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

1510435(杜利)、1510541(雅尼克)含硫化合物是石油资源中普遍存在的杂质，会毒害用于将原油和天然气提炼和升级为燃料和化学品的催化剂。这项拟议的研究旨在开发和了解新型耐硫催化剂，用于将天然气转化为用于合成液体燃料和化学品的气体。为此，这项工作有可能开发一种简化、高效的天然气转化过程，而不需要昂贵的“上游”脱硫。研究人员还将提高教育和科学意识，让本科生参与他们的研究，重点是少数民族、女性和第一代学生。大量的天然气是从页岩资源中生产的，这为通过重整反应将天然气转化为液体燃料提供了机会。这项研究通过使甲烷与二氧化碳反应来改革甲烷，从而产生液体燃料的原料，同时减少大气中二氧化碳(一种温室气体)的负荷。将使用实验和理论工具相结合的方法来设计混合金属氧化物催化剂(结合过渡金属和稀土氧化物)，与目前的催化剂相比，这些催化剂既耐硫，又不容易结焦中毒。具体地说，这项工作提出了这样的假设，即混合过渡金属和稀土氧化物催化剂在反应条件下形成稳定和活性的硫氧化合物，好处是这些硫氧化物破坏焦炭前体的稳定性。计算方法将被用来预测候选的氧硫化催化剂材料，然后将被合成、测试和表征，结果用于完善理论预测。除了直接的研究，这个项目的两位PI在各自机构的教育推广方面有着良好的记录，包括本科生参与他们的研究计划，以及Dooley在路易斯安那州化学教育基金会(专注于初中生)的“你是化学家的挑战”中的工作。

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).