Understanding laccase/HBT-catalyzed grass delignification at the molecular level

Hilgers, Roelant; Erven, Gijs van; Boerkamp, Vincent J.P.; Sulaeva, Irina; Potthast, Antje; Kabel, Mirjam A.; Vincken, Jean‐Paul

doi:10.1039/c9gc04341a

Cited by 29 publications

(41 citation statements)

References 65 publications

(95 reference statements)

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“…Interestingly, diketone products, pyrolysis markers for dihydroxyphenylketones, had increased significantly after fungal growth from 0.16 ± 0.00% to 0.25 ± 0.00% of the relative abundance of lignin-derived pyrolysis products; and consequently explained a major part of the increase of the C α -oxidized substructures. These markers have also been observed after the action of the white-rot fungus Ceriporiopsis subvermispora [19] and for laccase-mediator systems [27], suggesting that O-4′-cleavage of β-O-4′ aryl ethers is likely one of the involved ligninolysis routes. anserina on wheat straw lignin isolate and insoluble wheat glucoronoarabinoxylan.…”

Section: Structural Characterization Of Lignin After Growth Of P Ansmentioning

confidence: 78%

Evidence for ligninolytic activity of the ascomycete fungus Podospora anserina

Erven

Kleijn

Patyshakuliyeva

et al. 2020

Biotechnol Biofuels

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Background: The ascomycete fungus Podospora anserina has been appreciated for its targeted carbohydrate-active enzymatic arsenal. As a late colonizer of herbivorous dung, the fungus acts specifically on the more recalcitrant fraction of lignocellulose and this lignin-rich biotope might have resulted in the evolution of ligninolytic activities. However, the lignin-degrading abilities of the fungus have not been demonstrated by chemical analyses at the molecular level and are, thus far, solely based on genome and secretome predictions. To evaluate whether P. anserina might provide a novel source of lignin-active enzymes to tap into for potential biotechnological applications, we comprehensively mapped wheat straw lignin during fungal growth and characterized the fungal secretome.Results: Quantitative 13 C lignin internal standard py-GC-MS analysis showed substantial lignin removal during the 7 days of fungal growth (24% w/w), though carbohydrates were preferably targeted (58% w/w removal). Structural characterization of residual lignin by using py-GC-MS and HSQC NMR analyses demonstrated that C α -oxidized substructures significantly increased through fungal action, while intact β-O-4′ aryl ether linkages, p-coumarate and ferulate moieties decreased, albeit to lesser extents than observed for the action of basidiomycetes. Proteomic analysis indicated that the presence of lignin induced considerable changes in the secretome of P. anserina. This was particularly reflected in a strong reduction of cellulases and galactomannanases, while H 2 O 2 -producing enzymes clearly increased. The latter enzymes, together with laccases, were likely involved in the observed ligninolysis. Conclusions:For the first time, we provide unambiguous evidence for the ligninolytic activity of the ascomycete fungus P. anserina and expand the view on its enzymatic repertoire beyond carbohydrate degradation. Our results can be of significance for the development of biological lignin conversion technologies by contributing to the quest for novel lignin-active enzymes and organisms.

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Section: Structural Characterization Of Lignin After Growth Of P Ansmentioning

confidence: 78%

Evidence for ligninolytic activity of the ascomycete fungus Podospora anserina

Erven

Kleijn

Patyshakuliyeva

et al. 2020

Biotechnol Biofuels

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“…While many of the reports focus strictly their attention on the cytotoxicity and biocompatibility studies, the biodegradability of these materials remains largely unexplored. It is well known that lignin can be partially decomposed by enzymes, 16,184 but most of these smart materials described above are based on chemical modification of lignin, which probably disrupts the degradability process. For instance, cross-linked lignin materials are likely drastically less biodegradable and the absence of phenolic hydroxyl groups hinders accessibility of these primary sites in enzymatic degradation processes.…”

Section: Biomedical Applicationsmentioning

confidence: 99%

Lignin-based smart materials: a roadmap to processing and synthesis for current and future applications

2020

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“…2.9 incubated with steamexploded biomass (Eucalyptus globulus) at 60 °C for 24 h in the presence of HBT as mediator obtaining a decrease in the intensity of the IR bands associated with lignin aromatic backbone and lignin−hemicellulose linkages. 152 A very recent study sheds light on the intimate mechanism of straw delignification by a LC/HBT mediator system: 153 subtle analytical methods revealed Cα oxidation and Cα−Cβ and β-O−4 oxidative cleavage. In the same study, a significant reduction in phenylcoumaran and resinol linkages was found, showing that also the poorly reactive β−β and β−5 C−C links could be targets of the laccase/mediator system.…”

Section: Protocolsmentioning

confidence: 99%

Recent Developments in the Delignification and Exploitation of Grass Lignocellulosic Biomass

Tocco

Carucci

Monduzzi

et al. 2021

ACS Sustainable Chem. Eng.

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Biofuels could be defined as the fuels of the future, although much work is still required before they will replace fossil fuels. In this review, lignocellulosic biomass based on straw and related crops and wastes is described concerning its lignin contents, structure, and properties, and an overview on the means of current and predictable delignification protocols is presented. The discussion is focused on herbaceous monocot materials and their available pretreatments (physical, chemical, and enzymatic), with special emphasis on fungal ligninolytic enzymes and the most recent findings and developments in their current application, issues, and perspectives.

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Understanding laccase/HBT-catalyzed grass delignification at the molecular level

Abstract: An in-depth study on the pathways underlying wheat straw and corn stover delignification by a laccase/HBT system. New insights were obtained by comprehensive fractionation, purification and analysis.

Cited by 29 publications

References 65 publications

Evidence for ligninolytic activity of the ascomycete fungus Podospora anserina

Evidence for ligninolytic activity of the ascomycete fungus Podospora anserina

Lignin-based smart materials: a roadmap to processing and synthesis for current and future applications

Recent Developments in the Delignification and Exploitation of Grass Lignocellulosic Biomass

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