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Hexane Aromatization: Analysis of the K-Edges of S and K Provides New Insight into H2S Poisoning of Pt/KL

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Abstract

The purpose of this investigation was to examine the effect of sulfur impurity on 1%Pt/KL-zeolite catalyst by co-feeding 500 ppbv hydrogen sulfide (H2S) during hexane aromatization under industrially relevant conditions using a plug flow reactor. Product selectivity and hexane conversion were measured with time-on-stream and compared to a clean run carried out under otherwise identical conditions. Sulfur addition to the feed accelerated the rate of deactivation as observed by rapid declines in both hexane conversion and benzene selectivity; hexene selectivity, the product of the less structurally sensitive dehydrogenation reaction, increased significantly. After 20 h, which was enough time to observe sufficient deactivation, the reaction was stopped. For the purpose of catalyst characterization, after cooling to 150 °C, the catalyst was preserved in Polywax 725 to prevent catalyst oxidation. XANES analysis at the potassium K-edge suggests that the local environment for potassium was not significantly altered by sulfur addition, while sulfur K-edge results indicate that sulfur bound to platinum to form platinum sulfide (PtS, not PtS2). Platinum sulfide is likely responsible for accelerating Pt growth, as observed in DRIFTS of adsorbed CO and HR-TEM/STEM micrographs.

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reproduced with permission from Taylor & Francis (2016)

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Acknowledgements

This work carried out at the CAER was supported by the Commonwealth of Kentucky. Research described in this paper was performed in part at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan.

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Authors and Affiliations

  1. Center for Applied Energy Research, University of Kentucky, 2540 Research Park Drive, Lexington, KY, 40511, USA

    Wilson D. Shafer, Gary Jacobs, Venkat Rao Ramana Pendyala, Michela Martinelli, Gerald A. Thomas, Thani Jermwongratanachai & Burtron H. Davis

  2. Asbury University, One Macklem Drive, Wilmore, KY, 40390, USA

    Wilson D. Shafer

  3. Chemical Engineering Program - Department of Biomedical Engineering, and Department of Mechanical Engineering, University of San Antonio, One UTSA Circle, San Antonio, TX, 78249, USA

    Gary Jacobs

  4. Topasol, 1525 Bull Lea Rd. Suite # 5, Lexington, KY, 40511, USA

    Uschi M. Graham

  5. Canadian Light Source, Inc., 44 Innovation Blvd., Saskatoon, SK-S7N 2V3, Canada

    Aimee MacLennan & Yongfeng Hu

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  1. Wilson D. Shafer
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Correspondence to Burtron H. Davis.

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Shafer, W.D., Jacobs, G., Graham, U.M. et al. Hexane Aromatization: Analysis of the K-Edges of S and K Provides New Insight into H2S Poisoning of Pt/KL. Catal Lett 148, 97–107 (2018). https://doi.org/10.1007/s10562-017-2242-y

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