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Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites.


ABSTRACT: Isomerization of sugars is used in a variety of industrially relevant processes and in glycolysis. Here, we show that hydrophobic zeolite beta with framework tin or titanium Lewis acid centers isomerizes sugars, e.g., glucose, via reaction pathways that are analogous to those of metalloenzymes. Specifically, experimental and theoretical investigations reveal that glucose partitions into the zeolite in the pyranose form, ring opens to the acyclic form in the presence of the Lewis acid center, isomerizes into the acyclic form of fructose, and finally ring closes to yield the furanose product. The zeolite catalysts provide processing advantages over metalloenzymes such as an ability to work at higher temperatures and in acidic conditions that allow for the isomerization reaction to be coupled with other important conversions.

SUBMITTER: Bermejo-Deval R 

PROVIDER: S-EPMC3382492 | biostudies-literature | 2012 Jun

REPOSITORIES: biostudies-literature

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Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites.

Bermejo-Deval Ricardo R   Assary Rajeev S RS   Nikolla Eranda E   Moliner Manuel M   Román-Leshkov Yuriy Y   Hwang Son-Jong SJ   Palsdottir Arna A   Silverman Dorothy D   Lobo Raul F RF   Curtiss Larry A LA   Davis Mark E ME  

Proceedings of the National Academy of Sciences of the United States of America 20120604 25


Isomerization of sugars is used in a variety of industrially relevant processes and in glycolysis. Here, we show that hydrophobic zeolite beta with framework tin or titanium Lewis acid centers isomerizes sugars, e.g., glucose, via reaction pathways that are analogous to those of metalloenzymes. Specifically, experimental and theoretical investigations reveal that glucose partitions into the zeolite in the pyranose form, ring opens to the acyclic form in the presence of the Lewis acid center, iso  ...[more]

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