Toward understanding the catalytic synergy in the design of bimetallic molecular sieves for selective aerobic oxidations

Structure-property correlations and mechanistic implications are important in the design of single-site catalysts for the activation of molecular oxygen. In this study we rationalize trends in catalytic synergy to elucidate the nature of the active site through structural and spectroscopic correlati...

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Main Authors: Leithall, Rebecca M. (Author), Shetti, Vasudev N. (Author), Maurelli, Sara (Author), Chiesa, Mario (Author), Gianotti, Enrica (Author), Raja, Robert (Author)
Format: Article
Language:English
Published: 2013-02-27.
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Online Access:Get fulltext
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100 1 0 |a Leithall, Rebecca M.  |e author 
700 1 0 |a Shetti, Vasudev N.  |e author 
700 1 0 |a Maurelli, Sara  |e author 
700 1 0 |a Chiesa, Mario  |e author 
700 1 0 |a Gianotti, Enrica  |e author 
700 1 0 |a Raja, Robert  |e author 
245 0 0 |a Toward understanding the catalytic synergy in the design of bimetallic molecular sieves for selective aerobic oxidations 
260 |c 2013-02-27. 
856 |z Get fulltext  |u https://eprints.soton.ac.uk/348354/1/ja3119064 
520 |a Structure-property correlations and mechanistic implications are important in the design of single-site catalysts for the activation of molecular oxygen. In this study we rationalize trends in catalytic synergy to elucidate the nature of the active site through structural and spectroscopic correlations. In particular, the redox behavior and coordination geometry in isomorphously substituted, bimetallic VTiAlPO-5 catalysts are investigated with a view to specifically engineering and enhancing their reactivity and selectivity in aerobic oxidations. By using a combination of HYSCORE EPR and in situ FTIR studies, we show that the well-defined and isolated oxophilic tetrahedral titanium centers coupled with redox-active VO2+ ions at proximal framework positions provide the loci for the activation of oxidant that leads to a concomitant increase in catalytic activity compared to analogous monometallic systems. 
655 7 |a Article