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A Mechanism of Adsorption of β-Nicotinamide Adenine Dinucleotide on Graphene Sheets: Experiment and Theory

Authors

  • Martin Pumera Dr.,

    1. International Center for Materials Nanoarchitectonics and Biomaterials Center, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan), Fax: (+81) 29-860-4714
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  • Roberto Scipioni Dr.,

    1. International Center for Young Scientists, International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)
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  • Hideo Iwai Dr.,

    1. Materials Analysis Station, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan)
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  • Takahisa Ohno Dr.,

    1. Computational Materials Center, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan)
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  • Yuji Miyahara Dr.,

    1. International Center for Materials Nanoarchitectonics and Biomaterials Center, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan), Fax: (+81) 29-860-4714
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  • Mauro Boero Prof.

    1. Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), UMR 7504 CNRS-University of Strasbourg, 23 rue du Loess, BP 43, 67034 Strasbourg Cedex 2 (France)
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Abstract

β-Nicotinamide adenine dinucleotide (NAD+) and its reduced form (NADH) play major roles in the development of electrochemical enzyme biosensors and biofuel cells. Unfortunately, the oxidation of NADH at carbon electrodes suffers from passivation of the electrodes and a decrease in passing currents. Here, we investigate experimentally and theoretically the reasons for such passivation. High-resolution X-ray photoelectron spectroscopy (HR-XPS), voltammetry, and amperometry show that adsorption occurs on the edges and “edge-like” defects of graphene sheets. HR-XPS and ab initio molecular dynamics show that the adsorption of NAD+ molecules on the edges of graphene happens due to interaction with oxygen-containing groups such as carboxylic groups, while graphene edges substituted only with hydrogen are prone to passivation.

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