Elucidation of in Situ Ligninolysis Mechanisms of the Selective White-Rot Fungus Ceriporiopsis subvermispora

Gijs van Erven, Roelant Hilgers, Pieter de Waard, Erik Jan Gladbeek, Willem J.H. van Berkel, Mirjam A. Kabel*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

14 Citations (Scopus)

Abstract

Lignin degradation by white-rot fungi is an essential step in terrestrial carbon cycling and has great potential for biotechnological applications. Selective white-rot fungi have been recognized for their ability to effectively delignify lignocellulose, but the underlying mechanisms, particularly in situ, have largely remained elusive to date. In this work, we elucidate specific degradation routes of β-O-4 aryl ethers in actual lignocellulosic biomass for the industrially relevant selective white-rot fungus Ceriporiopsis subvermispora. Multidimensional NMR and py-GC-MS analyses together with enzymatically synthesized model compounds enabled, for the first time, the identification of various diagnostic lignin cleavage products in residual wheat straw. Our results support that in situ ligninolysis by C. subvermispora is initiated by single-electron transfer, which then cascades into the cleavage of Cα-Cβ, Cβ-O, and O-4-aryl bonds of β-O-4 aryl ethers. The high abundance of 1-(benzyl)-2,3-dihydroxypropan-1-ones indicated that β-O-|4 cleavage is a more important pathway than previously considered. Our approach highlights key diagnostic substructures for providing mechanistic insight into fungal ligninolysis.

Original languageEnglish
Pages (from-to)16757-16764
JournalACS Sustainable Chemistry and Engineering
Volume7
Issue number19
DOIs
Publication statusPublished - 7 Oct 2019

Keywords

  • Lignin
  • NMR spectroscopy
  • Oxidation
  • py-GC-MS
  • Selective delignification

Fingerprint

Dive into the research topics of 'Elucidation of in Situ Ligninolysis Mechanisms of the Selective White-Rot Fungus Ceriporiopsis subvermispora'. Together they form a unique fingerprint.

Cite this