• English
  • Deutsch
  • Log In
    Password Login
    Research Outputs
    Fundings & Projects
    Researchers
    Institutes
    Statistics
Repository logo
Fraunhofer-Gesellschaft
  1. Home
  2. Fraunhofer-Gesellschaft
  3. Scopus
  4. Natural photoredox catalysts promote light-driven lytic polysaccharide monooxygenase reactions and enzymatic turnover of biomass
 
  • Details
  • Full
Options
2022
Journal Article
Title

Natural photoredox catalysts promote light-driven lytic polysaccharide monooxygenase reactions and enzymatic turnover of biomass

Abstract
Lytic polysaccharide monooxygenases (LPMOs) catalyze oxidative cleavage of crystalline polysaccharides such as cellulose and chitin and are important for biomass conversion in the biosphere as well as in biorefineries. The target polysaccharides of LPMOs naturally occur in copolymeric structures such as plant cell walls and insect cuticles that are rich in phenolic compounds, which contribute rigidity and stiffness to these materials. Since these phenolics may be photoactive and since LPMO action depends on reducing equivalents, we hypothesized that LPMOs may enable light-driven biomass conversion. Here, we show that redox compounds naturally present in shed insect exoskeletons enable harvesting of light energy to drive LPMO reactions and thus biomass conversion. The primary underlying mechanism is that irradiation of exoskeletons with visible light leads to the generation of H2O2, which fuels LPMO peroxygenase reactions. Experiments with a cellulose model substrate show that the impact of light depends on both light and exoskeleton dosage and that light-driven LPMO activity is inhibited by a competing H2O2-consuming enzyme. Degradation experiments with the chitin-rich exoskeletons themselves show that solubilization of chitin by a chitin-active LPMO is promoted by light. The fact that LPMO reactions, and likely reactions catalyzed by other biomass-converting redox enzymes, are fueled by light-driven abiotic reactions in nature provides an enzyme-based explanation for the known impact of visible light on biomass conversion.
Author(s)
Kommedal, Eirik G.
Sæther, Fredrikke
Hahn, Thomas  orcid-logo
Fraunhofer-Institut für Grenzflächen- und Bioverfahrenstechnik IGB  
Eijsink, Vincent G.H.
Journal
Proceedings of the National Academy of Sciences of the United States of America : PNAS  
Open Access
DOI
10.1073/pnas.2204510119
Language
English
Fraunhofer-Institut für Grenzflächen- und Bioverfahrenstechnik IGB  
Keyword(s)
  • biomass conversion

  • catecholamines

  • insect exuviae

  • lytic polysaccharide monooxygenases

  • photobiocatalysis

  • Cookie settings
  • Imprint
  • Privacy policy
  • Api
  • Contact
© 2024