Lytic Polysaccharide Monooxygenase Increases Cellobiohydrolases Activity by Promoting Decrystallization of Cellulose Surface

Taku Uchiyama, Takayuki Uchihashi, Takuya Ishida, Akihiko Nakamura, Josh Vermaas, Michael Crowley, Masahiro Samejima, Gregg Beckham, Kiyohiko Igarashi

Research output: Contribution to journalArticlepeer-review

16 Scopus Citations

Abstract

Efficient depolymerization of crystalline cellulose requires cooperation between multiple cellulolytic enzymes. Through biochemical approaches, molecular dynamics (MD) simulation, and single-molecule observations using high-speed atomic force microscopy (HS-AFM), we quantify and track synergistic activity for cellobiohydrolases (CBHs) with a lytic polysaccharide monooxygenase (LPMO) from Phanerochaete chrysosporium. Increasing concentrations of LPMO (AA9D) increased the activity of a glycoside hydrolase family 6 CBH, Cel6A, whereas the activity of a family 7 CBH (Cel7D) was enhanced only at lower concentrations of AA9D. MD simulation suggests that the result of AA9D action to produce chain breaks in crystalline cellulose can oxidatively disturb the crystalline surface by disrupting hydrogen bonds. HS-AFM observations showed that AA9D increased the number of Cel7D molecules moving on the substrate surface and increased the processivity of Cel7D, thereby increasing the depolymerization performance, suggesting that AA9D not only generates chain ends but also amorphizes the crystalline surface, thereby increasing the activity of CBHs.

Original languageAmerican English
Article numbereade5155
Number of pages11
JournalScience Advances
Volume8
Issue number51
DOIs
StatePublished - Dec 2022

Bibliographical note

Publisher Copyright:
Copyright © 2022 The Authors, some rights reserved.

NREL Publication Number

  • NREL/JA-2A00-83478

Keywords

  • biobased feedstock
  • cellobiohydrolases
  • cellulose depolymerization
  • molecular dynamics

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