UNS:Collaborative Reasearch: Hydrocarbon conversion on oxysulfide surfaces: Towards the design of sulfur-tolerant reforming catalysts

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1510435 (Dooley), 1510541(Janik)Sulfur-containing compounds are ubiquitous impurities in petroleum resources that poison catalysts used for the refining and upgrading of both crude oil and natural gas to fuels and chemicals. The proposed research seeks to develop and understand novel sulfur-tolerant catalysts for the conversion of natural gas to gases used to synthesize liquid fuels and chemicals. To this end, the work has potential to develop a simplified, efficient process for natural gas conversion without the need for expensive "upstream" desulfurization. The researchers will also advance education and scientific awareness by involving undergraduate students in their research with an emphasis on minority, women, and first-generation students.Large quantities of natural gas are being produced from shale resources, providing opportunities to convert the gas to liquid fuels via reforming reactions. This study reforms methane by reacting it with carbon dioxide, thus generating feedstocks for liquid fuels while reducing the atmospheric loading of carbon dioxide (a greenhouse gas). A combination of experimental and theoretical tools will be used to design mixed metal oxide catalysts (combining transition metals and rare earth oxides) that are both sulfur tolerant and less prone to poisoning by coking than current catalysts. Specifically, the work addresses the hypothesis that the mixed transition metal and rare earth oxide catalysts form stable and active oxysulfides under reaction conditions, with the benefit that the oxysulfides destabilize coke precursors. Computational methods will be used to predict candidate oxysulfided catalyst materials that will then be synthesized, tested, and characterized, with results used to refine the theoretical predictions. Beyond the direct research, the two PIs on this project have a strong track record of educational outreach at their respective institutions including involvement of undergraduates in their research programs and Dooley's work with the "You be the Chemist Challenge" of the Louisiana Chemical Education Foundation (focused on middle- and high-school students).