UNS:Designing Metal-Exchanged Zeolites with Improved Activity, Selectivity and Stability for Non-Oxidative Methane Upgrade

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1512224(Rimer)The study addresses a critical area of catalysis research - upgrading of methane to higher value products - brought on by the emergence of large quantities of shale gas resources in the United States, along with both commercial and environmental incentives to avoid gas flaring and instead convert the gas to higher value, transportable, fuel and chemical products. Zeolite catalysis represents a potential path to methane upgrading. The study will focus on the design of new zeolite catalysts with improved capability, utilizing both experimental methods and theoretical tools. The proposed work brings together expertise in zeolite synthesis and characterization, kinetic studies, and density functional theory calculations to design metal-exchanged zeolites with improved product yield and durability for non-oxidative methane upgrading via two processes: non-oxidative coupling and dehydroaromtization. To this end the work will focus on 4 specific aims related to Lewis acidity (associated with different exchanged metals), confinement effects, choice of zeolite framework, and a theory-guided screening protocol for mixed metal zeolites. Given the complexity of the reactions and the reaction environment within the zeolite structures, the linkage between synthesis, characterization and theory is especially needed for significant advances to be made in zeolite-based methane upgrading. The emergence of large quantities of shale gas has dramatically changed the commercial and environmental landscape for natural gas resources. Much of the remote gas is presently flared with the production of large quantities of carbon dioxide - a major contributor to the greenhouse gas inventory. Direct processes for converting methane to higher value liquid fuel and chemical products are sorely needed. Yet the catalytic challenge is daunting. This proposal will address the current gap in technology and will provide a theoretical basis for future research in the area of zeolite-based methane conversion processes. To this end, it has potential to significantly advance our understanding of both the challenges associated with direct catalytic methane upgrading and the potential utility of zeolite-based catalysis for overcoming those challenges. The PIs will also conduct education and outreach programs to students at all levels to raise awareness of the role of STEM disciplines in addressing energy-related issues.