Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 28, Pages 8827-8832Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b04669
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Funding
- MINECO (Spain) [CTQ2016-75671-P, CTQ2014-56312-P, CTQ2014-55178-R]
- MINECO (Spain) Excellence Unit Severo Ochoa [SEV-2016-0683, MDM-2015-0538]
- MINECO (Spain) Excellence Unit Maria de Maeztu [SEV-2016-0683, MDM-2015-0538]
- Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy)
- mineco
- fBBVA
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The search for simple, earth-abundant, cheap, and nontoxic metal catalysts able to perform industrial hydrogenations is a topic of interest, transversal to many catalytic processes. Here, we show that isolated Fe-III-O sites on solids are able to dissociate and chemoselectively transfer H-2 to acetylene in an industrial process. For that, a novel, robust, and highly crystalline metal-organic framework (MOF), embedding Fe-III-OH2 single sites within its pores, was prepared in multigram scale and used as an efficient catalyst for the hydrogenation of 1% acetylene in ethylene streams under front-end conditions. Cutting-edge X-ray crystallography allowed the resolution of the crystal structure and snapshotted the single-atom nature of the catalytic Fe-III-O site. Translation of the active site concept to even more robust and inexpensive titania and zirconia supports enabled the industrially relevant hydrogenation of acetylene with similar activity to the Pd-catalyzed process.
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