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- Erlandsson, Johan, et al.
(author)
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On the mechanism behind freezing-induced chemical crosslinking in ice-templated cellulose nanofibril aerogels
- 2018
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In: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 6:40, s. 19371-19380
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Journal article (peer-reviewed)abstract
- The underlying mechanism related to freezing-induced crosslinking of aldehyde-containing cellulose nanofibrils (CNFs) has been investigated, and the critical parameters behind this process have been identified. The aldehydes introduced by periodate oxidation allows for formation of hemiacetal bonds between the CNFs provided the fibrils are in sufficiently close contact before the water is removed. This is achieved during the freezing process where the cellulose components are initially separated, and the growth of ice crystals forces the CNFs to come into contact in the thin lamellae between the ice crystals. The crosslinked 3-D structure of the CNFs can subsequently be dried under ambient conditions after solvent exchange and still maintain a remarkably low density of 35 kg m-3, i.e. a porosity greater than 98%. A lower critical amount of aldehydes, 0.6 mmol g-1, was found necessary in order to generate a crosslinked 3-D CNF structure of sufficient strength not to collapse during the ambient drying. The chemical stability of the 3-D structure can be further enhanced by converting the hemiacetals to acetals by treatment with an alcohol under acidic conditions.
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2. |
- Hult, Daniel, 1986-, et al.
(author)
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Degradable High Tg Sugar Derived Polycarbonates from Isosorbide and Dihydroxyacetone
- 2018
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In: Polymer Chemistry. - : Royal Society of Chemistry. - 1759-9954 .- 1759-9962. ; 9:17, s. 2238-2246
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Journal article (peer-reviewed)abstract
- Polycarbonates from isosorbide and dihydroxyacetone (DHA) have been synthesised using organocatalytic step-growth polymerization of their corresponding diols and bis-carbonylimidazolides monomers. By choice of feed ratio and monomer activation, either isosorbide or ketal protected DHA, random and alternating poly(Iso-co-DHA) carbonates have been formed. Thermal properties by DSC and TGA were herein strongly correlated to monomer composition. Dilution studies using 1H-NMR of a model compound DHA-diethyl carbonate in acetonitrile and deuterated water highlighted the influence of α-substituents on the keto/hydrate equilibrium of DHA. Further kinetics studies of in the pH* range of 4.7 to 9.6 serve to show the hydrolytic pH-profile of DHA-carbonates. The Hydrolytic degradation of deprotected polymer pellets show an increased degradation with increasing DHA content. Pellets with a random or alternating configuration show different characteristics in terms of mass loss and molecular weight loss profile over time.
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