Toward Single-Enzyme Molecule Electrochemistry: [NiFe]-Hydrogenase Protein Film Voltammetry at Nanoelectrodes

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• 作者：Freek J. M. Hoeben ; F. Stefan Meijer ; Cees Dekker ; Simon P. J. Albracht ; Hendrik A. Heering ; Serge G. Lemay
• 刊名：ACS Nano
• 出版年：2008
• 出版时间：December 23, 2008
• 年：2008
• 卷：2
• 期：12
• 页码：2497-2504
• 全文大小：426K
• 年卷期：0
• ISSN：1936-086X

文摘

We have scaled down electrochemical assays of redox-active enzymes enabling us to study small numbers of molecules. Our approach is based on lithographically fabricated Au nanoelectrodes with dimensions down to ca. 70 × 70 nm². We first present a detailed characterization of the electrodes using a combination of scanning electron microscopy, cyclic voltammetry, and finite-element modeling. We then demonstrate the viability of the approach by focusing on the highly active [NiFe]-hydrogenase from Allochromatium vinosum immobilized on polymyxin-pretreated Au. Using this system, we successfully demonstrate a distinct catalytic response from less than 50 enzyme molecules. These results strongly suggest the feasibility of using bioelectrochemistry as a new tool for studying redox enzymes at the single-molecule level.