NAD⁺/NADH Tethering on MWNTs-Bucky Papers for Glucose Dehydrogenase-Based Anodes

Abstract

Reagentless and non-reagentless nicotinamide adenine dinucleotide (NAD + )-dependent glucose dehydrogenase (GDH) bioanodes integrating multiwalled nanotubes (WMNTs)-bucky papers are introduced in this study. The NAD + was tethered by pyrene butanoic acid succinimidyl ester (PBSE) to the wall of the carbonic MWNTs composing the bucky paper by π-π stacking interactions. The designs have been evaluated electrochemically and by X-ray spectroscopy. The electrodes have been assembled to a quasi-2D microfluidic system with capillary driven flow. Michaelis-Menten analysis on CMN-MG-PBSE-NAD + -GDH, reagentless bioanode, in an electrolytic cell shows a limiting current and constant of I Max = 3.252 ± 0.134 mA.cm −2 and K M = 48.3 ± 4.6 mM at 4 • C, and I Max = 2.568 ± 0.085 mA.cm −2 and K M = 13.6 ± 1.8 mM at 25 • C for 0.1 M glucose. Results demonstrate the enzymatic system, in non-reagentless and reagentless bioanode, has an extraordinary current density generation. In the reagentless bioanode design, the enzyme and its cofactor are highly catalytically active, and the design can be feasible integrated into biofuel cell assembly and later used as a power source for small portable devices. The development and implementation of alternative energy systems is highly desired and envisioned for overcoming environmental issues. Furthermore, designing environmentally friendly power devices is needed because current systems such as conventional batteries have shown to contain toxic compounds and produce toxic residues. 1Harvesting energy from glucose, for example, would make possible the utilization of fruits as well as commercial drinks as source of biofuel and the products of their oxidation are naturally biodegradable. Enzymatic biofuel cells are devices engineered for that purpose. 2-4These biofuel cells are envisioned to power small portable devices and devices for biomedical applications. [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17] Increasing the efficiency of the biofuel cell systems requires decreasing limitations on the kinetics of the catalytic layer, resistivity losses of the electrode materials and mass transport losses. In previous work, we reported the integration of bucky papers 18 (multiwalled carbon nanotube (MWNTs)-based papers) to bioelectrode designs to reduce kinetic and ohmic limitations. The employment of a quasi-2D microfluidic system (paper-based fan) was employed to decrease mass transport limitations of fuel to the catalytic layer. The enzymatic systems were immobilized within CNTs network-Chitosan 3D-matrix in order to improve electron transfer and enzyme life-time. Herein, the improvement of the NAD + -dependent glucose dehydrogenase (GDH)-based bioanode is presented.Harvesting energy from glucose by enzymatic biofuel cells could be performed by using oxidoreductase enzymes such as glucose dehydrogenase (GDH) on the anode 19 and analogous enzymatic systems on the cathode for reduction of oxygen from air. 20,21 At the anode, GDH shows a biocatalytic activity when coupled to its NAD + /NADH-...

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