Journal
ACS CATALYSIS
Volume 6, Issue 1, Pages 55-59Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b02061
Keywords
metal-organic frameworks; catalysis; C-O bond cleavage; hydrogenolysis; aromatic ethers
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Funding
- Sandia Laboratory Directed Research and Development Program
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- DOE Joint BioEnergy Institute - U. S. Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-05CH11231]
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We demonstrate that metal organic frameworks (MOFs) can catalyze hydrogenolysis of aryl ether bonds under mild conditions. Mg-IRMOF-74(I) and Mg-IRMOF-74(II) are stable under reducing conditions and can cleave phenyl ethers containing beta-O-4, alpha-O-4, and 4-O-5 linkages to the corresponding hydrocarbons and phenols. Reaction occurs at 10 bar H-2 and 120 degrees C without added base. DFT-optimized structures and charge transfer analysis suggest that the MOF orients the substrate near Mg2+ ions on the pore walls. Ti and Ni doping further increase conversions to as high as 82% with 96% selectivity for hydrogenolysis versus ring hydrogenation. Repeated cycling induces no loss of activity, making this a promising route for mild aryl-ether bond scission.
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