Complex carbohydrates play crucial roles in energy storage, cell recognition, and structural building, but cellular polysaccharides are under-investigated compared to proteins and nucleic acids. Solid-state NMR characterization of polysaccharide structure in either intact cells or native physical status, since its emergence, has presented an important technique to glycoanalysis. The bioenergy and biomedical systems being studied have expanded from the cell walls plants and bacteria to other organisms such as algae and fungi. Here we will use two photosynthetic organisms, plants (grass and wood) and microalgae, as examples to briefly discuss how ssNMR can help to address the structural complexity and dynamical heterogeneity of polysaccharides. Notably, we have revealed how carbohydrates pack with an aromatic polymer named lignin to form the mechanical core of plant secondary cell walls. The functions of carbohydrates were found to be conformation-dependent: the hemicellulose xylan uses its non-flat domains to bind lignin and preferentially relies on its flat-ribbon domains to coat the even surface of cellulose microfibrils. Cellulose only serves as the secondary binding target of lignin which happens more frequently in woody materials. Such insights provide the structural foundation for designing improved processes for using plant biomass for energy and material production.

Solid-state NMR techniques for investigating polysaccharide structure and interactions with lignin in plant biomaterials

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