[NSF-DMREF] Design and Discovery of Multimetallic Heterogeneous Catalysts for a Future Biorefining Industry

Amount: $840,000
Duration: 09/2015 – 09/2019
PI: Andreas Heyden
Co-PIs: Gabriel Terejanu (share $270,000), Ammal Salai

Abstract

The project utilizes statistical analysis to estimate uncertainties in both experimental data and theoretical calculations relating to catalytic hydrodeoxygenation of succinic acid (SUCC HDO) – an important reaction in the refining of biomass-derived chemicals to commercially valuable products. The experimental and computational methods employed – combined with statistical error analysis – provide a more accurate and powerful approach for identifying improved catalytic materials than possible by either experiments or theory alone. The approach is applicable to a broad range of catalytic applications and could provide a blueprint for a new approach to the discovery and design of catalytic materials.

Specifically, the project involves preparation of well-defined and well-dispersed bimetallic clusters of tin (Sn) adsorbed on ruthenium (Ru), platinum (Pt) or rhodium (Rh) deposited on amorphous silica or carbon supports. The catalysts will be characterized in detail with respect to structure, composition, and surface acidity, and then evaluated in the SUCC HDO reaction. A multiscale strategy will be used for the computations based on DFT methods and techniques developed in the investigators’ laboratory aimed at reducing uncertainties in the estimation of free energies. Uncertainties in both the experimental and computational analyses will be subjected to Bayesian statistical analysis. Refinements to both the experimental and computational methods will be made to minimize the uncertainties and obtain meaningful comparisons between theory and experiment.

The methodology employed in the study can potentially guide materials selection and catalyst design for many applications beyond the specific catalysts and reaction demonstrated here. Rigorous standards are set for both the experimental and computational work, that when combined with statistical analysis, provide confidence heretofore lacking in the certainty with which new catalytic materials can be predicted.

Papers

  • A. J. Chowdhury, W. Yang, E. Walker, O. Mamun, A. Heyden, and G. A. Terejanu, “Prediction of Adsorption Energies for Chemical Species on Metal Catalyst Surfaces Using Machine Learning,” The Journal of Physical Chemistry C, vol. 122, iss. 49, pp. 28142-28150, 2018. doi:10.1021/acs.jpcc.8b09284
    [BibTeX]
    @article{ChowdhuryJ_JPCC_2018,
    author = {Chowdhury, Asif J. and Yang, Wenqiang and Walker, Eric and Mamun, Osman and Heyden, Andreas and Terejanu, Gabriel A.},
    title = {{Prediction of Adsorption Energies for Chemical Species on Metal Catalyst Surfaces Using Machine Learning}},
    journal = {{The Journal of Physical Chemistry C}},
    volume = {122},
    number = {49},
    pages = {28142-28150},
    year = {2018},
    doi = {10.1021/acs.jpcc.8b09284},
    }

  • E. A. Walker, D. Mitchell, G. A. Terejanu, and A. Heyden, “Identifying Active Sites of the Water–Gas Shift Reaction over Titania Supported Platinum Catalysts under Uncertainty,” ACS Catalysis, p. 3990–3998, 2018.
    [BibTeX]
    @article{Walker_JACS_2018,
    author = {Walker, Eric A and Mitchell, Donald and Terejanu, Gabriel A and Heyden, Andreas},
    title = {{Identifying Active Sites of the Water--Gas Shift Reaction over Titania Supported Platinum Catalysts under Uncertainty}},
    journal = {{ACS Catalysis}},
    year = {2018},
    pages = {3990--3998},
    annote = {doi: 10.1021/acscatal.7b03531}
    }

  • E. Walker, S. C. Ammal, G. Terejanu, and A. Heyden, “Uncertainty Quantification Framework Applied to the Water-Gas Shift Reaction over Pt-Based Catalysts,” J. Phys. Chem. C, vol. 120, iss. 19, pp. 10328-10339, 2016.
    [BibTeX]
    @article{EricJ_JC_2015,
    year = {2016},
    volume = {120},
    number = {19},
    pages = {10328-10339},
    journal = {{J. Phys. Chem. C}},
    title = {{Uncertainty Quantification Framework Applied to the Water-Gas Shift Reaction over Pt-Based Catalysts}},
    author = {Eric Walker and Salai Cheettu Ammal and Gabriel Terejanu and Andreas Heyden},
    }

Team Members @ USC (we also collaborate with Dr. Jesse Bond’s group @ Syracuse University)

Gabriel Terejanu : Associate Professor
Gabriel Terejanu
Associate Professor
Computer Science
UNCC
Andreas Heyden : Professor
Andreas Heyden
Professor
Chemical Engineering
UofSC
Salai Ammal : Research Asst. Prof.
Salai Ammal
Research Asst. Prof.
Chemical Engineering
UofSC

Asif Chowdhury : PhD Student
Asif Chowdhury
PhD Student
Computer Science
and Engineering
UofSC
Eric Walker : PhD 2016
Eric Walker
PhD 2016
Chemical Engineering
UofSC
Wenqiang Yang : PhD Candidate
Wenqiang Yang
PhD Candidate
Chemical Engineering
UofSC