Enzymatic biofuel cells designed for direct power generation from biofluids in living organisms

Miyake, Takeo; Haneda, K.; Nagai, Nobuhiro; Yatagawa, Y.; Onami, Hideyuki; Yoshino, Syuhei; Abe, Toshiaki; Nishizawa, Masatoyo

doi:10.1039/c1ee02200h

Cited by 229 publications

(176 citation statements)

References 32 publications

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“…We use GDH (EC 1.1.1.47, 250 U mg −1 ) donated from TOYOBO. 23,24 Two input signals activate GDH; input A is NAD + and input B is glucose (Fig. 4(a)).…”

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confidence: 99%

An enzyme logic bioprotonic transducer

et al. 2014

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Translating ionic currents into measureable electronic signals is essential for the integration of bioelectronic devices with biological systems. We demonstrate the use of a Pd/PdHx electrode as a bioprotonic transducer that connects H+ currents in solution into an electronic signal. This transducer exploits the reversible formation of PdHx in solution according to PdH↔Pd + H+ + e−, and the dependence of this formation on solution pH and applied potential. We integrate the protonic transducer with glucose dehydrogenase as an enzymatic and gate for glucose and NAD+. PdHx formation and associated electronic current monitors the output drop in pH, thus transducing a biological function into a measurable electronic output.

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“…We use GDH (EC 1.1.1.47, 250 U mg −1 ) donated from TOYOBO. 23,24 Two input signals activate GDH; input A is NAD + and input B is glucose (Fig. 4(a)).…”

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confidence: 99%

An enzyme logic bioprotonic transducer

et al. 2014

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“…1,2 Applications of EBFCs range from energy sources for small electronic devices, 3 self-powered sensors 4 and more recently as implantable power sources. [5][6][7] To improve this technology, much research has been focused on engineering and modifying the cathode half of these biofuel cells. [8][9][10][11][12][13][14][15][16][17][18] One such engineered bioelectrode system, previously developed by our group, employs anthracene modified multi-walled carbon nanotubes (anth-MWCNTs) for docking of the oxidoreductase enzyme laccase to the current collector.…”

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confidence: 99%

Operational Stability Assays for Bioelectrodes for Biofuel Cells: Effect of Immobilization Matrix on Laccase Biocathode Stability

Shrier

Giroud

Rasmussen

2014

J. Electrochem. Soc.

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One of the main issues of enzymatic biofuel cells is the need to develop stable bioelectrodes. However, there is no standard method to study bioelectrode stability. In this study, laccase and anthracene modified multiwall carbon nanotubes (anth-MWCNTs) were used in conjunction with different immobilization polymers in order to increase the stability of the biocathodes. A series of stability assays were used to understand the operational stability of the biocathode in a biofuel cell environment. The immobilization matrices used in this study were tetrabutyl ammonium bromide modified Nafion (TBAB modified Nafion), octyl modified linear polyethylenimine (C 8 -LPEI), and vapor deposited tetramethyl orthosilicate (TMOS) gels. The decrease in activity of the galvanostatic and potentiostatic measurements over a 24 hour period of the TBAB modified Nafion were 4.0 ± 0.6% and 4.1 ± 0.4%; C 8 -LPEI were 0.7 ± 0.1% and 9.6 ± 0.5%; and TMOS were 4.1 ± 0.1% and 10 ± 2.0%, respectively. This data show that potentiostatic measurements provide a harsher environment for the enzyme and result in lower stability, as well as showing that the TBAB modified Nafion offers a more stabilizing immobilization strategy compared to the C 8 -LPEI or TMOS matrices. The increasing interest in producing electrical energy from renewable resources has caused the field of biofuel cells to flourish. Enzymatic biofuel cell systems are capable of producing energy from renewable fuels. Basically, enzymatic biofuel cells (EBFC) generate electricity from the oxidation of the fuel at the anode and the reduction of the oxidant at the cathode using biological catalysts (enzymes) instead of traditional metal catalysts. More detailed descriptions of such biofuel cells can be found in reviews that discuss the fundamental concepts of this technology.1,2 Applications of EBFCs range from energy sources for small electronic devices, 3 self-powered sensors 4 and more recently as implantable power sources. [5][6][7] To improve this technology, much research has been focused on engineering and modifying the cathode half of these biofuel cells. [8][9][10][11][12][13][14][15][16][17][18] One such engineered bioelectrode system, previously developed by our group, employs anthracene modified multi-walled carbon nanotubes (anth-MWCNTs) for docking of the oxidoreductase enzyme laccase to the current collector. This biocathode uses anthracene covalently modified to the ends of the multi-walled carbon nanotubes (MWCNTs) in order to favorably orient the laccase enzyme to the ends of the carbon nanotubes, since laccase has a hydrophobic binding site for anthracene and the aromatic structure allows for improved conductivity between the active site and the carbon surface. The steric orientation provides increased catalytic reduction of oxygen to water and favorable distances such that the laccase performs direct electron transfer (DET). 8In biofuel cells, DET occurs through the enzyme's ability to oxidize or reduce a substrate while transferring the necessary electrons to or fro...

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“…Curve fitting analysis was completed first on the high resolution spectra of reference compounds using the above parameters and then similar constraints were applied to mixture spectra and new peaks were added (if necessary) to obtain an optimal curve fit. Identification of peaks is based on Scienta ESCA300 database [14] and NIST Standard Reference Database [15].…”

Section: Methodsmentioning

confidence: 99%

“…[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.…”

Section: -4mentioning

confidence: 99%

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

Villarrubia

Artyushkova

Garcia

et al. 2014

J. Electrochem. Soc.

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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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Enzymatic biofuel cells designed for direct power generation from biofluids in living organisms

Cited by 229 publications

References 32 publications

An enzyme logic bioprotonic transducer

An enzyme logic bioprotonic transducer

Operational Stability Assays for Bioelectrodes for Biofuel Cells: Effect of Immobilization Matrix on Laccase Biocathode Stability

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

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Enzymatic biofuel cells designed for direct power generation from biofluids in living organisms

Cited by 229 publications

References 32 publications

An enzyme logic bioprotonic transducer

An enzyme logic bioprotonic transducer

Operational Stability Assays for Bioelectrodes for Biofuel Cells: Effect of Immobilization Matrix on Laccase Biocathode Stability

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

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