Standardization of catalyst preparation using reference catalyst: Ion exchange of mordenite type zeolite, Remarkable dealumination accompanying ion exchange

Naonobu Katada, Tatsuya Takeguchi, Tatsuya Suzuki, Toshihisa Fukushima, Kinya Inagaki, Setsuo Tokunaga, Hiromichi Shimada, Koichi Sato, Yasunori Oumi, Tsuneji Sano, Kohichi Segawa, Kazuyuki Nakai, Hiroshi Shoji, Peng Wu, Takashi Tatsumi, Takayuki Komatsu, Takao Masuda, Kazunari Domen, Eisuke Yoda, Junko N. KondoToshio Okuhara, Yasuyoshi Kageyama, Miki Niwa, Masaru Ogura, Masahiko Matsukata, Eiichi Kikuchi, Noriyasu Okazaki, Motoi Takahashi, Akio Tada, Shogo Tawada, Yoshihiro Kubota, Yoshihiro Sugi, Yasuhiko Higashio, Masahiko Kamada, Yukiyo Kioka, Kohei Yamamoto, Takayuki Shouji, Yusaku Arima, Yasuaki Okamoto, Hideyuki Matsumoto

    Research output: Contribution to journalArticle

    15 Citations (Scopus)

    Abstract

    A joint study was organized to establish a standard set of conditions for the ion exchange of zeolite from sodium into proton-form. The sodium-form mordenite with Si/Al2 = ca. 15 was ion exchanged into an NH4-form, followed by calcination according to various recipes. Then various advanced techniques for characterization (ICP, TG, XPS, SEM, XRD, N2 adsorption, 29Si and 27AlNMR, benzene diffusion, IR of OH and adsorbed pyridine and CO, ammonia TPD) were applied, and some test reactions (cracking of cumene, isopropylation of biphenyl, oligomerization of propene and chichibabin condensation of acetaldehyde and ammonia into picoline) were conducted. The ion exchange (removal of sodium) proceeded as expected, but remarkable differences were observed in physicochemical and catalytic properties of the thus-prepared proton-form samples. Exceptionally high temperature (383 K) for the ion exchange resulted in the structural degradation, while most samples exchanged at 333-353 K maintained the crystallinity and pore volume. The use of NH4Cl slightly changed the crystal morphology. Extra-framework aluminum species was formed on most samples after calcination above 773 K. In contrast, calcination at 673 K maintained the framework aluminum. Therefore, the dealumination is considered to proceed after complete removal of ammonia from the ammonium-form zeolite. However, the proton-form zeolite was stable under dry conditions, so it is speculated that the dealumination was induced by the contact of the proton-form zeolite to atmosphere with humidity. The total and Brønsted acidity decreased with the dealumination, while Lewis acidity increased. On the other hand, rapid heating of the ammonium type zeolite caused narrowing of the micropores. These structural changes seriously affected the catalytic activities for various reactions.

    Original languageEnglish
    Pages (from-to)63-74
    Number of pages12
    JournalApplied Catalysis A: General
    Volume283
    Issue number1-2
    DOIs
    Publication statusPublished - 2005 Apr 8

    Fingerprint

    Zeolites
    Standardization
    Ion exchange
    Protons
    Calcination
    Ammonia
    Catalysts
    Sodium
    Acidity
    Aluminum
    Ammonium Compounds
    Picolines
    Oligomerization
    Acetaldehyde
    Temperature programmed desorption
    Pyridine
    Propylene
    Condensation
    Catalyst activity
    Carbon Monoxide

    Keywords

    • Acidity
    • Catalyst preparation
    • Dealumination
    • Ion exchange
    • Mordenite
    • Reference catalyst
    • Standardization
    • Zeolite

    ASJC Scopus subject areas

    • Catalysis
    • Process Chemistry and Technology

    Cite this

    Standardization of catalyst preparation using reference catalyst : Ion exchange of mordenite type zeolite, Remarkable dealumination accompanying ion exchange. / Katada, Naonobu; Takeguchi, Tatsuya; Suzuki, Tatsuya; Fukushima, Toshihisa; Inagaki, Kinya; Tokunaga, Setsuo; Shimada, Hiromichi; Sato, Koichi; Oumi, Yasunori; Sano, Tsuneji; Segawa, Kohichi; Nakai, Kazuyuki; Shoji, Hiroshi; Wu, Peng; Tatsumi, Takashi; Komatsu, Takayuki; Masuda, Takao; Domen, Kazunari; Yoda, Eisuke; Kondo, Junko N.; Okuhara, Toshio; Kageyama, Yasuyoshi; Niwa, Miki; Ogura, Masaru; Matsukata, Masahiko; Kikuchi, Eiichi; Okazaki, Noriyasu; Takahashi, Motoi; Tada, Akio; Tawada, Shogo; Kubota, Yoshihiro; Sugi, Yoshihiro; Higashio, Yasuhiko; Kamada, Masahiko; Kioka, Yukiyo; Yamamoto, Kohei; Shouji, Takayuki; Arima, Yusaku; Okamoto, Yasuaki; Matsumoto, Hideyuki.

    In: Applied Catalysis A: General, Vol. 283, No. 1-2, 08.04.2005, p. 63-74.

    Research output: Contribution to journalArticle

    Katada, N, Takeguchi, T, Suzuki, T, Fukushima, T, Inagaki, K, Tokunaga, S, Shimada, H, Sato, K, Oumi, Y, Sano, T, Segawa, K, Nakai, K, Shoji, H, Wu, P, Tatsumi, T, Komatsu, T, Masuda, T, Domen, K, Yoda, E, Kondo, JN, Okuhara, T, Kageyama, Y, Niwa, M, Ogura, M, Matsukata, M, Kikuchi, E, Okazaki, N, Takahashi, M, Tada, A, Tawada, S, Kubota, Y, Sugi, Y, Higashio, Y, Kamada, M, Kioka, Y, Yamamoto, K, Shouji, T, Arima, Y, Okamoto, Y & Matsumoto, H 2005, 'Standardization of catalyst preparation using reference catalyst: Ion exchange of mordenite type zeolite, Remarkable dealumination accompanying ion exchange', Applied Catalysis A: General, vol. 283, no. 1-2, pp. 63-74. https://doi.org/10.1016/j.apcata.2004.12.036
    Katada, Naonobu ; Takeguchi, Tatsuya ; Suzuki, Tatsuya ; Fukushima, Toshihisa ; Inagaki, Kinya ; Tokunaga, Setsuo ; Shimada, Hiromichi ; Sato, Koichi ; Oumi, Yasunori ; Sano, Tsuneji ; Segawa, Kohichi ; Nakai, Kazuyuki ; Shoji, Hiroshi ; Wu, Peng ; Tatsumi, Takashi ; Komatsu, Takayuki ; Masuda, Takao ; Domen, Kazunari ; Yoda, Eisuke ; Kondo, Junko N. ; Okuhara, Toshio ; Kageyama, Yasuyoshi ; Niwa, Miki ; Ogura, Masaru ; Matsukata, Masahiko ; Kikuchi, Eiichi ; Okazaki, Noriyasu ; Takahashi, Motoi ; Tada, Akio ; Tawada, Shogo ; Kubota, Yoshihiro ; Sugi, Yoshihiro ; Higashio, Yasuhiko ; Kamada, Masahiko ; Kioka, Yukiyo ; Yamamoto, Kohei ; Shouji, Takayuki ; Arima, Yusaku ; Okamoto, Yasuaki ; Matsumoto, Hideyuki. / Standardization of catalyst preparation using reference catalyst : Ion exchange of mordenite type zeolite, Remarkable dealumination accompanying ion exchange. In: Applied Catalysis A: General. 2005 ; Vol. 283, No. 1-2. pp. 63-74.
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    abstract = "A joint study was organized to establish a standard set of conditions for the ion exchange of zeolite from sodium into proton-form. The sodium-form mordenite with Si/Al2 = ca. 15 was ion exchanged into an NH4-form, followed by calcination according to various recipes. Then various advanced techniques for characterization (ICP, TG, XPS, SEM, XRD, N2 adsorption, 29Si and 27AlNMR, benzene diffusion, IR of OH and adsorbed pyridine and CO, ammonia TPD) were applied, and some test reactions (cracking of cumene, isopropylation of biphenyl, oligomerization of propene and chichibabin condensation of acetaldehyde and ammonia into picoline) were conducted. The ion exchange (removal of sodium) proceeded as expected, but remarkable differences were observed in physicochemical and catalytic properties of the thus-prepared proton-form samples. Exceptionally high temperature (383 K) for the ion exchange resulted in the structural degradation, while most samples exchanged at 333-353 K maintained the crystallinity and pore volume. The use of NH4Cl slightly changed the crystal morphology. Extra-framework aluminum species was formed on most samples after calcination above 773 K. In contrast, calcination at 673 K maintained the framework aluminum. Therefore, the dealumination is considered to proceed after complete removal of ammonia from the ammonium-form zeolite. However, the proton-form zeolite was stable under dry conditions, so it is speculated that the dealumination was induced by the contact of the proton-form zeolite to atmosphere with humidity. The total and Br{\o}nsted acidity decreased with the dealumination, while Lewis acidity increased. On the other hand, rapid heating of the ammonium type zeolite caused narrowing of the micropores. These structural changes seriously affected the catalytic activities for various reactions.",
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    T2 - Ion exchange of mordenite type zeolite, Remarkable dealumination accompanying ion exchange

    AU - Katada, Naonobu

    AU - Takeguchi, Tatsuya

    AU - Suzuki, Tatsuya

    AU - Fukushima, Toshihisa

    AU - Inagaki, Kinya

    AU - Tokunaga, Setsuo

    AU - Shimada, Hiromichi

    AU - Sato, Koichi

    AU - Oumi, Yasunori

    AU - Sano, Tsuneji

    AU - Segawa, Kohichi

    AU - Nakai, Kazuyuki

    AU - Shoji, Hiroshi

    AU - Wu, Peng

    AU - Tatsumi, Takashi

    AU - Komatsu, Takayuki

    AU - Masuda, Takao

    AU - Domen, Kazunari

    AU - Yoda, Eisuke

    AU - Kondo, Junko N.

    AU - Okuhara, Toshio

    AU - Kageyama, Yasuyoshi

    AU - Niwa, Miki

    AU - Ogura, Masaru

    AU - Matsukata, Masahiko

    AU - Kikuchi, Eiichi

    AU - Okazaki, Noriyasu

    AU - Takahashi, Motoi

    AU - Tada, Akio

    AU - Tawada, Shogo

    AU - Kubota, Yoshihiro

    AU - Sugi, Yoshihiro

    AU - Higashio, Yasuhiko

    AU - Kamada, Masahiko

    AU - Kioka, Yukiyo

    AU - Yamamoto, Kohei

    AU - Shouji, Takayuki

    AU - Arima, Yusaku

    AU - Okamoto, Yasuaki

    AU - Matsumoto, Hideyuki

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    AB - A joint study was organized to establish a standard set of conditions for the ion exchange of zeolite from sodium into proton-form. The sodium-form mordenite with Si/Al2 = ca. 15 was ion exchanged into an NH4-form, followed by calcination according to various recipes. Then various advanced techniques for characterization (ICP, TG, XPS, SEM, XRD, N2 adsorption, 29Si and 27AlNMR, benzene diffusion, IR of OH and adsorbed pyridine and CO, ammonia TPD) were applied, and some test reactions (cracking of cumene, isopropylation of biphenyl, oligomerization of propene and chichibabin condensation of acetaldehyde and ammonia into picoline) were conducted. The ion exchange (removal of sodium) proceeded as expected, but remarkable differences were observed in physicochemical and catalytic properties of the thus-prepared proton-form samples. Exceptionally high temperature (383 K) for the ion exchange resulted in the structural degradation, while most samples exchanged at 333-353 K maintained the crystallinity and pore volume. The use of NH4Cl slightly changed the crystal morphology. Extra-framework aluminum species was formed on most samples after calcination above 773 K. In contrast, calcination at 673 K maintained the framework aluminum. Therefore, the dealumination is considered to proceed after complete removal of ammonia from the ammonium-form zeolite. However, the proton-form zeolite was stable under dry conditions, so it is speculated that the dealumination was induced by the contact of the proton-form zeolite to atmosphere with humidity. The total and Brønsted acidity decreased with the dealumination, while Lewis acidity increased. On the other hand, rapid heating of the ammonium type zeolite caused narrowing of the micropores. These structural changes seriously affected the catalytic activities for various reactions.

    KW - Acidity

    KW - Catalyst preparation

    KW - Dealumination

    KW - Ion exchange

    KW - Mordenite

    KW - Reference catalyst

    KW - Standardization

    KW - Zeolite

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