polyethylene into High-Quality Liquid Products." ACS Central Science 5, no. 11:1795-1803. doi:10.1021/acscentsci.9b00722
Mamun O., M. Saleheen, J.Q. Bond, and A. Heyden. 2019. "Investigation of Solvent Effects in the Hydrodeoxygenation of Levulinic Acid to c-valerolactone over Ru Catalysts." Journal of Catalysis 379. doi:10.1016/j.jcat.2019.09.026
Saleheen M., A. Mohan Verma, O. Mamun, J. Lu, and A. Heyden. 2019. "Investigation of Solvent Effects on the Hydrodeoxygenation of Guaiacol over Ru Catalysts." Catalysis Science & Technology 9. doi:10.1039/c9cy01763a
Saleheen M., M. Zare, M. Faheem, and A. Heyden. 2019. "Computational Investigation of Aqueous Phase Effects on the Dehydrogenation and Dehydroxylation of Polyols over Pt(111)." Journal of Physical Chemistry C 123, no. 31:19052-19065. doi:10.1021/acs.jpcc.9b04994
Yang W., R.V. Solomon, J. Lu, O. Mamun, J.Q. Bond, and A. Heyden. 2020. "Unraveling the Mechanism of the Hydrodeoxygenation of Propionic Acid Over a Pt (1 1 1) Surface in Vapor and Liquid Phases." Journal of Catalysis 381. doi:10.1016/j.jcat.2019.11.036
You K., S. Ammal, Z. Lin, W. Wan, J.G. Chen, and A. Heyden. 2020. "Understanding the Effect of Mo2C Support on the Activity of Cu for the Hydrodeoxygenation of Glycerol." Journal of Catalysis 388.