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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

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

Yongjie Xi
Institution
University of South Carolina

Supriya Saha
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

Md Osman Mamun
Institution
University of South Carolina

Salai Ammal
Institution
University of South Carolina