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The acidic nature of “NMR-invisible” tri-coordinated framework aluminum species in zeolites

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Abstract

The unambiguous characterization of different acid sites in zeolites is of great importance for understanding their catalytic performance and the rational design of highly efficient zeolite catalysts. In addition to various well-characterized extra-framework Al species, a tri-coordinated framework aluminum species can also serve as a Lewis acid site in zeolites, which is “NMR-invisible” owing to its extremely distorted local environment. Here we provide a feasible and reliable approach to elucidate the acidic nature of the tri-coordinated framework Al in dehydrated H-ZSM-5 zeolites via sensitivity-enhanced two-dimensional (2D) multiple nuclear correlation NMR experiments coupled with trimethylphosphine oxide (TMPO) probe molecules. Two types of tri-coordinated framework Al sites have been unambiguously identified, which amount to 11.6% of the total Brønsted and Lewis acid sites. Furthermore, it was found that synergistic effects arising from the close spatial proximity between the tri-coordinated framework Al site and the Brønsted acid site lead to the generation of superacidity (with an acid strength stronger than 100% H2SO4) in the zeolite.

Graphical abstract: The acidic nature of “NMR-invisible” tri-coordinated framework aluminum species in zeolites

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Publication details

The article was received on 30 May 2019, accepted on 11 Sep 2019 and first published on 12 Sep 2019


Article type: Edge Article
DOI: 10.1039/C9SC02634G
Chem. Sci., 2019, Advance Article
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    The acidic nature of “NMR-invisible” tri-coordinated framework aluminum species in zeolites

    S. Xin, Q. Wang, J. Xu, Y. Chu, P. Wang, N. Feng, G. Qi, J. Trébosc, O. Lafon, W. Fan and F. Deng, Chem. Sci., 2019, Advance Article , DOI: 10.1039/C9SC02634G

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