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Strong and Weakly Acidic OH Groups of HY Zeolite into the Different Routes of Cyclohexene Reaction: An IR Operando Study

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Abstract

IR operando study of cyclohexene reaction on HY zeolite (Si/Al = 15) was performed to determine the role of the OH groups located in the different zeolitic cages and the silanol groups (SiOH). A parallel between the product yield and type and amount of OH groups poisoned by coking and pyridine pulses was established. The role of silanol and zeolitic OH groups during cyclohexene conversion and the coverage rate of surface groups of the dealuminated HY zeolite, were evaluated by FT-IR operando study. At the beginning of the reaction, zeolite exhibited a very intense deactivation due to coke formation. Coke is initially deposited on strong acid sites, inhibiting the H-transfer activity. Further, coke formation decreased. At this stage of the reaction, pyridine addition markedly decreased the isomerization activity. In parallel, it is noted that mainly SiOH, OH groups at hexagonal prisms, and perturbed OH groups in sodalite cages were mainly affected, indicating that these groups are responsible for the isomerization steps. These results showed that even weakly acidic sites are active sites for isomerization reaction.

Graphic Abstract

In cyclohexene conversion, hydrogen transfer occurs on supercage OH groups of HY zeolite. In contrast, perturbed sodalite OH and hexagonal prisms OH, as well as SiOH groups, are responsible for isomerization steps, as revealed by pyridine pulse addition during the reaction.

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Acknowledgments

The authors would like to thank Dr. Philippe Bazin for the support in the pyridine adsorption experiments and operando setup development, as well as Dr. Alexandre Vimont and Yoann Levaque. The authors are also grateful to PETROBRAS and LCS for the financial support and the authorization for using the facilities for carrying out the experiments.

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Authors and Affiliations

  1. Centro de Pesquisas e Desenvolvimento, PETROBRAS, Rio de Janeiro, Brazil

    Bruno M. Santos & José L. Zotin

  2. Normandie Univ, ENSICAEN, UNICAEN, CNRS, LCS, 14000, Caen, France

    Françoise Maugé, Laetitia Oliviero & Weitao Zhao

  3. Escola de Química, Centro de Tecnologia, Universidade Federal Do Rio de Janeiro, Rio de Janeiro, Brazil

    Bruno M. Santos & Mônica A. P. da Silva

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  1. Bruno M. Santos
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Santos, B.M., Zotin, J.L., Maugé, F. et al. Strong and Weakly Acidic OH Groups of HY Zeolite into the Different Routes of Cyclohexene Reaction: An IR Operando Study. Catal Lett 151, 1566–1577 (2021). https://doi.org/10.1007/s10562-020-03424-4

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