Agaricales mushroom lignin peroxidase: from structure–function to degradative capabilities

Sánchez-Ruiz, María Isabel ; Ayuso Fernández, Iván ; Rencoret, Jorge ; González Ramírez, Andrés Manuel (Universidad de Zaragoza) ; Linde, Dolores ; Davó Siguero, Irene ; Romero, Antonio ; Gutiérrez, Ana ; Martínez, Angel T. ; Ruiz Dueñas, Francisco Javier

Resumen: Lignin biodegradation has been extensively studied in white-rot fungi, which largely belong to order Polyporales. Among the enzymes that wood-rotting polypores secrete, lignin peroxidases (LiPs) have been labeled as the most efficient. Here, we characterize a similar enzyme (ApeLiP) from a fungus of the order Agaricales (with ~13,000 described species), the soil-inhabiting mushroom Agrocybe pediades. X-ray crystallography revealed that ApeLiP is structurally related to Polyporales LiPs, with a conserved heme-pocket and a solvent-exposed tryptophan. Its biochemical characterization shows that ApeLiP can oxidize both phenolic and non-phenolic lignin model-compounds, as well as different dyes. Moreover, using stopped-flow rapid spectrophotometry and 2D-NMR, we demonstrate that ApeLiP can also act on real lignin. Characterization of a variant lacking the above tryptophan residue shows that this is the oxidation site for lignin and other high redox-potential substrates, and also plays a role in phenolic substrate oxidation. The reduction potentials of the catalytic-cycle intermediates were estimated by stopped-flow in equilibrium reactions, showing similar activation by H2O2, but a lower potential for the rate-limiting step (compound-II reduction) compared to other LiPs. Unexpectedly, ApeLiP was stable from acidic to basic pH, a relevant feature for application considering its different optima for oxidation of phenolic and nonphenolic compounds.

Idioma: Inglés

DOI: 10.3390/antiox10091446

Año: 2021

Publicado en: Antioxidants 10, 9 (2021), 1446 [23 pp]
ISSN: 2076-3921

Factor impacto JCR: 7.675 (2021)

Categ. JCR: BIOCHEMISTRY & MOLECULAR BIOLOGY rank: 50 / 297 = 0.168 (2021) - Q1 - T1
Categ. JCR: FOOD SCIENCE & TECHNOLOGY rank: 12 / 144 = 0.083 (2021) - Q1 - T1
Categ. JCR: CHEMISTRY, MEDICINAL rank: 4 / 63 = 0.063 (2021) - Q1 - T1

Factor impacto CITESCORE: 6.5 - Biochemistry, Genetics and Molecular Biology (Q2)

Factor impacto SCIMAGO: 1.008 - Biochemistry (Q1) - Physiology (Q1) - Molecular Biology (Q1) - Clinical Biochemistry (Q1)

Financiación: info:eu-repo/grantAgreement/ES/CSIC/PIE-202120E019
Financiación: info:eu-repo/grantAgreement/ES/MCIN/FEDER/BIO2017-86559-R

Tipo y forma: Artículo (Versión definitiva)

Área (Departamento): Área Bioquímica y Biolog.Mole. (Dpto. Bioq.Biolog.Mol. Celular)