The DOI matches its Crossref record; 43 of the 43 references it cites were found in a registry or an index.
Methane to Methanol: Structure–Activity Relationships for Cu-CHA
Open accessAbstract
Cu-exchanged zeolites possess active sites that are able to cleave the C–H bond of methane at temperatures ≤200 °C, enabling its selective partial oxidation to methanol. Herein we explore this process over Cu-SSZ-13 materials. We combine activity tests and X-ray absorption spectroscopy (XAS) to thoroughly investigate the influence of reaction parameters and material elemental composition on the productivity and Cu speciation during the key process steps. We find that the Cu II moieties responsible for the conversion are formed in the presence of O 2 and that high temperature together with prolonged activation time increases the population of such active sites. We evidence a linear correlation between the reducibility of the materials and their methanol productivity. By optimizing the process conditions and material composition, we are able to reach a methanol productivity as high as 0.2 mol CH 3 OH/mol Cu (125 μmol/g), the highest value reported to date for Cu-SSZ-13. Our results clearly demonstrate that high populations of 2Al Z 2 Cu II sites in 6r, favored at low values of both Si:Al and Cu:Al ratios, inhibit the material performance by being inactive for the conversion. Z[Cu II OH] complexes, although shown to be inactive, are identified as the precursors to the methane-converting active sites. By critical examination of the reported catalytic and spectroscopic evidence, we propose different possible routes for active-site formation.
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Small-Pore Zeolites: Synthesis and Catalysis
Dusselier, M., & Davis, M. E. (2018) · Chemical Reviews · doi:10.1021/acs.chemrev.7b00738 · Cited by 831
Bioinspired Metal–Organic Framework Catalysts for Selective Methane Oxidation to Methanol
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Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities
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Fast room temperature lability of aluminosilicate zeolites
Heard, C. J., Grajciar, L., Rice, C. M., Pugh, S. M., Nachtigall, P., Ashbrook, S. E., & Morris, R. E. (2019) · Nature Communications · doi:10.1038/s41467-019-12752-y · Cited by 121
Metadata
- Authors
- Pappas, D. K., Borfecchia, E., Dyballa, M., Pankin, I. A., Lomachenko, K. A., Martini, A., Signorile, M., Teketel, S., Arstad, B., Berlier, G., Lamberti, C., Bordiga, S., Olsbye, U., Lillerud, K. P., Svelle, S., & Beato, P.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-10-17
- Volume
- 139
- Issue
- 42
- Pages
- 14961-14975
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2756602711
- Cited by
- 371
- References
- 43
- FWCI
- 13.70
- Type
- journal article
- Language
- en
- Open access
- green
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- Pappas, D. K., Borfecchia, E., Dyballa, M., Pankin, I. A., Lomachenko, K. A., Martini, A., Signorile, M., Teketel, S., Arstad, B., Berlier, G., Lamberti, C., Bordiga, S., Olsbye, U., Lillerud, K. P., Svelle, S., & Beato, P. (2017). Methane to Methanol: Structure–Activity Relationships for Cu-CHA. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.7b06472
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