Heterogeneous catalysts design for biorefining and energy conversion processes
EMSL Project ID
49246
Abstract
The overall goal of this project is to develop, implement, and apply a set of computational, multiscale techniques for heterogeneous catalysts design with special emphasis on the EMSL theme, "Energy Materials and Processes (EMP)". 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 efficient conversion of natural gas to fuels and chemicals. 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 methane to dimethyl ether, a clean-burning diesel fuel, using innovative chemical pathways and catalyst/membrane assemblies. Specifically, we will investigate the methane activation process on LaOCl catalyst surface models 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
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2018-09-30
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
Ammal SC, Heyden A. 2017. "Titania-Supported Single-Atom Platinum Catalystfor Water-Gas Shift Reaction" Chemie Engenieur Technik 89(10): 1343-1349. DOI: 10.1002/cite.201700046
Chowdhury A.J., W. Yang, E.A. Walker, M.G. Mamun, A. Heyden, and G.A. Terejanu. 2018. "Prediction of Adsorption Energies for Chemical Species on Metal Catalyst Surfaces Using Machine Learning." Journal of Physical Chemistry C 122. doi:10.1021/acs.jpcc.8b09284
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.
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
Mamun O, Saleheen M, Bond JQ, and Heyden A. 2017. "Importance of Angelica Lactone Formation in the Hydrodeoxygenation of Levulinic Acid to γ‑Valerolactone over a Ru(0001) Model Surface". Journal of Physical Chemistry C 121: 18746-18761. DOI: 10.1021/acs.jpcc.7b06369
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, Heyden, A. 2018. "Liquid-Phase Modeling in Heterogeneous Catalysis". ACS Catalysis 8: 2188-2194. DOI: 10.1021/acscatal.7b04367.
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
Wan W., S. Ammal, Z. Lin, K. You, A. Heyden, and J.G. Chen. 2018. "Controlling Reaction Pathways of Selective C–O Bond Cleavage of Glycerol." Nature Communications 9. doi:10.1038/s41467-018-07047-7
Xi Y., and A. Heyden. 2019. "Direct Oxidation of Methane to Methanol Enabled by Electronic Atomic Monolayer-Metal Support Interaction." ACS Catalysis 9, no. 7:6073-6079. doi:10.1021/acscatal.9b01619
Xi Y., and A. Heyden. 2020. "Highly Efficient Deoxydehydration and Hydrodeoxygenation on MoS2‑Supported Transition-Metal Atoms through a C−H Activation Mechanism." ACS Catalysis 10, 11346-11355. doi:10.1021/acscatal.0c02669
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.
Xi Y., J. Lauterbach, Y. P-Torres, and A. Heyden. 2020. "Deoxydehydration of 1,4-anhydroerythritol over anatase TiO2IJ101)-supported ReOx and MoOx." Catalysis Science & Technology 10, 3731-3738.
Xi Y., W. Yang, S. Ammal, J. Lauterbach, Y. Pagan-Torres, and A. Heyden. 2018. "Mechanistic Study of the Ceria Supported, Re-catalyzed Deoxydehydration of Vicinal OH Groups." Catalysis Science & Technology. doi:10.1039/c8cy01782d