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[2021] Comparing Ligninolytic Capabilities of Bacterial and Fungal Dye-Decolorizing Peroxidases and Class-II Peroxidase-Catalases
Linde D, Ayuso-Fernández I, Laloux M, Aguiar-Cervera JE, De Lacey AL, Ruiz-Dueñas FJ, Martínez AT
Int. J. Mol. Sci., 22: 2629
We aim to clarify the ligninolytic capabilities of dye-decolorizing peroxidases (DyPs) from bacteria and fungi, compared to fungal lignin peroxidase (LiP) and versatile peroxidase [...]
[2021] Early-stage sustainability assessment of enzyme production in the framework of lignocellulosic biorefinery
Bello S, Pérez N, Kiebist J, Scheibner K, Sánchez-Ruiz MI, Serrano A, Martínez AT, Feijoó G, Moreira MT
J. Clean. Prod., 285: 125461
The use and integration of enzymatic processes for the biotransformation of biomass within the biorefinery framework creates the need to confirm whether these novel production [...]
[2020] Reaction mechanisms and applications of aryl-alcohol oxidase
Serrano A, Carro J, Martínez AT
The Enzymes, 47: 167-192
Aryl-alcohol oxidases (AAO) constitute a family of FAD-containing enzymes, included in the glucose-methanol-choline oxidase/dehydrogenase superfamily of proteins. They are [...]
[2020] Directed evolution of the aryl-alcohol oxidase: beyond the lab bench
Viña-Gonzalez J, Alcalde M
Comput. Struct. Biotechnol. J ., 18: 1800-1810
Aryl-alcohol oxidase (AAO) is a fungal GMC flavoprotein secreted by white-rot fungi that supplies H2O2 to the ligninolytic consortium. This enzyme can oxidize a wide array [...]
[2020] Screening and Evaluation of New Hydroxymethylfurfural Oxidases for Furandicarboxylic Acid Production
Viñambres M, Espada M, Martínez AT, Serrano A
Appl. Environ. Microbiol., 86: 84220
The enzymatic production of 2,5-furandicarboxylic acid (FDCA) from 5-hydroxy-methylfurfural (HMF) has gained interest in recent years, as the renewable precursor of poly(ethylene-2,5-furandicarboxylate) [...]
[2020] Selective Oxygenation of Ionones and Damascones by Fungal Peroxygenases
Babot ED, Aranda C, del Río JC, Ullrich R, Kiebist J, Scheibner K, Hofrichter M, Martínez AT, Gutiérrez A
J. Agric. Food Chem., 68: 5375-5383
Apocarotenoids are among the most highly valued fragrance constituents, being also appreciated as synthetic building blocks. This work shows the ability of unspecific peroxygenases [...]
[2020] Genome sequencing of Rigidoporus microporus provides insights on genes important for wood decay, latex tolerance and interspecific fungal interactions
Oghenakaro AO, Kovalchuk A, Raffaello T, Camarero S, Gressler M, Henrissat B, Lee J, Liu M, Martínez AT, Miettinen O, Mihaltcheva S, Pangilinan J, Ren F, Riley R, Ruiz-Dueñas FJ, Serrano A, Thon MR, Wen Z, Zhen Z, Barry K, Grigoriev IV, Martin F, Asiegbu FO
Sci. Rep., 10: 5250
Fungal plant pathogens remain a serious threat to the sustainable agriculture and forestry, despite the extensive efforts undertaken to control their spread. White root rot [...]
[2020] Lignin degradation and detoxification of eucalyptus wastes by on-site manufacturing fungal enzymes to enhance second-generation ethanol yield
Schneider WDH, Fontana RC, Baudel HM, Gonçalves de Siqueira F, Rencoret J, Gutiérrez A, de Eugenio LI, Prieto A, Martínez MJ, Martínez AT, Pinheiro Dillon AJ, Camassola M
Applied Energy, 262: 114493
Novel laccases have promising and valuable applications in biorefineries. This investigation documents, for the first time, the potential of depolymerising and repolymerising [...]
[2020] Sequential oxidation of 5-hydroxymethylfurfural to furan-2,5-dicarboxylic acid by an evolved aryl-alcohol oxidase
Viña-Gonzalez J, Martínez AT, Guallar V, Alcalde M
Biochim. Biophys. Acta - Proteins and Proteomics, 1868: 140293
Furan-2,5-dicarboxylic acid (FDCA) is a building block of biodegradable plastics that can be used to replace those derived from fossil carbon sources. In recent years, much [...]
[2020] Towards improving the sustainability of bioplastics: Process modelling and life cycle assessment of two separation routes for 2,5-furandicarboxylic acid
Bello S, Méndez-Trelles P, Rodil E, Feijoó G, Moreira MT
Sep. Purif. Technol., 233: 116056
Within the framework of an economy excessively dependent on fossil resources, the concept of sustainable development, aimed at obtaining environmentally friendly consumer [...]
[2019] Complete oxidation of hydroxymethylfurfural to furandicarboxylic acid by aryl-alcohol oxidase
Serrano A, Calviño E, Carro J, Sánchez-Ruiz MI, Cañada FJ, Martínez AT
Biotechnol. Biofuels, 12: 127, 10.1186/s13068-019-1555-z
Background: 5‑Hydroxymethylfurfural (HMF) is a highly valuable platform chemical that can be obtained from plant biomass carbohydrates. HMF can be oxidized to 2,5‑furandicarboxylic aci [...]
[2019] Peroxidase evolution in white-rot fungi follows wood lignin evolution in plants
Ayuso-Fernández I, Rencoret J, Gutiérrez A, Ruiz-Dueñas FJ, Martínez AT
Proc. Natl. Acad. Sci. USA, 10.1073/pnas.1905040116
A comparison of sequenced Agaricomycotina genomes suggests that efficient degradation of wood lignin was associated with the appearance of secreted peroxidases with a solvent-exposed [...]
[2019] Binding and Catalytic Mechanisms of Veratryl Alcohol Oxidation by Lignin Peroxidase: A Theoretical and Experimental Study
Romero JO, Fernandez-Fueyo E, Avila-Salas F, Recabarren R, Alzate-Morales J, Martínez AT
Comput. Struct. Biotechnol. J ., 17: 1066-1074
Lignin peroxidase (LiP) and its natural substrate veratryl alcohol (VA) play a crucial role in lignin degradation by white-rot fungi. Understanding the molecular determinants [...]
[2019] Formate oxidase (FOx) from Aspergillus oryzae: one catalyst to promote H2O2‐dependent biocatalytic oxidation reactions
Tieves F, Willot SJ-P, van Schie MMCH, Rauch MCR, Younes SHH, Zhang W, Dong J, Gómez de Santos P, Robbins JM, Bommarius B, Alcalde M, Bommarius AS, Hollmann F
Angew. Chem. Int. Ed., 58: 7873-7877, 10.1002/anie.201902380
An increasing number of biocatalytic oxidation reactions rely on H2O2 as clean oxidant. The poor robustness of most enzymes towards H2O2, however, necessitates more efficient [...]
[2019] Structure-Guided Immobilization of an Evolved Unspecific Peroxygenase
Molina-Espeja P, Santos-Moriano P, García-Ruiz E, Ballesteros A, Plou FJ, Alcalde M
Int. J. Mol. Sci., 20: 1627-1639
Unspecific peroxygenases (UPOs) are highly promiscuous biocatalyst with self-sufficient mono(per)oxygenase activity. A laboratory-evolved UPO secreted by yeast was covalently [...]
[2019] Selective synthesis of 4-hydroxyisophorone and 4-ketoisophorone by fungal peroxygenases
Aranda C, Municoy M, Guallar V, Kiebist J, Scheibner K, Ullrich R, del Río JC, Hofrichter M, Martínez AT, Gutiérrez A
Catal. Sci. Technol., 9: 1398-1405
The recently discovered unspecific peroxygenases (UPOs) from the ascomycetes Chaetomium globosum and Humicola insolens were capable of selectively hydroxylating isophorone [...]
[2019] Energising the E-factor: The E+-factor
Tieves F, Tonin F, Fernandez-Fueyo E, Robbins JM, Bommarius B, Bommarius AS, Alcalde M, Hollmann F
Tetrahedron, 75: 1311-1314
The E-factor has become an important measure for the environmental impact of (bio)chemical reactions. However, summing up the obvious wastes generated in the laboratory neglects [...]
[2019] Redox potential increased during the evolution of enzymes degrading recalcitrant lignin
Ayuso-Fernández I, De Lacey AL, Cañada FJ, Ruiz-Dueñas FJ, Martínez AT
Chem. Eur. J., 25: 2708-2712
To investigate how ligninolytic peroxidases acquired the uniquely high redox‐potential they show today, their ancestors were resurrected and characterized. Unfortunately, t [...]
[2018] Structural Insights into the Substrate Promiscuity of a Laboratory-Evolved Peroxygenase
Ramírez-Escudero M, Molina-Espeja P, Gómez de Santos P, Hofrichter M, Sanz-Aparicio J, Alcalde M
ACS Chem. Biol., 13: 3259-3268
Because of their minimal requirements, substrate promiscuity and product selectivity, fungal peroxygenases are now considered to be the jewel in the crown of C–H oxyfunctionalization b [...]
[2019] Environmental sustainability assessment of HMF and FDCA production from lignocellulosic biomass through life cycle assessment (LCA)
Bello S, Salim I, Méndez-Trelles P, Rodil E, Feijoó G, Moreira MT
Holzforschung, 73: 105-115
2,5-Furandicarboxylic acid (FDCA) and 5-hydroxymethylfurfural (HMF) are top biomass-based platform chemicals with promising potential and an essential part of the future of [...]
[2018] Biocatalytic Oxidation Reactions: A Chemist's Perspective
Dong J, Fernandez-Fueyo E, Hollmann F, Paul CE, Pesic M, Schmidt S, Wang Y, Younes S, Zhang W
Angew. Chem. Int. Ed., 57-9238
Oxidation chemistry using enzymes is approaching maturity and practical applicability in organic synthesis. Oxidoreductases (enzymes catalysing redox reactions) enable chemists [...]
[2018] Description of a Non-Canonical Mn(II)-Oxidation Site in Peroxidases
Fernandez-Fueyo E, Davó-Siguero I, Almendral D, Linde D, Baratto MC, Pogni R, Romero A, Guallar V, Martínez AT
ACS-Catalysis, 8: 8386-8395
A dye-decolorizing peroxidase (DyP) from Pleurotus ostreatus (PosDyP4) catalyzes the oxidation of Mn2+ to Mn3+, in the presence of H2O2, with an efficiency similar to the [...]
[2018] Evolutionary convergence in lignin-degrading enzymes
Ayuso-Fernández I, Ruiz-Dueñas FJ, Martínez AT
Proc. Natl. Acad. Sci. USA, 115: 6428-6433
The resurrection of ancestral enzymes of now-extinct organisms (paleogenetics) is a developing field that allows the study of evolutionary hypotheses otherwise impossible [...]
[2018] Multiple implications of an active site phenylalanine in the catalysis of aryl-alcohol oxidase
Carro J, Amengual-Rigo P, Sancho F, Medina M, Guallar V, Ferreira P, Martínez AT
Scientific Reports, 8: 8121
Aryl-alcohol oxidase (AAO) has demonstrated to be an enzyme with a bright future ahead due to its biotechnological potential in deracemisation of chiral compounds, production [...]
[2018] Shuffling the Neutral Drift of Unspecific Peroxygenase in Saccharomyces cerevisiae
Martín-Díaz J, Paret C, García-Ruiz E, Molina-Espeja P, Alcalde M
Appl. Environ. Microbiol., 86: 808-18
Unspecific peroxygenase (UPO) is a highly promiscuous biocatalyst, and its selective mono(per)oxygenase activity makes it useful for many synthetic chemistry applications. [...]