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    Functional and Anionic Cellulose-Interacting Polymers by Selective Chemo-Enzymatic Carboxylation of Galactose-Containing Polysaccharides

    Year: 2012

    Journal: Biomacromolecules, 2012, 13 (8), pp 2418–2428, 20120922

    Authors: Kirsti Parikka *†, Ann-Sofie Leppänen ‡, Chunlin Xu ‡§// , Leena Pitkänen †, Paula Eronen , Monika Österberg , Harry Brumer §// , Stefan Willför ‡, and Maija Tenkanen †

    Last authors: Maija Tenkanen

    Organizations: † Department of Food and Environmental Sciences, University of Helsinki, P.O. Box 27, FI-00014 Helsinki, Finland ‡ Process Chemistry Centre, Laboratory of Wood and Paper Chemistry, Åbo Akademi University, Porthansgatan 3, FI-20500 Turku, Finland § Division of Glycoscience, School of Biotechnology, Royal Institute of Technology (KTH), AlbaNova University Center, SE-10691 Stockholm, Sweden //Wallenberg Wood Science Center, Royal Institute of Technology (KTH), SE-10044 Stockholm, Sweden Department of Forest Products Technology, School of Chemical Technology, Aalto University, P.O. Box 16300, FI-00076 Aalto, Espoo, Finland

    Country: Finland, Sverige, Sweden

    Carboxylated, anionic polysaccharides were selectively prepared using a combination of enzymatic and chemical reactions. The galactose-containing polysaccharides studied were spruce galactoglucomannan, guar galactomannan, and tamarind galactoxyloglucan. The galactosyl units of the polysaccharides were first oxidized with galactose oxidase (EC 1.1.3.9) and then selectively carboxylated, resulting in the galacturonic acid derivatives with good conversion and yield. The degrees of oxidation (DO) of the products were determined by gas chromatography–mass spectrometry (GC-MS). A novel feasible electrospray ionization-mass spectrometry (ESI-MS) method was also developed for the determination of DO. The solution properties and charge densities of the products were investigated. The interaction of the products with cellulose was studied by two methods, bulk sorption onto bleached birch kraft pulp and adsorption onto nanocellulose ultrathin films by quartz crystal microbalance with dissipation (QCM-D). To study the effect of the location of the carboxylic acid groups on the physicochemical properties, polysaccharides were also oxidized by 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-mediated reaction producing polyuronic acids. The chemo-enzymatically oxidized galacturonic polysaccharides with an unmodified backbone had a better ability to interact with cellulose than the TEMPO-oxidized products. The selectively carboxylated polysaccharides can be further exploited, as such, or in the targeted functionalization of cellulose surfaces.