Intermediates of thiamine catalysis immobilized on silica surface as active biocatalysts for alpha-ketoacid decarboxylation
| dc.contributor.author | Stamatis, A. | en |
| dc.contributor.author | Malandrinos, G. | en |
| dc.contributor.author | Butler, I. S. | en |
| dc.contributor.author | Hadjiliadis, N. | en |
| dc.contributor.author | Louloudi, M. | en |
| dc.date.accessioned | 2015-11-24T16:40:23Z | |
| dc.date.available | 2015-11-24T16:40:23Z | |
| dc.identifier.issn | 1381-1169 | - |
| dc.identifier.uri | https://olympias.lib.uoi.gr/jspui/handle/123456789/8270 | |
| dc.rights | Default Licence | - |
| dc.subject | thiamine catalysis | en |
| dc.subject | decarboxylation | en |
| dc.subject | immobilised biocatalysts | en |
| dc.subject | modified silica | en |
| dc.subject | 2-hydroxy-ketones | en |
| dc.subject | diphosphate-dependent enzymes | en |
| dc.subject | sol-gel materials | en |
| dc.subject | benzoylformate decarboxylase | en |
| dc.subject | crystal-structure | en |
| dc.subject | metal-complexes | en |
| dc.subject | pyrophosphate | en |
| dc.subject | mechanism | en |
| dc.subject | models | en |
| dc.subject | cadmium(ii) | en |
| dc.subject | resolution | en |
| dc.title | Intermediates of thiamine catalysis immobilized on silica surface as active biocatalysts for alpha-ketoacid decarboxylation | en |
| heal.abstract | Thiamine-dependent enzymes catalyse the decarboxylation of alpha-ketoacids, by both non-oxidative and oxidative mechanisms. Based on the ability of thiamine-cofactor to catalyse itself the decarboxylation of pyruvate to some extent, we have immobilized on a silica surface two 'active aldehyde' intermediates of thiamine catalysis, 2-alpha-hydroxybenzyl-thiamine pyrophosphate (HBTPP) and 2-alpha-hydroxyethyl-thiamine pyrophosphate (HETPP). The two intermediates have been tethered by a convenient method on silica support via their phosphate groups providing the covalently heterogenised biomolecules [HBTh-OP2O6-SiO3/2](n)center dot xSiO(2), and [HETh-OP2O6-SiO3/2](n)center dot xSiO(2). These bio-composite materials have been evaluated as catalysts for pyruvate and benzoyl-formate decarboxylation in either the presence or not of an aldehyde additive. Our data show that they are stable, very effective and recyclable catalysts for the production of 2-hydroxy-ketones, acetoine and benzoin. Their catalytic behavior is much better than the corresponding behavior of the homogeneous thiamine-systems due to the selected immobilization mode which bears similarities to that of the thiamine-cofactor binding to the protein. Considering our results, possible catalytic pathways of the prepared bio-composite materials are suggested. (C) 2006 Elsevier B.V. All rights reserved. | en |
| heal.access | campus | - |
| heal.fullTextAvailability | TRUE | - |
| heal.identifier.primary | DOI 10.1016/j.molcata.2006.11.049 | - |
| heal.identifier.secondary | <Go to ISI>://000245880900017 | - |
| heal.identifier.secondary | http://ac.els-cdn.com/S1381116906014075/1-s2.0-S1381116906014075-main.pdf?_tid=7c1b87479e8b7a862c552f056d00b985&acdnat=1333034662_fa5d43f85f387379c81307d9bc4dc3e0 | - |
| heal.journalName | Journal of Molecular Catalysis a-Chemical | en |
| heal.journalType | peer reviewed | - |
| heal.language | en | - |
| heal.publicationDate | 2007 | - |
| heal.publisher | Elsevier | en |
| heal.recordProvider | Πανεπιστήμιο Ιωαννίνων. Σχολή Θετικών Επιστημών. Τμήμα Χημείας | el |
| heal.type | journalArticle | - |
| heal.type.el | Άρθρο Περιοδικού | el |
| heal.type.en | Journal article | en |
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