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Effect of Gold Nanoparticles on the Structure and Electron Transfer Characteristics of Glucose Oxidase Redox Polyelectrolyte-Surfactant Complexes

Year: 2014

Journal: CHEMISTRY-A EUROPEAN JOURNAL, Volume 20, Issue 41, pages 13366–13374, October 6, 2014, 20150427

Authors: Lorena Cortez, M.; Marmisolle, Waldemar; Pallarola, Diego; Pietrasanta, Lia I.; Murgida, Daniel H.; Ceolin, Marcelo; Azzaroni, Omar; Battaglini, Fernando

Organizations: Univ Buenos Aires, Fac Ciencias Exactas & Nat, CONICET, INQUIMAE Dept Quim Inorgan Analit & Quim Fis, Buenos Aires, DF, Argentina; Univ Nacl La Plata, Fac Ciencias Exactas, Inst Invest Fis Quim Tas & Aplicadas INIFTA, CONICET,Dept Quim, RA-1900 La Plata, Argentina; Univ Buenos Aires, Fac Ciencias Exactas & Nat, Ctr Microscopias Avanzadas, Buenos Aires, DF, Argentina; Univ Buenos Aires, Fac Ciencias Exactas & Nat, Dept Fis, RA-1428 Buenos Aires, DF, Argentina

Efficient electrical communication between redox proteins and electrodes is a critical issue in the operation and development of amperometric biosensors. The present study explores the advantages of a nanostructured redoxactive polyelectrolyte surfactant complex containing [Os(bpy)(2)Clpy](2+) (bpy=2,2'-bipyridine, py= pyridine) as the redox centers and gold nanoparticles (AuNPs) as nanodomains for boosting the electron-transfer propagation throughout the assembled film in the presence of glucose oxidase (GOx). Film structure was characterized by grazingincidence small-angle X-ray scattering (GISAXS) and atomic force microscopy (AFM), GOx incorporation was followed by surface plasmon resonance (SPR) and quartz-crystal microba- lance with dissipation (QCM-D), whereas Raman spectroelectrochemistry and electrochemical studies confirmed the ability of the entrapped gold nanoparticles to enhance the electron-transfer processes between the enzyme and the electrode surface. Our results show that nanocomposite films exhibit five-fold increase in current response to glucose compared with analogous supramolecular AuNP-free films. The introduction of colloidal gold promotes drastic mesostructural changes in the film, which in turn leads to a rigid, amorphous interfacial architecture where nanoparticles, redox centers, and GOx remain in close proximity, thus improving the electron-transfer