Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (10): 1689-1699.DOI: 10.1016/S1872-2067(20)63775-5

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Methane combustion over palladium catalyst within the confined space of MFI zeolite

Mingyang Gaoa, Zhongmiao Gongb, Xuefei Wengb, Weixiang Shanga, Yuchao Chaia, Weili Daia, Guangjun Wua, Naijia Guana, Landong Lia()   

  1. aSchool of Materials Science and Engineering, Nankai University, Tianjin 300350, China
    bVacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123,Jiangsu, China
  • Received:2021-01-15 Accepted:2021-01-29 Online:2021-10-18 Published:2021-02-03
  • Contact: Landong Li
  • About author:Professor Landong Li received his B.S. in 2001 and Ph.D degree in 2006 from Nankai University. From 2006 to 2009, he worked in the Research Center of Eco-environment Science, CAS, as an assistant professor. Afterwards, he moved back to Nankai University, where he now holds a position of Talent Professor. His research interests currently focus on zeolite adsorption and catalysis with emphases on both fundamental understandings and industrial applications. Some of his recent progresses include the construction of coordinatively unsaturated sites confined in zeolites, the selective transformation of small molecules over zeolite catalysts and the chemoselective separation of small molecules by decorated zeolites. He has published over 150 peer-reviewed papers, 30 authorized patents, and received the National Science Fund for Distinguished Young Scholars. He joined the Editorial Board of Chin. J Catal. in 2020.
  • Supported by:
    National Natural Science Fundation of China(22025203);National Natural Science Fundation of China(21872072);Municipal Natural Science Fund of Tianjin(18JCJQJC47400);Nano-X (SINANO, CAS)

Abstract:

Isolated cationic Pd species encapsulated in MFI zeolite, i.e., Pd@MFI, have been successfully prepared via in situ hydrothermal route followed by oxidative treatment. The as-prepared Pd@MFI samples are investigated as promising catalysts in the reaction of methane combustion. Typically, Pd@H-ZSM-5 shows remarkable activity in methane catalytic combustion with a low apparent activation energy value of 70.7 kJ/mol as well as good catalytic stability even in excess water vapor. Detailed characterization results demonstrate the strong interaction between Pd sites and zeolite framework in Pd@ZSM-5 and the efficient stabilization of isolated Pd sites by zeolite thereof. Spectroscopy analyses reveal that the presence of Brønsted acid sites is beneficial to methane adsorption and its subsequent activation on adjacent Pd sites, constructing cooperation between Brønsted acid sites and Pd sites within the confined space of MFI zeolite toward high-efficiency methane catalytic combustion. The reaction mechanism of methane combustion catalyzed by Pd@H-ZSM-5 model catalyst is finally discussed.

Key words: Methane combustion, Palladium catalyst, Zeolite, Encapsulation, Br?nsted acid sites