Elucidation of quantitative effects of zeolitic pores in Mo-impregnated MWW type zeolites on catalytic activities and stabilities of methane dehydroaromatization reaction

  • Gihoon Lee
  • , Tristan James Sim
  • , Yanghwan Jeong
  • , Taehee Lee
  • , Hionsuck Baik
  • , Ji Chul Jung
  • , Kyoung Su Ha
  • , Sung June Cho
  • , Alex C.K. Yip*
  • , Jungkyu Choi
  • *Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    Abstract

    The quantitative effects of the pores in Mo-impregnated zeolites on their catalytic activity and stability during methane dehydroaromatization (MDA) were investigated. For this, MCM-22 (Mobil Composition of Matter-22) and its derivatives (MCM-36, ITQ-2, and delaminated MCM-22 in this study), having MWW type zeolite topologies but different zeolite structures, were applied. Although Mo-impregnated catalysts exhibited different catalytic activities and stabilities, interestingly, all Mo-impregnated catalysts showed similar intrinsic benzene-toluene formation rates per zeolitic pore at the initial time-on-stream regardless of the different structures. Moreover, investigation of spent Mo-impregnated catalysts revealed that the coke deposited inside the zeolitic channels (viz., internal coke) was the cause of catalyst deactivation. In particular, the preferential deposition of internal coke in the 12-membered-ring supercage can retard zeolite channel blocking and, consequently, catalyst deactivation. Thus, the amount of zeolitic pore volumes in the catalyst structure is a crucial factor that determines the catalytic activity and stability during MDA.

    Original languageEnglish
    Article number119184
    JournalApplied Catalysis A: General
    Volume659
    DOIs
    Publication statusPublished - 2023 Jun 5

    Bibliographical note

    Funding Information:
    This work was supported by the C1 Gas Refinery Program ( 2018M3D3A1A01018004 ) and the Mid-Career Researcher Program ( 2020R1A2C1101974 ) through the National Research Foundation of Korea (NRF) funded by the Korea Government (Ministry of Science and ICT; MSIT). TEM characterizations were conducted at the Seoul Center in the Korea Basic Science Institute (KBSI). We would like to thank Ms. Jisong Kang and Dr. Jeong-Myeong Ha (Korea Institute of Science and Technology) for Raman spectroscopy measurements.

    Funding Information:
    This work was supported by the C1 Gas Refinery Program (2018M3D3A1A01018004) and the Mid-Career Researcher Program (2020R1A2C1101974) through the National Research Foundation of Korea (NRF) funded by the Korea Government (Ministry of Science and ICT; MSIT). TEM characterizations were conducted at the Seoul Center in the Korea Basic Science Institute (KBSI). We would like to thank Ms. Jisong Kang and Dr. Jeong-Myeong Ha (Korea Institute of Science and Technology) for Raman spectroscopy measurements.

    Publisher Copyright:
    © 2023 Elsevier B.V.

    Keywords

    • CH utilization
    • Deactivation
    • Hierarchical MWW zeolites
    • MCM-22
    • Methane dehydroaromatization

    ASJC Scopus subject areas

    • Catalysis
    • Process Chemistry and Technology

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