Biomolecular Systems in the Context of Sustainable Applications Studied by NMR

Abstract

The rapid substitution of non-sustainable practices at all levels of global industrial production processes has become of primary importance due to the strain worldwide ecosystems nowadays face. Notably, biomolecular complexes formed by renewable fungal sources can be employed as biodegradable mycelium-based materials to reduce the use of for instance (petro)chemical plastics that are major contributors to worldwide pollution. Meanwhile, the pervasive use of biohazardous solvents in large scale reactions for the production of everyday compounds may be alleviated by the introduction of biocatalytic approaches. Favorably, advancements are being made in the field of designer enzyme based (bio)catalysis of novel new-to-nature reactions that abolish harsh reaction conditions. However, full exploitation of (large) biomolecular complexes remains limited as long as structural, dynamical and chemical insight in native conditions remain elusive. Nuclear magnetic resonance (NMR) spectroscopy in both solution and solid-state (ss) applications has emerged as a powerful tool for the non-destructive study of molecules and their motions and structures at atomic-level resolution. In this work, we applied diverse NMR tools to disentangle the composition and arrangement of the carbohydrates in fungal cell walls that are essential to the properties of the mycelial ensemble, and the structural and chemical equilibria of the artificial metalloenzyme (ArM) based on the lactococcal multidrug resistance regulator (LmrR) following directed evolution steps to improve its reactivity.