EAGER: Selectivity Control in Direct Non-oxidative Methane Conversion over Fe?SiO2 Catalyst by Manipulating the Feed Composition

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The project is an exploratory study aimed at confirming and extending a report published in Science (Guo et al. 2014) of an iron-silica catalyst and reaction conditions leading to direct, non-oxidative, methane conversion (DNMC) to higher-value chemical feedstocks including ethylene, benzene, and naphthalene. The technology, if proven, represents a significant technological breakthrough with transformative potential for converting the large quantities of shale gas derived methane to transportable, high-value chemical feedstocks rather than the current practice of flaring with associated emissions of the greenhouse gas, carbon dioxide.The underlying challenge in methane chemistry is active and selective catalytic conversion to form fuels and chemicals in an economical approach without deactivating the catalyst via thermal processes or coke formation. The PIs will elucidate the reaction pathways and mechanisms in the DNMC reactions over Fe©SiO2 catalyst by ex-situ analysis of catalyst fine structures and using Molecular Beam Mass Spectroscopy (MBMS)to analyze both stable and radical gas phase reaction intermediates and products. The study will also evaluate the effects of hydrogen and hydrocarbon species on catalysis as a parameter to control DNMC and demonstrate its applicability in context of the following specific aims: (i) Successfully synthesize the catalyst and understand its activation mechanism; (ii) Systematically tune the product selectivity and methane conversion by controlling the feed stream compositions; (iii) Rigorously describe the kinetic effects of feed composition on methane reaction pathways and catalyst deactivation. The proposed research will provide specific guidance for the development of catalysts and processes useful in manufacturing value-added products from low cost methane gas resources. To this end the broader impact of a practical DNMC process would transform the fuels and chemicals industry while reducing the atmospheric burden of CO2 and the impact of fossil resources on global warming. The technology could also have potential application in other areas such as processing of pyrolysis gases from biorenewable sources. The study will create a unique opportunity for graduate and undergraduate students to experience cross-cutting education in aspects of catalysis, reaction engineering, gas analysis, and chemical kinetics.This award is co-funded by the Engineering Directorate Office of Emerging Frontiers and Multidisciplinary Activities.