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[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., 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 [...]
[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. [...]
[2018] Draft Genome Sequence of the Sordariomycete Lecythophora (Coniochaeta) hoffmannii CBS 245.38
Leonhardt S, Büttner E, Gebauer AM, Hofrichter M, Kellner H
Genome Announc., 6
Lecythophora (Coniochaeta) hoffmannii, a soil- and lignocellulose-inhabiting sordariomycete (Ascomycota) that can also live as a facultative tree pathogen causing soft rot, [...]
[2018] Side chain removal from corticosteroids by unspecific peroxygenase
Ullrich R, Poraj-Kobielska M, Scholze S, Halbout C, Sandvoss M, Pecyna MJ, Scheibner K, Hofrichter M
J. Inorg. Biochem., 183: 84-93
Two unspecific peroxygenases (UPO, EC 1.11.2.1) from the basidiomycetous fungi Marasmius rotula and Marasmius wettsteinii oxidized steroids with hydroxyacetyl and hydroxyl [...]
[2018] Nonconventional regeneration of redox enzymes – a practical approach for organic synthesis?
Zhang W, Hollmann F
Chem. Commun., 54: 7281-7289
Oxidoreductases have become useful tools in the hands of chemists to perform selective and mild oxidation and reduction reactions. Instead of mimicking native catalytic cycles, [...]
[2018] Selective Synthesis of the Human Drug Metabolite 5′-Hydroxypropranolol by an Evolved Self-Sufficient Peroxygenase
Gómez de Santos P, Cañellas M, Tieves F, Younes SHH, Molina-Espeja P, Hofrichter M, Hollmann F, Guallar V, Alcalde M
ACS-Catalysis, 8: 4789-4799
Propranolol is a widely used beta-blocker that is metabolized by human liver P450 monooxygenases into equipotent hydroxylated human drug metabolites (HDMs). It is paramount [...]
[2018] Biological Lignin Degradation
Martínez AT, Camarero S, Ruiz-Dueñas FJ, Martínez MJ
Lignin Valorization: Emerging Approaches. Ed. Gregg Beckham. RSC: 199-225
In nature, white-rot fungi and some bacteria secrete powerful oxidative enzymes such as peroxidases and laccases to break down lignin and lignin products. These enzymes, together [...]
[2018] Selective synthesis of the resveratrol analogue 4,4′-dihydroxy-trans-stilbene and stilbenoids modification by fungal peroxygenases
Aranda C, Ullrich R, Kiebist J, Scheibner K, del Río JC, Hofrichter M, Martínez AT, Gutiérrez A
Catal. Sci. Technol., 8: 2394-2401
This work gives first evidence that the unspecific peroxygenases (UPOs) from the basidiomycetes Agrocybe aegerita (AaeUPO), Coprinopsis cinerea (rCciUPO) and Marasmius rotula [...]
[2018] Self-sustained enzymatic cascade for the production of 2,5-furandicarboxylic acid from 5-methoxymethylfurfural
Carro J, Fernandez-Fueyo E, Fernández-Alonso C, Cañada J, Ullrich R, Hofrichter M, Alcalde M, Ferreira P, Martínez AT
Biotechnol. Biofuels, 11: 86-96
Background 2,5-Furandicarboxylic acid is a renewable building block for the production of polyfurandicarboxylates, which are biodegradable polyesters expected to substitute [...]
[2018] Stepwise Hydrogen Atom and Proton Transfers in Dioxygen Reduction by Aryl-Alcohol Oxidase
Carro J, Ferreira P, Martínez AT, Gadda G
Biochemistry, 57: 1790-1797
The mechanism of dioxygen reduction by the flavoenzyme aryl-alcohol oxidase was investigated with kinetic isotope, viscosity, and pL (pH/pD) effects in rapid kinetics experiments [...]
[2018] Enzymatic Preparation of 2,5-Furandicarboxylic Acid (FDCA)—A Substitute of Terephthalic Acid—By the Joined Action of Three Fungal Enzymes
Karich A, Kleeberg SB, Ullrich R, Hofrichter M
Microorganisms, 6: 5
Enzymatic oxidation of 5-hydroxymethylfurfural (HMF) and its oxidized derivatives was studied using three fungal enzymes: wild-type aryl alcohol oxidase (AAO) from three fungal [...]
[2017] Fatty Acid Chain Shortening by a Fungal Peroxygenase
Olmedo A, del Río JC, Kiebist J, Ullrich R, Hofrichter M, Scheibner K, Martínez AT, Gutiérrez A
Chem. Eur. J., 23: 16985-16989
A recently discovered peroxygenase from the fungus Marasmius rotula (MroUPO) is able to catalyze the progressive one-carbon shortening of medium and long-chain mono- and dicarboxylic [...]
[2017] Draft Genome Sequence of the Wood-Degrading Ascomycete Kretzschmaria deusta DSM 104547
Büttner E, Gebauer AM, Hofrichter M, Liers C, Kellner H
Genome Announc., 5
We report here the draft genome of Kretzschmaria (Ustulina) deusta, an ascomycetous fungus that colonizes and substantially degrades hardwood and can infest living broad-leaved [...]
[2017] Mapping the Long-Range Electron Transfer Route in Ligninolytic Peroxidases
Acebes S, Ruiz-Dueñas FJ, Toubes M, Saez-Jimenez V, Pérez-Boada M, Lucas F, Martínez AT, Guallar V
J. Phys. Chem. B, 121: 3946-3954
Combining a computational analysis with site-directed mutagenesis, we have studied the long-range electron transfer pathway in versatile and lignin peroxidases, two enzymes [...]
[2017] Protein dynamics promote hydride tunnelling in substrate oxidation by aryl-alcohol oxidase
Carro J, Martínez A, Medina M, Martínez AT, Ferreira P
Phys. Chem. Chem. Phys., 18: 28666-28675
The temperature dependence of hydride transfer from the substrate to the N5 of the FAD cofactor during the reductive half-reaction of Pleurotus eryngii aryl-alcohol oxidase [...]
[2017] Selective activation of C-H bonds by cascading photochemistry with biocatalysis
Zhang W, Burek BO, Fernandez-Fueyo E, Alcalde M, Bloh JZ, Hollmann F
Angew. Chem. Int. Ed., 56: 15451-15455
Selective oxyfunctionalisation of inert C-H bonds under mild conditions can be achieved using peroxygenases. This approach, however, is impaired by the [...]