title: Electrodeposition of a biopolymeric hydrogel: potential for one-step protein electroaddressing.
abstract: The electrodeposition of hydrogels provides a programmable means to assemble soft matter for various technological applications. We report an anodic method to deposit hydrogel films of the aminopolysaccharide chitosan. Evidence suggests the deposition mechanism involves the electrolysis of chloride to generate reactive chlorine species (e.g., HOCl) that partially oxidize chitosan to generate aldehydes that can couple covalently with amines (presumably through Schiff base linkages). Chitosan's anodic deposition is controllable spatially and temporally. Consistent with a covalent cross-linking mechanism, the deposited chitosan undergoes repeated swelling/deswelling in response to pH changes. Consistent with a covalent conjugation mechanism, proteins could be codeposited and retained within the chitosan film even after detergent washing. As a proof-of-concept, we electroaddressed glucose oxidase to a side-wall electrode of a microfabricated fluidic channel and demonstrated this enzyme could perform electrochemical biosensing functions. Thus, anodic chitosan deposition provides a reagentless, single-step method to electroaddress a stimuli-responsive and biofunctionalized hydrogel film.
authors.affiliation: Institute for Bioscience and Biotechnology Research, University of Maryland, College Park, Maryland 20742, United States.
authors.forename: Kelsey M
authors.initials: KM
authors.lastname: Gray
authors.forename: Benjamin D
authors.initials: BD
authors.lastname: Liba
authors.forename: Yifeng
authors.initials: Y
authors.lastname: Wang
authors.forename: Yi
authors.initials: Y
authors.lastname: Cheng
authors.forename: Gary W
authors.initials: GW
authors.lastname: Rubloff
authors.forename: William E
authors.initials: WE
authors.lastname: Bentley
authors.forename: Alexandra
authors.initials: A
authors.lastname: Montembault
authors.forename: Isabelle
authors.initials: I
authors.lastname: Royaud
authors.forename: Laurent
authors.initials: L
authors.lastname: David
authors.forename: Gregory F
authors.initials: GF
authors.lastname: Payne
mesh_terms: D001704:Biopolymers / Q000737:chemistry*; D015374:Biosensing Techniques; D048271:Chitosan / Q000737:chemistry*; D003432:Cross-Linking Reagents / Q000737:chemistry; D055664:Electrochemical Techniques; D004566:Electrodes; D004595:Electroplating / Q000379:methods*; D005949:Glucose Oxidase / Q000737:chemistry* / Q000378:metabolism; D020100:Hydrogels / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration
chemical_list: D001704:Biopolymers; D003432:Cross-Linking Reagents; D020100:Hydrogels; D048271:Chitosan; D005949:Glucose Oxidase