Enzyme-modified particles for selective biocatalytic hydrogenation by hydrogen-driven NADH recycling
| dc.contributor.author | Reeve, Holly A. | |
| dc.contributor.author | Lauterbach, Lars | |
| dc.contributor.author | Lenz, Oliver | |
| dc.contributor.author | Vincent, Kylie A. | |
| dc.date.accessioned | 2017-07-14T10:50:11Z | |
| dc.date.available | 2017-07-14T10:50:11Z | |
| dc.date.issued | 2015 | |
| dc.description.abstract | We describe a new approach to selective H-2-driven hydrogenation that exploits a sequence of enzymes immobilised on carbon particles. We used a catalyst system that comprised alcohol dehydrogenase, hydrogenase and an NAD(+) reductase on carbon black to demonstrate a greater than 98% conversion of acetophenone to phenylethanol. Oxidation of H-2 by the hydrogenase provides electrons through the carbon for NAD(+) reduction to recycle the NADH cofactor required by the alcohol dehydrogenase. This biocatalytic system operates over the pH range 6-8 or in un-buffered water, and can function at low concentrations of the cofactor (10m NAD(+)) and at H-2 partial pressures below 1bar. Total turnover numbers >130000 during acetophenone reduction indicate high enzyme stability, and the immobilised enzymes can be recovered by a simple centrifugation step and re-used several times. This offers a route to convenient, atom-efficient operation of NADH-dependent oxidoreductases for selective hydrogenation catalysis. | en |
| dc.description.sponsorship | EC/FP7/258600/EU/Understanding and Exploiting Biological Catalysts for Energy Cycling: Development of Infrared Spectroelectrochemistry for Studying Intermediates in Metalloenzyme Catalysis/EnergyBioCatalysis | en |
| dc.description.sponsorship | EC/FP7/297503/EU/Modular beads for regeneration of bio-cofactors in enzyme-catalysed synthesis/HydRegen | en |
| dc.description.sponsorship | DFG, EXC 314, Unifying Concepts in Catalysis | en |
| dc.identifier.eissn | 1867-3899 | |
| dc.identifier.issn | 1867-3880 | |
| dc.identifier.uri | https://depositonce.tu-berlin.de/handle/11303/6492 | |
| dc.identifier.uri | http://dx.doi.org/10.14279/depositonce-6000 | |
| dc.language.iso | en | |
| dc.rights.uri | https://creativecommons.org/licenses/by-nc/4.0/ | |
| dc.subject.ddc | 540 Chemie und zugeordnete Wissenschaften | de |
| dc.subject.other | biocatalysis | en |
| dc.subject.other | biotransformations | en |
| dc.subject.other | enzyme catalysis | en |
| dc.subject.other | hydrogenation | en |
| dc.subject.other | heterogeneous catalysis | en |
| dc.title | Enzyme-modified particles for selective biocatalytic hydrogenation by hydrogen-driven NADH recycling | en |
| dc.type | Article | en |
| dc.type.version | publishedVersion | en |
| dcterms.bibliographicCitation.doi | 10.1002/cctc.201500766 | |
| dcterms.bibliographicCitation.issue | 21 | |
| dcterms.bibliographicCitation.journaltitle | ChemCatChem | en |
| dcterms.bibliographicCitation.originalpublishername | Wiley-VCH | en |
| dcterms.bibliographicCitation.originalpublisherplace | Weinheim | en |
| dcterms.bibliographicCitation.pageend | 3487 | |
| dcterms.bibliographicCitation.pagestart | 3480 | |
| dcterms.bibliographicCitation.volume | 7 | |
| tub.accessrights.dnb | free | |
| tub.affiliation | Fak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Physikalische Chemie / Biophysikalische Chemie | de |
| tub.affiliation.faculty | Fak. 2 Mathematik und Naturwissenschaften | de |
| tub.affiliation.group | FG Physikalische Chemie / Biophysikalische Chemie | de |
| tub.affiliation.institute | Inst. Chemie | de |
| tub.publisher.universityorinstitution | Technische Universität Berlin |
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