Propane dehydro-aromatization reaction over PtFe@S-1 coupling with Zn/ZSM-5 tandem catalysts: the role of Zn species

doi:10.1007/s11705-024-2440-2

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (8) : 87 https://doi.org/10.1007/s11705-024-2440-2

Propane dehydro-aromatization reaction over PtFe@S-1 coupling with Zn/ZSM-5 tandem catalysts: the role of Zn species

Kai Bian^1,², Sirui Liu², Huahua Fan², Guanghui Zhang²(

), Xinwei Zhang¹, Gideon Abaidoo Ocran², Mingrui Wang², Quanjie Liu¹, Xiaowa Nie², Shuandi Hou¹(

), Xinwen Guo²(

)

¹. Sinopec Dalian Research Institute of Petroleum and Petrochemicals, Dalian 116045, China
². State Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China

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Abstract

Unraveling the structure-activity relationship and improving the catalytic performance is paramount in propane dehydro-aromatization reactions. Herein, a tandem catalyst with high propane dehydro-aromatization reaction performance was prepared via coupling the PtFe@S-1 with Zn/ZSM-5 zeolites (PtFe@S-1&1.0Zn/ZSM-5), which exhibits high dehydrogenation activity, aromatics selectivity (~60% at ~78% propane conversion), and stability. The addition of zinc inhibits the cleavage of C₆⁼ intermediates on ZSM-5 and promotes the aromatization pathway by weakening zeolite acid strength, significantly improving the selectivity to aromatics. This understanding of the structure-activity relationship in propane dehydro-aromatization reaction helps develop future high-performance catalysts.

Keywords propane dehydro-aromatization reaction tandem catalysts the structure-activity relationship of zinc species

Corresponding Author(s): Guanghui Zhang,Shuandi Hou,Xinwen Guo

Just Accepted Date: 15 March 2024 Issue Date: 28 April 2024

Cite this article:

Kai Bian,Sirui Liu,Huahua Fan, et al. Propane dehydro-aromatization reaction over PtFe@S-1 coupling with Zn/ZSM-5 tandem catalysts: the role of Zn species[J]. Front. Chem. Sci. Eng., 2024, 18(8): 87.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2440-2
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I8/87

Scheme1 The design of tandem catalysts in PDA reaction.

Fig.1 (a) The XRD patterns and (b) UV-Vis spectra of ZSM-5-25 and xZn/ZSM-5 samples.

Fig.2 The SEM images for the reduced PtFe@S-1, ZSM-5-25 and xZn/ZSM-5 samples. (a, b) PtFe@S-1; (c) ZSM-5-25; (d) 0.5Zn/ZSM-5; (e) 1.0Zn/ZSM-5; (f) 2.0Zn/ZSM-5.

Fig.3 The PDA catalytic performance for (a, c, e) PtFe@S-1&ZSM-5-25 and (b, d, f) PtFe@S-1&1.0Zn/ZSM-5 catalysts with different filling methods (Dual bed; granule stack and powder mixing; reaction conditions: T = 550 °C, ambient pressure, 0.15 g of PtFe@S-1 (blue ball) and 0.15 g of ZSM-5-25 or 1.0Zn/ZSM-5 zeolites (yellow ball), C₃H₈/N₂ = 5/35 mL·min^–1).

Fig.4 The mass spectra of C₃H₈-TPSR results on (a) ZSM-5-25, (b) 1.0Zn/ZSM-5, (c) PtFe@S-1, (d) PtFe@S-1&ZSM-5-25, and (e) PtFe@S-1&1.0Zn/ZSM-5.

Scheme2 The conjecture on the role of zinc in dehydro-aromatization of propane catalyzed by PtFe@S-1&1.0Zn/ZSM-5.

Fig.5 The catalytic performance of propylene conversion on (a) ZSM-5-25, (b) Pt/ZSM-5, (c) PtFe/ZSM-5 and (d) 1.0Zn/ZSM-5 (reaction conditions: T = 550 °C, ambient pressure, 0.07 g of catalysts, C₃H₆/N₂ = 1.25/30 mL·min^–1).

Fig.6 The catalytic performance of (a) cyclohexene and (b) 1-hexene conversion on different catalysts (reaction conditions: T = 550 °C, ambient pressure, 0.07 g of catalysts, C₆H₁₂/N₂ = 0.02/40 mL·min^–1).

Fig.7 The optimal reaction energy diagrams of 1-hexene cracking to C₂ and C₄ olefins on (a) ZSM-5 and (b) Zn/ZSM-5.

Fig.8 (a) The C₃H₆-TPD, (b) NH₃-TPD and (c) Py-IR spectra for ZSM-5-25 and different xZn/ZSM-5 samples.

Fig.9 The PDA catalytic performance for PtFe@S-1&xZn/ZSM-5 with different amount of Zn. (a) ZSM-5-25; (b) 0.5Zn/ZSM-5; (c) 1.0Zn/ZSM-5; (d) 2.0Zn/ZSM-5 (reaction conditions: T = 550 °C, ambient pressure, 0.30 g of PtFe@S-1&xZn/ZSM-5, C₃H₈/N₂ = 5/35 mL·min^–1).

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