title: Effect of deglycosylation of cellobiose dehydrogenases on the enhancement of direct electron transfer with electrodes.
abstract: Cellobiose dehydrogenase (CDH) is a monomeric extracellular flavocytochrome composed of a catalytic dehydrogenase domain (DH(CDH)) containing flavin adenine dinucleotide (FAD), a cytochrome domain (CYT(CDH)) containing heme b, and a linker region connecting the two domains. In this work, the effect of deglycosylation on the electrochemical properties of CDH from Phanerochaete chrysosporium (PcCDH) and Ceriporiopsis subvermispora (CsCDH) is presented. All the glycosylated and deglycosylated enzymes show direct electron transfer (DET) between the CYT(CDH) and the electrode. Graphite electrodes modified with deglycosylated PcCDH (dPcCDH) and CsCDH (dCsCDH) have a 40-65% higher I(max) value in the presence of substrate than electrodes modified with their glycosylated counterparts. CsCDH trapped under a permselective membrane showed similar changes on gold electrodes protected by a thiol-based self-assembled monolayer (SAM), in contrast to PcCDH for which deglycosylation did not exhibit any different electrocatalytical response on SAM-modified gold electrodes. Glycosylated PcCDH was found to have a 30% bigger hydrodynamic radius than dPcCDH using dynamic light scattering. The basic bioelectrochemistry as well as the bioelectrocatalytic properties are presented.
authors.affiliation: Department of Analytical Chemistry/Biochemistry and Structural Biology, Lund University, Sweden.
authors.forename: Roberto
authors.initials: R
authors.lastname: Ortiz
authors.forename: Hirotoshi
authors.initials: H
authors.lastname: Matsumura
authors.forename: Federico
authors.initials: F
authors.lastname: Tasca
authors.forename: Kawah
authors.initials: K
authors.lastname: Zahma
authors.forename: Masahiro
authors.initials: M
authors.lastname: Samejima
authors.forename: Kiyohiko
authors.initials: K
authors.lastname: Igarashi
authors.forename: Roland
authors.initials: R
authors.lastname: Ludwig
authors.forename: Lo
authors.initials: L
authors.lastname: Gorton
mesh_terms: D002237:Carbohydrate Dehydrogenases / Q000737:chemistry / Q000378:metabolism*; D002244:Carbon / Q000737:chemistry; D002462:Cell Membrane / Q000378:metabolism; D002475:Cellobiose / Q000378:metabolism; D055453:Coriolaceae / Q000201:enzymology*; D003460:Crystallization; D004563:Electrochemistry; D004566:Electrodes; D004579:Electron Transport; D004583:Electrons; D005182:Flavin-Adenine Dinucleotide / Q000378:metabolism; D006031:Glycosylation; D006046:Gold / Q000737:chemistry; D006108:Graphite / Q000737:chemistry; D007700:Kinetics; D053758:Nanoparticles; D020075:Phanerochaete / Q000201:enzymology*; D017434:Protein Structure, Tertiary
chemical_list: D005182:Flavin-Adenine Dinucleotide; D002475:Cellobiose; D002244:Carbon; D006046:Gold; D006108:Graphite; D002237:Carbohydrate Dehydrogenases; C019859:cellobiose-quinone oxidoreductase