Atomic Layer Deposition in a Metal-Organic Framework: Synthesis, Characterization, and Performance of a Solid Acid

Martino Rimoldi, Varinia Bernales, Joshua Borycz, Aleksei Vjunov, Leighanne C. Gallington, Ana E. Platero-Prats, I. S. Kim, John L. Fulton, A. B F Martinson, Johannes A. Lercher, Karena W. Chapman, Christopher J. Cramer, Laura Gagli, Joseph T Hupp, Omar K. Farha

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25 Citations (Scopus)

Abstract

NU-1000, a zirconium-based metal-organic framework (MOF) featuring mesoporous channels, has been postsynthetically metalated via atomic layer deposition in a MOF (AIM) employing dimethylaluminum iso-propoxide ([AlMe2OiPr]2, DMAI), a milder precursor than widely used trimethylaluminum (AlMe3, TMA). The aluminum-modified NU-1000 (Al-NU-1000) has been characterized with a comprehensive suite of techniques that points to the formation of aluminum oxide clusters well dispersed through the framework and stabilized by confinement within small pores intrinsic to the NU-1000 structure. Experimental evidence allows for identification of spectroscopic similarities between Al-NU-1000 and γ-Al2O3. Density functional theory modeling provides structures and simulated spectra, the relevance of which can be assessed via comparison to experimental IR and EXAFS data. The catalytic performance of Al-NU-1000 has been benchmarked against γ-Al2O3, with promising results in terms of selectivity.

Original languageEnglish
Pages (from-to)1058-1068
Number of pages11
JournalChemistry of Materials
Volume29
Issue number3
DOIs
Publication statusPublished - Feb 14 2017

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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    Rimoldi, M., Bernales, V., Borycz, J., Vjunov, A., Gallington, L. C., Platero-Prats, A. E., Kim, I. S., Fulton, J. L., Martinson, A. B. F., Lercher, J. A., Chapman, K. W., Cramer, C. J., Gagli, L., Hupp, J. T., & Farha, O. K. (2017). Atomic Layer Deposition in a Metal-Organic Framework: Synthesis, Characterization, and Performance of a Solid Acid. Chemistry of Materials, 29(3), 1058-1068. https://doi.org/10.1021/acs.chemmater.6b03880