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An Exceptionally Stable Metal–Organic Framework Supported Molybdenum(VI) Oxide Catalyst for Cyclohexene Epoxidation
Abstract
Molybdenum(VI) oxide was deposited on the Zr 6 node of the mesoporous metal–organic framework NU-1000 via condensed-phase deposition where the MOF is simply submerged in the precursor solution, a process named solvothermal deposition in MOFs (SIM). Exposure to oxygen leads to a monodisperse, porous heterogeneous catalyst, named Mo-SIM, and its structure on the node was elucidated both computationally and spectroscopically. The catalytic activity of Mo-SIM was tested for the epoxidation of cyclohexene. Near-quantitative yields of cyclohexene oxide and the ring-opened 1,2-cyclohexanediol were observed, indicating activity significantly higher than that of molybdenum(VI) oxide powder and comparable to that of a zirconia-supported analogue (Mo-ZrO 2 ) prepared in a similar fashion. Despite the well-known leaching problem of supported molybdenum catalysts (i.e., loss of Mo species thus causes deactivation), Mo-SIM demonstrated no loss in the metal loading before and after catalysis, and no molybdenum was detected in the reaction mixture. In contrast, Mo-ZrO 2 led to significant leaching and close to 80 wt % loss of the active species. The stability of Mo-SIM was further confirmed computationally, with density functional theory calculations indicating that the dissociation of the molybdenum(VI) species from the node of NU-1000 is endergonic, corroborating the experimental data for the Mo-SIM material.
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Stable Metal–Organic Frameworks with Group 4 Metals: Current Status and Trends
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Optimized Separation of Acetylene from Carbon Dioxide and Ethylene in a Microporous Material
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Metadata
- Authors
- Noh, H., Cui, Y., Peters, A. W., Pahls, D. R., Ortuño, M. A., Vermeulen, N. A., Cramer, C. J., Gagliardi, L., Hupp, J. T., & Farha, O. K.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-10-25
- Volume
- 138
- Issue
- 44
- Pages
- 14720-14726
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2531995234
- Cited by
- 256
- References
- 46
- FWCI
- 14.43
- Type
- journal article
- Language
- en
- Open access
- closed
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- Noh, H., Cui, Y., Peters, A. W., Pahls, D. R., Ortuño, M. A., Vermeulen, N. A., Cramer, C. J., Gagliardi, L., Hupp, J. T., & Farha, O. K. (2016). An Exceptionally Stable Metal–Organic Framework Supported Molybdenum(VI) Oxide Catalyst for Cyclohexene Epoxidation. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.6b08898
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