Facilitation of High-Rate NADH Electrocatalysis Using Electrochemically Activated Carbon Materials

Li, Hanzi; Li, Rui; Worden, R. Mark; Barton, Scott Calabrese

doi:10.1021/am500087a

Cited by 22 publications

(15 citation statements)

References 84 publications

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“…NADH is a biomolecule with crucial role in redox enzymatic reactions and has wide applications in biosensors, bioenergy and bioconversion processes. [ 65–67 ] However, the electrochemical oxidation of NADH is a very challenging task because of its high detection potential [ 11 ] and slow kinetics on conventional electrodes. [ 65 ]…”

Section: Resultsmentioning

confidence: 99%

Polydopamine nanofilms for high‐performance paper‐based electrochemical devices

et al. 2021

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Since the discovery of polydopamine (PDA), there has been a lot of progress on using this substance to functionalize many different surfaces. However, little attention has been given to prepare functionalized surfaces for the preparation of flexible electrochemical paper‐based devices. After fabricating the electrodes on paper substrates, we formed PDA on the surface of the working electrode using a chemical polymerization route. PDA nanofilms on carbon were characterized by contact angle (CA) experiments, X‐ray photoelectron spectroscopy, scanning electron microscopy, atomic force microscopy (topography and electrical measurements) and electrochemical techniques. We observed that PDA introduces chemical functionalities (RNH2 and RC═O) that decrease the CA of the electrode. Moreover, PDA nanofilms did not block the heterogeneous electron transfer. In fact, we observed one of the highest standard heterogeneous rate constants (ks) for electrochemical paper‐based electrodes (2.5 ± 0.1) × 10−3 cm s−1, which is an essential parameter to obtain larger currents. In addition, our results suggest that carbonyl functionalities are ascribed for the redox activity of the nanofilms. As a proof‐of‐concept, the electrooxidation of nicotinamide adenine dinucleotide showed remarkable features, such as, lower oxidation potential, electrocatalytic peak currents more than 30 times higher when compared to unmodified paper‐based electrodes and electrocatalytic rate constant (kobs) of (8.2 ± 0.6) × 102 L mol−1 s−1.

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Section: Resultsmentioning

confidence: 99%

Polydopamine nanofilms for high‐performance paper‐based electrochemical devices

et al. 2021

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“…The partially polymerized MG is due to adsorbed MG which was cycled three times in the potential window −1.2 V to 0.3 V, causing the adsorbed MG to partially polymerize. This was done in order to provide a comparison to other CVs presented with adsorbed MG, 47 For the bare carbon electrodes, N-CNTs display the lowest E p , as previously reported. 27 In this report, the third cycle is shown in Figure 7 and displayed in Table I, which will be slightly different than those values previously reported, which used the first cycle.…”

Section: Spontaneous Oxidation Of Nadh By Mg In Solution-mentioning

confidence: 99%

“…[38][39][40][41][42][43][44][45][46] Recently, Barton and coworkers reported that adsorption of MG onto CNTs was a more effective method to couple the carbon electrode material with the redox mediator than electropolymerization. 47 Herein, we present a detailed investigation of the electrochemical oxidation of NADH at CNT and N-CNT electrodes using the redox mediator MG as immobilized through electropolymerization or spontaneous adsorption. Our technique is sensitive to surface oxidation, which is inherent to the electropolymerization of MG due to the high potentials employed.…”

mentioning

confidence: 99%

Enhanced Electrochemical Oxidation of NADH at Carbon Nanotube Electrodes Using Methylene Green: Is Polymerization Necessary?

Goran

Favela

Rust

et al. 2014

J. Electrochem. Soc.

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Carbon nanotubes (CNTs) have been established as an electrocatalytic material for the oxidation of dihydronicotinamide adenine dinucleotide (NADH). Heteroatom doped CNTs, either boron or nitrogen, have been shown to enhance the electrocatalytic oxidation. Methylene green (MG), a well-established redox mediator for NADH oxidation, is shown here to further enhance the electrocatalytic oxidation of NADH at CNTs and nitrogen-doped CNTs (N-CNTs), but the standard technique of electropolymerizing MG on the surface of the electrode attenuates the natural reactivity of the nanotube/MG couple as formed through spontaneous adsorption. Additionally, MG coupled CNT/N-CNTs produces a leveling effect on N-CNTs, eliminating their electrocatalytic enhancement due to nitrogen doping. Nondoped CNTs display a slightly more efficient oxidation of NADH after adsorption of MG, due to an increased hydrophobic character which causes the adsorbed MG to reside slightly closer to the nanotube surface, and thus, facilitates more facile electron transfer between the nanotube/MG redox couple. Investigation of the influence of potential on MG adsorbed onto CNT/N-CNT electrodes allows the detection of MG polymerization, which is initiated at 0.05 V (vs. Hg/Hg 2 SO 4 ) as an anodic stripping peak, along with the appearance of a reversible surface wave with E 1/2 at −1.0 V (0.1 M sodium phosphate buffer pH 7.0).Bioelectrodes 1 for biosensor 2-4 and biofuel cell 5-7 applications have always paid special attention to the electrochemical oxidation of dihydronicotinamide adenine dinucleotide (NADH), since the oxidized form (NAD + ) is a cofactor for dehydrogenases, the largest group of oxidoreductase enzymes. Oxidation of NADH at bare electrode surfaces requires a large overpotential and subsequently fouls the electrode surface. 4 In order to mitigate these problems, mediators were applied to electrodes, often called mediator-modified or chemically modified electrodes. 8-11 Methylene green (MG) was found to be one of the most promising redox mediators employed, mainly being polymerized or electropolymerized to ensure immobilization onto the electrode surface. 12-17 The use of electropolymerized MG as an electrode modifier has even been employed as a way to standardize electrocatalytic electrode performance across multiple laboratories. 18 Advanced electrode materials such as carbon nanotubes (CNTs) have been shown to lower the overpotential for NADH oxidation without the use of a mediator, due to their unique physicochemical properties. [19][20][21][22] Oxidizing the CNTs increased their catalytic character, as shown by Wooten et al. 23 and Chakraborty et al. 24 Tominaga et al. have demonstrated that the peak oxidation potential for NADH at single walled CNTs is a function of the oxidation level, as measured by Raman and X-ray photoelectron spectroscopy. 25 As a further enhancement, heteroatom doped CNTs, either boron 26 or nitrogen, 27 have been shown to possess higher electrocatalytic activity toward NADH oxidation than their nondoped counterparts....

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“…It is a very important coenzyme in biological reactions, and the ratio of the reduced/oxidized forms, NADH/NAD, can indicate some critical changes in the organism, such as the decrease of the energy production due to their influence on the ATP level, in addition to showing the emergence of Parkinson's diseases and insomnia . For this reason, NADH analysis is an important issue, and is usually carried out by electrochemistry techniques, exploiting a great variety of electrodes, such as those modified with SWCNTs, oxidized reduced graphene oxide, polymers, dyes and ferrite nanocomposite . In general, the modified electrodes have advantages over the conventional electrodes such as gold (Au), platinum (Pt) and glassy Carbon (GCE) , e. g. by allowing to perform under less positive oxidation potentials, and exhibiting a greater sensitivity associated with an improved electron transfer kinetics at the electrode‐solution interface.…”

Section: Introductionmentioning

confidence: 99%

Magnetite Nanoparticles Bonded Carbon Quantum Dots Magnetically Confined onto Screen Printed Carbon Electrodes and their Performance as Electrochemical Sensor for NADH

et al. 2017

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Hybrid magnetite/carbon quantum dots (MagNP/C‐dots) were prepared and their characterization performed by high resolution transmission electron microscopy (HR‐TEM), X‐ray diffraction (XRD) and X‐ray photoelectron spectroscopy (XPS). Because of their suitable magnetization and electrochemical properties, they were used as versatile electrode modifiers after magnetically confining onto screen printed carbon electrodes (SPE), with the aid of a miniature external magnet. The reported strategy introduces a convenient procedure for assembling modified electrodes, since the nanoparticles can be easily released by removing the magnet. The non‐enzymatic magnetic biosensor showed excellent performance in the determination of NADH at the concentration range 2×10−7 to 5×10−6 mol L−1, exhibiting a sensitivity of 0.15 μmol L−1 and detection limit of 20 nmol L−1. The MagNP/C‐dots/SPE sensor was also successfully applied for the determination of NADH in serum samples. The interference of typical biological molecules has also been investigated.

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Facilitation of High-Rate NADH Electrocatalysis Using Electrochemically Activated Carbon Materials

Cited by 22 publications

References 84 publications

Polydopamine nanofilms for high‐performance paper‐based electrochemical devices

Polydopamine nanofilms for high‐performance paper‐based electrochemical devices

Enhanced Electrochemical Oxidation of NADH at Carbon Nanotube Electrodes Using Methylene Green: Is Polymerization Necessary?

Magnetite Nanoparticles Bonded Carbon Quantum Dots Magnetically Confined onto Screen Printed Carbon Electrodes and their Performance as Electrochemical Sensor for NADH

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