title: Functionalized Celluloses with Regular Substitution Pattern by Glycosynthase-Catalyzed Polymerization.
abstract: Control of the monomer sequence in polymers is extraordinarily difficult by chemical synthesis, though Nature routinely exerts such control, including in the biosynthesis of polysaccharides. This inability has prevented us from being able to match the exquisite structure-activity control exhibited in biosynthesis of bioactive natural polysaccharides. We here address a powerful approach, whereby enzyme-catalyzed polymerization of properly modified building blocks is introduced as a simple route affording polysaccharides with controlled sequence and functionalization pattern. Targeting cellulose as a versatile scaffold for novel biomaterials, we describe the preparation of a perfectly alternating polysaccharide with repeat unit 6'-azido-6'-deoxycellobiose by a glycosynthase-catalyzed polymerization using the Humicola insolens cellulase Cel7B E197A mutant, and its further functionalization to give novel modified cellulose derivatives with a regular substitution pattern.
authors.affiliation: Laboratory of Biochemistry, Institut Químic de Sarrià, Universitat Ramon Llull , Via Augusta 390, 08017 Barcelona, Spain.
authors.forename: Victoria
authors.initials: V
authors.lastname: Codera
authors.affiliation: Department of Sustainable Biomaterials, Macromolecules and Interfaces Institute, and Institute for Critical Technologies and Applied Science, Virginia Tech , Blacksburg, Virginia 24061, United States.
authors.forename: Kevin J
authors.initials: KJ
authors.lastname: Edgar
authors.affiliation: Laboratory of Biochemistry, Institut Químic de Sarrià, Universitat Ramon Llull , Via Augusta 390, 08017 Barcelona, Spain.
authors.forename: Magda
authors.initials: M
authors.lastname: Faijes
authors.affiliation: Laboratory of Biochemistry, Institut Químic de Sarrià, Universitat Ramon Llull , Via Augusta 390, 08017 Barcelona, Spain.
authors.forename: Antoni
authors.initials: A
authors.lastname: Planas
mesh_terms: D001203:Ascomycota / Q000201:enzymology; D002384:Catalysis; D002480:Cellulase / Q000378:metabolism; D002482:Cellulose / Q000031:analogs & derivatives* / Q000737:chemistry*; D058105:Polymerization; D011108:Polymers / Q000138:chemical synthesis* / Q000737:chemistry; D011134:Polysaccharides / Q000737:chemistry*
chemical_list: C000590804:6-azido-6-deoxycellulose; D011108:Polymers; D011134:Polysaccharides; D002482:Cellulose; D002480:Cellulase