Propane Dehydrogenation on Single-Site [PtZn4] Intermetallic Catalysts

Chen, Sai; Zhao, Zhi-Jian; Mu, Rentao; Chang, Xin; Luo, Jun; Purdy, Stephen C.; Kropf, A. Jeremy; Sun, Guodong; Pei, Chunlei; Miller, Jeffrey T.; Zhou, Xiaohong; Vovk, Evgeny; Yang, Yong; Gong, Jinlong

doi:10.1016/j.chempr.2020.10.008

DOE OSTI · 1819661

Propane Dehydrogenation on Single-Site [PtZn4] Intermetallic Catalysts

Chen, Sai·Zhao, Zhi-Jian·Mu, Rentao·Chang, Xin·Luo, Jun·Purdy, Stephen C.·Kropf, A. Jeremy·Sun, Guodong·Pei, Chunlei·Miller, Jeffrey T.·Zhou, Xiaohong·Vovk, Evgeny·Yang, Yong·Gong, Jinlong

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Abstract

Propane dehydrogenation (PDH) is a commercial propylene production technology that has received much attention, but high reaction temperature results in decrease of propylene selectivity and catalyst stability. This paper describes a single-site [PtZn 4 ] catalyst by assembling atomically ordered intermetallic alloy (IMA) as a selective and ultrastable PDH catalyst. The catalyst enables more than 95% propylene selectivity from 520 to 620 oC. No obvious deactivation is observed within 160-hours test, superior to PtSn/Al 2 O 3 and state-of-the-art Pt-based catalysts. Additionally, based on in situ X-ray absorption fine-structure, X-ray photoelectron spectroscopy measurements and density functional theory calculations, we reveal that the surface [PtZn 4 ] ensembles in PtZn IMAs serve as the key active site structures, wherein the geometry-isolated and electron-rich Pt1 site in [PtZn 4 ] ensembles readily promotes the first and second C–H cleavage of propane, but inhibits further dehydrogenation of surface-bounded propylene. This significantly improves the selectivity and stability by prohibiting coke side reactions.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Pt catalyst intermetallic alloy propane dehydrogenation single-site catalysts

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Chen, Sai, Zhao, Zhi-Jian, Mu, Rentao, Chang, Xin, Luo, Jun, Purdy, Stephen C., Kropf, A. Jeremy, Sun, Guodong, Pei, Chunlei, Miller, Jeffrey T., Zhou, Xiaohong, Vovk, Evgeny, Yang, Yong, Gong, Jinlong. 2020-11-04. Propane Dehydrogenation on Single-Site [PtZn4] Intermetallic Catalysts. https://doi.org/10.1016/j.chempr.2020.10.008

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