Top-down production of nanocellulose structures is well-known, but self-assembly of cellulosic oligomers into higher ordered structures is less explored. It has been demonstrated that enzymatic synthesis of cellodextrins is possible. Beyond about DP9 these then self-assemble into a structure resembling a cellulose II antiparallel structure. We demonstrate further that site-selective fluorinated cellodextrins can be produced via chemoenzymatic synthesis with different degrees of fluorination. By preparing a 6-fluorinated glucose 1-phosphate (6F-Glc-1P) donor substrate, we produce multiply 6-fluorinated cellodextrin chains which assemble into particles with morphologies and crystal structures that are unprecedented for cellulose-like materials. It is also demonstrated that post-synthesis of assembly of these novel fluorinated cellodextrins in the presence of cellulose nanocrystals (CNCs) result in 'nanowebs', wherein in the assembled structures link CNCs. These have potential to build larger self-assembled structures and aid in the production of functional gels and composites.

Chemoenzymatic synthesis of cellulose oligomers: Structure and assembly

ACS Spring 2022

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