能源化学(英文版)

能源化学(英文) ›› 2019, Vol. 28 ›› Issue (7): 96-103.DOI: 10.1016/j.jechem.2018.09.009

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Pt supported on Zn modified silicalite-1 zeolite as a catalyst for n-hexane aromatization

Guodong Liua, Jiaxu Liua, Ning Hea, Shishan Shengb, Guiru Wanga, Hongchen Guoa   

  1. a Department of Catalytic Chemistry and Engineering & State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning, China;
    b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • 收稿日期:2018-08-04 修回日期:2018-09-12 出版日期:2019-07-15 发布日期:2019-07-15
  • 通讯作者: Hongchen Guo
  • 基金资助:
    This work is financially supported by the National Natural Science Foundation of China (21603023).

Pt supported on Zn modified silicalite-1 zeolite as a catalyst for n-hexane aromatization

Guodong Liua, Jiaxu Liua, Ning Hea, Shishan Shengb, Guiru Wanga, Hongchen Guoa   

  1. a Department of Catalytic Chemistry and Engineering & State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning, China;
    b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • Received:2018-08-04 Revised:2018-09-12 Online:2019-07-15 Published:2019-07-15
  • Contact: Hongchen Guo
  • Supported by:
    This work is financially supported by the National Natural Science Foundation of China (21603023).

摘要： Platinum (Pt) supported on Zinc (Zn) modified silicalite-1 (S-1) zeolite (denoted as Pt-Zn/S-1) was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time. Both Lewis and Brønsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH3 experiment, which were identified as mostly weak and medium ones. Besides, Pt and Zn species showed strong interaction, as revealed by the TPR (Temperature-programmed reduction) and XPS (X-ray photoelectron spectroscopy) experiments. Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane. Pulse experimental study showed that 75.6% of n-hexane conversion and 76.8% of benzene selectivity were obtained over Pt0.1-Zn6.0/S-1 catalyst at 550℃ and under atmospheric pressure. By spectroscopy tests and pulse experimental results, it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism. Furthermore, with the assistance of Zn, the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.

关键词: Silicalite-1 zeolite, Pt-Zn/Silicalite-1, n-Hexane aromatization, Sulfur-resistance

Abstract: Platinum (Pt) supported on Zinc (Zn) modified silicalite-1 (S-1) zeolite (denoted as Pt-Zn/S-1) was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time. Both Lewis and Brønsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH3 experiment, which were identified as mostly weak and medium ones. Besides, Pt and Zn species showed strong interaction, as revealed by the TPR (Temperature-programmed reduction) and XPS (X-ray photoelectron spectroscopy) experiments. Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane. Pulse experimental study showed that 75.6% of n-hexane conversion and 76.8% of benzene selectivity were obtained over Pt0.1-Zn6.0/S-1 catalyst at 550℃ and under atmospheric pressure. By spectroscopy tests and pulse experimental results, it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism. Furthermore, with the assistance of Zn, the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.

Key words: Silicalite-1 zeolite, Pt-Zn/Silicalite-1, n-Hexane aromatization, Sulfur-resistance