Optimized oxidoreductases for medium and large scale industrial biotransformations
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Project Secretariat
Dr Marta Pérez-Boada
E-mail: MPBoada@cib.csic.es
Consejo Superior de Investigaciones Científicas (CSIC)
Biological Research Centre (CIB)
Calle Ramiro de Maeztu 9, E-28040 Madrid, Spain
Phone: 34 918373112
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publications
Total records: 126
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[ 2017 ] Rencoret J, Pereira A, del Río JC, Martínez AT, Gutiérrez A Delignification and Saccharification Enhancement of Sugarcane Byproducts by a Laccase-Based Pretreatment Sustainable Chem. Eng., 5: 7145-7154
[ 2017 ] Rodríguez-Escribano D, de Salas F, Pardo I, Camarero S High-Throughput Screening Assay for Laccase Engineering toward Lignosulfonate Valorization Int. J. Mol. Sci., 18: 1793-1803
[ 2016 ] Acebes S, Fernandez-Fueyo E, Monza E, Lucas F, Almendral D, Ruiz-Dueñas FJ, Lund H, Martínez AT, Guallar V Rational Enzyme Engineering Through Biophysical and Biochemical Modeling ACS-Catalysis, 6: 1624-1629
[ 2016 ] Couturier M, Mathieu Y, Li A, Navarro D, Drula E, Haon M, Grisel S, Ludwig R, Berrin JG Characterization of a new aryl-alcohol oxidase secreted by the phytopathogenic fungus Ustilago maydis Appl. Microbiol. Biotechnol., 100: 697-706
[ 2016 ] de Salas F, Pardo I, Salavagione HJ, Aza P, Amourgi E, Vind J, Martínez AT, Camarero S Advanced Synthesis of Conductive Polyaniline Using Laccase as Biocatalyst PlosOne, 11
[ 2016 ] del Río JC, Prinsen P, Cadena EM, Martínez AT, Gutiérrez A, Rencoret J Lignin–carbohydrate complexes from sisal (Agave sisalana) and abaca (Musa textilis): chemical composition and structural modifications during the isolation process Planta, 243: 1143-1158
year2016
Asymmetric sulfoxidation by engineering the heme pocket of a dye-decolorizing peroxidase: An experimental and computational study
Linde D, Cañellas M, Coscolín C, Davó-Siguero I, Romero A, Lucas F, Ruiz-Dueñas FJ, Guallar V, Martínez AT
Catal. Sci. Technol., 6: 6277-6285

The so-called dye-decolorizing peroxidases (DyPs) constitute a new family of proteins exhibiting remarkable stability. With the aim of providing them new catalytic activities of biotechnological interest, the heme pocket of one of the few DyPs fully characterized to date (from the fungus Auricularia auricula-judae) was redesigned based on the crystal structure available, and its potential for asymmetric sulfoxidation was evaluated. Chiral sulfoxides are important targets in organic synthesis and enzyme catalysis, due to a variety of applications. Interestingly, one of the DyP variants, F359G, is highly stereoselective sulfoxidizing methyl-phenyl sulfide and methyl-p-tolyl sulfide (95-99% conversion, with up to 99% excess of the S enantiomer in short reaction times) while the parent DyP has no sulfoxidation activity, and the L357G variant produces both the R and S enantiomers. The two variants were crystallized and their crystal structures were used in molecular simulations to provide a rational explanation for the new catalytic activities. Protein energy landscape exploration (PELE) showed more favorable protein-substrate catalytic complexes for the above variants, with a considerable number of structures near the oxygen atom of the activated heme, which incorporates to the substrates as shown in 18O-labeling experiments, and improved affinity with respect to the parent enzyme, explaining their sulfoxidation activity. Additional quantum mechanics/molecular mechanics (QM/MM) calculations were performed to elucidate the high stereoselectivity observed for the F359G variant, which correlated with higher reactivity on the substrate molecules adopting pro-S poses at the active site. Similar computational analyses can help to introduce/improve (stereoselective) sulfoxidation activity in related hemeproteins.

Official webpage of indox [ industrialoxidoreductases ]. Optimized oxidoreductases for medium and large scale industrial biotransformations. This project has received funding from the European Union’s Seventh Framework Programme for research, technological development and demonstration under Grant Agreement nº: FP7-KBBE-2013-7-613549. © indox 2013. Developed by garcíarincón