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Gold nanoparticle assisted assembly of a heme protein for enhancement of long-range interfacial electron transfer

Jensen, Palle S. and Chi, Qijin and Grumsen, Flemming B. and Abad, Jose M. and Horsewell, Andy and Schiffrin, David J. and Ulstrup, Jens (2007) Gold nanoparticle assisted assembly of a heme protein for enhancement of long-range interfacial electron transfer. JOURNAL OF PHYSICAL CHEMISTRY C, 111 (16). pp. 6124-6132.

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Interfacial electron transfer (ET) of biological macromolecules such as metalloproteins is the key process in bioelectrochemistry, enzymatic electrocatalysis, artificial ET chains, single-molecule electronic amplification and rectification, and other phenomena associated with the area of bioelectronics. A key challenge in molecular bioelectronics is to improve the efficiency of long-range charge transfer. The present work shows that this can be achieved by nanoparticle (NP) assisted assembly of cytochrome c (cyt c) on macroscopic single-crystalline electrode surfaces. We present the synthesis and characterization of water-soluble gold nanoparticles (AuNPs) with core diameter 3-4 nm and their application for the enhancement of long-range interfacial ET of a heme protein. Gold nanoparticles were electrostatically conjugated with cyt c to form nanoparticle-protein hybrid ET systems with well-defined stoichiometry. The systems were investigated in homogeneous solution and at liquid/solid interface. Conjugation of cyt c results in a small but consistent broadening of the nanoparticle plasmon band. This phenomenon can be explained in terms of long-range electronic interactions between the gold nanoparticle and the protein molecule. When the nanoparticle-protein conjugates are assembled on Au(111) surfaces, long-range interfacial ET across a physical distance of over 50 A via the nanoparticle becomes feasible. Moreover, significant enhancement of the interfacial ET rate by more than an order of magnitude compared with that of cyt c in the absence of AuNPs is observed. AuNPs appear to serve as excellent ET relays, most likely by facilitating the electronic coupling between the protein redox center and the electrode surface.

Item Type:Article
Subjects:Biomedical Science > Nanobiotechnology
Material Science > Bio materials
Material Science > Nanostructured materials
ID Code:3273
Deposited By:Farnush Anwar
Deposited On:15 Jan 2009 13:59
Last Modified:15 Jan 2009 13:59

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