546501 Regenerable Single Atom Catalysts for Propane Dehydrogenation

Monday, June 3, 2019: 11:27 AM
Republic ABC (Grand Hyatt San Antonio)
Griffin A. Canning1, Ryan Alcala1, Haifeng Xiong1, Megan Senn1, Nicole LiBretto2, Jeffrey T. Miller2, Fabio H. Ribero2 and Abhaya Datye1, (1)Chemical and Biological Engineering, Center for Microengineered Materials, University of New Mexico, Albuquerque, NM, (2)Charles D. Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN

Single atom catalysts are currently of great interest due to high selectivity, reactivity and excellent atom efficiency. Here we have explored the use of single atom catalysts for high temperature reactions involving alkane conversions. The work is motivated by the availability of natural gas due to advancements in fracking and drilling technologies. The increased production has led to lower costs, which are beneficial in lowering the carbon footprint of fuels when methane is used to replace coal for electricity production. Ethane and other natural gas liquids (NGLs) recovered from shale with methane, however, have limited markets resulting in export of US produced ethane to Europe starting in 2016. These NGLs are attractive as feedstocks for chemical production. The conversion of these NGLs to value added products involves dehydrogenation as the first step. This has traditionally been done through steam cracking or catalytic dehydrogenation, both of which require large plants. Platinum based catalysts require regeneration which requires significant catalyst handling and the use of corrosive, halogen based treatments. The use of single atom catalysts provides an alternative approach which also alleviates the problem of coke formation which is less likely on single sites.

In previous work we have demonstrated the ease of synthesis of single atom Pt catalysts via vapor phase synthesis on industrial catalyst supports1. These single atom catalysts are regenerable using oxidizing conditions at modest temperatures2. The focus of the present work is the use of single atom dopants as modifiers to improve the selectivity and stability of the single atom catalysts for alkane conversions. Characterization via Aberration Corrected STEM and X-ray absorption spectroscopy helps us advance the applications of SACs to industrially relevant reactions.

(1) Jones, J.; Xiong, H.; DeLaRiva, A. T.; Peterson, E. J.; Pham, H.; Challa, S. R.; Qi, G.; Oh, S.; Wiebenga, M. H.; Hernández, X. I. P.; et al. Thermally Stable Single-Atom Platinum-on-Ceria Catalysts via Atom Trapping. Science (80-. ). 2016, 353 (6295), 150–154.

(2) Xiong, H.; Lin, S.; Goetze, J.; Pletcher, P.; Guo, H.; Kovarik, L.; Artyushkova, K.; Weckhuysen, B. M.; Datye, A. K. Thermally Stable and Regenerable Platinum–Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria. Angew. Chemie - Int. Ed. 2017, 56 (31), 8986–8991.

Extended Abstract: File Not Uploaded
See more of this Session: Direct Dehydrogenation of Alkanes
See more of this Group/Topical: General Submissions