2024-03-28T14:44:55Zhttp://digital.csic.es/dspace-oai/requestoai:digital.csic.es:10261/1906292020-01-28T13:33:00Zcom_10261_101com_10261_5col_10261_354
Immobilizing Systems Biocatalysis for the Selective Oxidation of Glycerol Coupled to InSitu Cofactor Recycling and Hydrogen Peroxide Elimination
Rocha-Martín, Javier
Acosta, Andreina
Guisán, José Manuel
López Gallego, Fernando
Ministerio de Economía y Competitividad (España)
European Cooperation in Science and Technology
Ikerbasque Basque Foundation for Science
Comunidad de Madrid
Biotransformations
Cofactors
Enzyme catalysis
Immobilization
Protein engineering
The combination of three different enzymes immobilized rationally on the same heterofunctional carrier allowed the selective oxidation of glycerol to 1,3‐dihydroxyacetone (DHA) coupled to in situ redox‐cofactor recycling and H2O2 elimination. In this cascade, engineered glycerol dehydrogenase with reduced product inhibition oxidized glycerol selectively to DHA with the concomitant reduction of NAD+ to NADH. NADH oxidase regenerated the NAD+ pool by oxidizing NADH to NAD+ to form H2O2 as the byproduct. Finally, catalase eliminated H2O2 to yield water and O2 as innocuous products, which avoided the spontaneous DHA oxidation triggered by H2O2. The co‐immobilization of the three enzymes on the same porous carrier allowed the in situ recycling and disproportionation of the redox cofactor and H2O2, respectively, to produce up to 9.5 mM DHA, which is 18‐ and 6‐fold higher than glycerol dehydrogenase itself and a soluble multienzyme system, respectively.
This work has been supported by the Spanish Ministry of Economy and Innovation (project CTQ2009‐07568). We acknowledge COST action CM103‐System biocatalysis. We would like to thank IKERBASQUE, Basque foundation for Science for the PhD funding for F.L.‐G. We also thank the Comunidad de Madrid government for funding the PhD fellowship for J.R.‐M.
Peer Reviewed
2019-09-13T06:52:12Z
2019-09-13T06:52:12Z
2015-07-03
2019-09-13T06:52:12Z
artículo
http://purl.org/coar/resource_type/c_6501
ChemCatChem 7(13): 1939-1947 (2015)
1867-3880
http://hdl.handle.net/10261/190629
10.1002/cctc.201500210
1867-3899
http://dx.doi.org/10.13039/100012818
http://dx.doi.org/10.13039/501100003989
http://dx.doi.org/10.13039/501100000921
http://dx.doi.org/10.13039/501100003329
https://doi.org/10.1002/cctc.201500210
Sí
none
Wiley-VCH