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

Propane Dehydrogenation on Single-Site [PtZn4] Intermetallic Catalysts

Journal Article · Wed Nov 04 00:00:00 EST 2020 · Chem

DOI:https://doi.org/10.1016/j.chempr.2020.10.008· OSTI ID:1819661

Chen, Sai ^[1]; Zhao, Zhi-Jian ^[1]; Mu, Rentao ^[1]; Chang, Xin ^[1]; Luo, Jun ^[2]; Purdy, Stephen C. ^[3]; Kropf, A. Jeremy ^[4]; Sun, Guodong ^[1]; Pei, Chunlei ^[1]; Miller, Jeffrey T. ^[3]; Zhou, Xiaohong ^[5]; Vovk, Evgeny ^[5]; Yang, Yong ^[5]; Gong, Jinlong ^[6]

Tianjin Univ. (China). Key Lab. for Green Chemical Technology; Collaborative Innovation Center for Chemical Science & Engineering, Tianjin (China)
Tianjin Univ. of Technology (China). Inst. for New Energy Materials and Low-Carbon Technologies, Center for Electron Microscopy
Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
ShanghaiTech Univ. (China)
Tianjin Univ. (China). Key Lab. for Green Chemical Technology; Collaborative Innovation Center for Chemical Science & Engineering, Tianjin (China); Joint School of National Univ. of Singapore and Tianjin Univ., Tianjin (China)

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 [PtZn₄] 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/Al₂O₃ 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 [PtZn₄] ensembles in PtZn IMAs serve as the key active site structures, wherein the geometry-isolated and electron-rich Pt1 site in [PtZn₄] 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Materials Research Collaborative Access Team (MRCAT); National Natural Science Foundation of China (NSFC); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1819661

Journal Information:: Chem, Journal Name: Chem Journal Issue: 2 Vol. 7; ISSN 2451-9294

Publisher:: Cell Press, ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Propane Dehydrogenation on Single-Site [PtZn4] Intermetallic Catalysts

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