Self-powered wireless carbohydrate/oxygen sensitive biodevice based on radio signal transmission

peer-reviewedHere for the first time, we detail self-contained (wireless and self-powered) biodevices with wireless signal transmission. Specifically, we demonstrate the operation of self-sustained carbohydrate and oxygen sensitive biodevices, consisting of a wireless electronic unit, radio transmitter and separate sensing bioelectrodes, supplied with electrical energy from a combined multi-enzyme fuel cell generating sufficient current at required voltage to power the electronics. A carbohydrate/oxygen enzymatic fuel cell was assembled by comparing the performance of a range of different bioelectrodes followed by selection of the most suitable, stable combination. Carbohydrates (viz. lactose for the demonstration) and oxygen were also chosen as bioanalytes, being important biomarkers, to demonstrate the operation of the self-contained biosensing device, employing enzyme-modified bioelectrodes to enable the actual sensing. A wireless electronic unit, consisting of a micropotentiostat, an energy harvesting module (voltage amplifier together with a capacitor), and a radio microchip, were designed to enable the biofuel cell to be used as a power supply for managing the sensing devices and for wireless data transmission. The electronic system used required current and voltages greater than 44 mu A and 0.57 V, respectively to operate; which the biofuel cell was capable of providing, when placed in a carbohydrate and oxygen containing buffer. In addition, a USB based receiver and computer software were employed for proof-of concept tests of the developed biodevices. Operation of bench-top prototypes was demonstrated in buffers containing different concentrations of the analytes, showcasing that the variation in response of both carbohydrate and oxygen biosensors could be monitored wirelessly in real-time as analyte concentrations in buffers were changed, using only an enzymatic fuel cell as a power supply.PUBLISHEDpeer-reviewe

Immobilization of redox enzymes on nanoporous gold electrodes: applications in biofuel cells

Nanoporous gold (NPG) electrodes were prepared by dealloying sputtered gold: silver alloys. Electrodes of different thicknesses and pore sizes areas were prepared by varying the temperature and duration of the dealloying procedure; these were then used as supports for FAD-dependent glucose dehydrogenase (GDH) (Glomorella cingulata) and bilirubin oxidase (BOx) (Myrothecium verrucaria). Glucose dehydrogenase was immobilized by drop-casting a solution of the enzyme with an osmium redox polymer together with a crosslinked polymer, whereas bilirubin oxidase was attached covalently through carbodiimide coupling to a diazonium-modified NPG electrode. The stability of the bilirubin-oxidase-modified NPG electrode was significantly improved in comparison with that of a planar gold electrode. Enzyme fuel cells were also prepared; the optimal response was obtained with a BOx-modified NPG cathode (500 nm thickness) and a GDH-modified anode (300 nm), which generated power densities of 17.5 and 7.0 mu W cm(-2) in phosphate-buffered saline and artificial serum, respectively

Immobilization of Redox Enzymes on Nanoporous Gold Electrodes: Applications in Biofuel Cells

Nanoporous gold (NPG) electrodes were prepared by dealloying sputtered gold:silver alloys. Electrodes of different thicknesses and pore sizes areas were prepared by varying the temperature and duration of the dealloying procedure; these were then used as supports for FAD‐dependent glucose dehydrogenase (GDH) (Glomorella cingulata) and bilirubin oxidase (BOx) (Myrothecium verrucaria). Glucose dehydrogenase was immobilized by drop‐casting a solution of the enzyme with an osmium redox polymer together with a crosslinked polymer, whereas bilirubin oxidase was attached covalently through carbodiimide coupling to a diazonium‐modified NPG electrode. The stability of the bilirubin‐oxidase‐modified NPG electrode was significantly improved in comparison with that of a planar gold electrode. Enzyme fuel cells were also prepared; the optimal response was obtained with a BOx‐modified NPG cathode (500 nm thickness) and a GDH‐modified anode (300 nm), which generated power densities of 17.5 and 7.0 μW cm−2 in phosphate‐buffered saline and artificial serum, respectively.This project has received funding from the European Union's Seventh Framework Programme for research, technological development and demonstration under grant agreement no. 607793 (BIOENERGY).Peer reviewe

Immobilization of redox enzymes on nanoporous gold electrodes: applications in biofuel cells

Nanoporous gold (NPG) electrodes were prepared by dealloying sputtered gold: silver alloys. Electrodes of different thicknesses and pore sizes areas were prepared by varying the temperature and duration of the dealloying procedure; these were then used as supports for FAD-dependent glucose dehydrogenase (GDH) (Glomorella cingulata) and bilirubin oxidase (BOx) (Myrothecium verrucaria). Glucose dehydrogenase was immobilized by drop-casting a solution of the enzyme with an osmium redox polymer together with a crosslinked polymer, whereas bilirubin oxidase was attached covalently through carbodiimide coupling to a diazonium-modified NPG electrode. The stability of the bilirubin-oxidase-modified NPG electrode was significantly improved in comparison with that of a planar gold electrode. Enzyme fuel cells were also prepared; the optimal response was obtained with a BOx-modified NPG cathode (500 nm thickness) and a GDH-modified anode (300 nm), which generated power densities of 17.5 and 7.0 mu W cm(-2) in phosphate-buffered saline and artificial serum, respectively

Characterization of Nanoporous Gold Electrodes for Bioelectrochemical Applications

The high surface areas of nanostructured electrodes can provide for significantly enhanced surface loadings of electroactive materials. The fabrication and characterization of nanoporous gold (np-Au) substrates as electrodes for bioelectrochemical applications is described. Robust np-Au electrodes were prepared by sputtering a gold–silver alloy onto a glass support and subsequent dealloying of the silver component. Alloy layers were prepared with either a uniform or nonuniform distribution of silver and, post dealloying, showed clear differences in morphology on characterization with scanning electron microscopy. Redox reactions under kinetic control, in particular measurement of the charge required to strip a gold oxide layer, provided the most accurate measurements of the total electrochemically addressable electrode surface area, <i>A</i>_real. Values of <i>A</i>_real up to 28 times that of the geometric electrode surface area, <i>A</i>_geo, were obtained. For diffusion-controlled reactions, overlapping diffusion zones between adjacent nanopores established limiting semi-infinite linear diffusion fields where the maximum current density was dependent on <i>A</i>_geo. The importance of measuring the surface area available for the immobilization was determined using the redox protein, <i>cyt</i> c. The area accessible to modification by a biological macromolecule, <i>A</i>_macro, such as <i>cyt</i> c was reduced by up to 40% compared to <i>A</i>_real, demonstrating that the confines of some nanopores were inaccessible to large macromolecules due to steric hindrances. Preliminary studies on the preparation of np-Au electrodes modified with osmium redox polymer hydrogels and Myrothecium verrucaria bilirubin oxidase (<i>Mv</i>BOD) as a biocathode were performed; current densities of 500 μA cm^–2 were obtained in unstirred solutions

Bench-top device test.

<p>Photographs of the set-up for the bench-top device test, showing (A) the oxygen sensitive wireless self-powered biodevice, <i>i.e.</i> an EFC (electrochemical cell containing the anodes, 1, and cathodes, 2) connected to the wireless operational unit (white box, 3) and a control device (voltmeter, 4) and (B) a computer with the developed control software and receiver (CC2530 radio highlighted with the white arrow, 5), placed roughly 4 m from the device.</p

Charge pump design.

<p>Overall scheme of the charge pump design divided into different modules connected to electronics for sensing, sampling, and wireless radio transmission of data.</p

Wireless carbohydrate sensing.

<p>Recorded signal from the carbohydrate sensitive self-contained biodevice in buffers with varying lactose concentrations.</p

Wireless oxygen sensing.

<p>Recorded signal from the self-contained biodevice for oxygen monitoring in buffers with varying oxygen concentrations.</p