Assembling Native Elementary Cellulose Nanofibrils via a Reversible and Regioselective Surface Functionalization

Marco Beaumont, Blaise L. Tardy, Guillermo Reyes, Tetyana V. Koso, Elisabeth Schaubmayr, Paul Jusner, Alistair W.T. King, Raymond R. Dagastine, Antje Potthast, Orlando J. Rojas, Thomas Rosenau

Research output: Contribution to journalArticleScientificpeer-review

1 Citation (Scopus)

Abstract

Selective surface modification of biobased fibers affords effective individualization and functionalization into nanomaterials, as exemplified by the TEMPO-mediated oxidation. However, such a route leads to changes of the native surface chemistry, affecting interparticle interactions and limiting the development of potential supermaterials. Here we introduce a methodology to extract elementary cellulose fibrils by treatment of biomass with N-succinylimidazole, achieving regioselective surface modification of C6-OH, which can be reverted using mild post-treatments. No polymer degradation, cross-linking, nor changes in crystallinity occur under the mild processing conditions, yielding cellulose nanofibrils bearing carboxyl moieties, which can be removed by saponification. The latter offers a significant opportunity in the reconstitution of the chemical and structural interfaces associated with the native states. Consequently, 3D structuring of native elementary cellulose nanofibrils is made possible with the same supramolecular features as the biosynthesized fibers, which is required to unlock the full potential of cellulose as a sustainable building block.

Original languageEnglish
Pages (from-to)17040-17046
Number of pages7
JournalJournal of the American Chemical Society
Volume143
Issue number41
DOIs
Publication statusPublished - 20 Oct 2021
MoE publication typeA1 Journal article-refereed

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