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Heterogeneous catalyst design for biorefining and energy conversion processes


EMSL Project ID
51163

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 which also involves developing machine learning techniques to predict the activity of a specific metal catalyst, 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
2019-10-01
End Date
2020-09-30
Status
Closed

Team

Principal Investigator

Andreas Heyden
Institution
University of South Carolina

Team Members

Kyung-Eun You
Institution
University of South Carolina

Subrata Kundu
Institution
University of South Carolina

Charles Fricke
Institution
University of South Carolina

Wenqiang Yang
Institution
University of South Carolina

Mohammad Saleheen
Institution
University of South Carolina

Salai Ammal
Institution
University of South Carolina

Related Publications

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
Andreas Heyden, Subrata Kumar Kundu, Mohammad Saleheen, Mehdi Zare. 2020. "Dependency of solvation effects on metal identity in surface reactions." Communications Chemistry 3 (1) https://doi.org/10.1038/s42004-020-00428-4
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
Chowdhury A.J., W. Yang, K.E. Abdelfatah, M. Zare, A. Heyden, and G.A. Terejanu. 2020. "A Multiple Filter Based Neural Network Approach to the Extrapolation of Adsorption Energies on Metal Surfaces for Catalysis Applications." Journal of Chemical Theory and Computation 16, no. 2:1105–1114.
Jesse Q. Bond, Andreas Heyden, Osman Mamun, Rajadurai Vijay Solomon, Wenqiang Yang. 2020. "Investigation of the reaction mechanism of the hydrodeoxygenation of propionic acid over a Rh(1 1 1) surface: A first principles study." Journal of Catalysis 391:98-110. https://doi.org/10.1016/j.jcat.2020.08.015
Rajbanshi B., S. Saha, S. Ammal, and A. Heyden. 2020. "Oxidative Dehydrogenation of Propane on the Oxygen Adsorbed Edges of Boron Nitride Nanoribbons." Catalysis Science & Technology 10, no. 15:5181-5195.
Xi Y., and A. Heyden. 2020. "Preferential Oxidation of CO in Hydrogen at Nonmetal Active Sites with High Activity and Selectivity." ACS Catalysis 10, 5362-5370. doi:10.1021/acscatal.0c00743
Xi Y., and A. Heyden. 2020. "Selective Activation of Methane CH Bond in the Presence of Methanol." Journal of Catalysis 386.
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.
Zare M., R. V.. Solomon, W. Yang, A. Yonge, and A. Heyden. 2020. "Theoretical Investigation of Solvent Effects on the Hydrodeoxygenation of Propionic Acid over a Ni(111) Catalyst Model." Journal of Physical Chemistry C 124, 16488-16500. doi:10.1021/acs.jpcc.0c04437