Co-reporter:Ross D. Milton, Fabien Giroud, Alfred E. Thumser, Shelley D. Minteer and Robert C. T. Slade
Chemical Communications 2014 vol. 50(Issue 1) pp:94-96
Publication Date(Web):29 Oct 2013
DOI:10.1039/C3CC47689H
Mediator-less, direct electro-catalytic reduction of oxygen to water by bilirubin oxidase (Myrothecium sp.) was obtained on anthracene-modified, multi-walled carbon nanotubes. H2O2 was found to significantly and irreversibly affect the electro-catalytic activity of bilirubin oxidase, whereas similar electrodes comprised of laccase (Trametes versicolor) were reversibly inhibited.
Co-reporter:Ross D. Milton, Fabien Giroud, Alfred E. Thumser, Shelley D. Minteer and Robert C. T. Slade
Physical Chemistry Chemical Physics 2013 vol. 15(Issue 44) pp:19371-19379
Publication Date(Web):08 Oct 2013
DOI:10.1039/C3CP53351D
Hydrogen peroxide production by glucose oxidase (GOx) and its negative effect on laccase performance have been studied. Simultaneously, FAD-dependent glucose dehydrogenase (FAD-GDH), an O2-insensitive enzyme, has been evaluated as a substitute. Experiments focused on determining the effect of the side reaction of GOx between its natural electron acceptor O2 (consumed) and hydrogen peroxide (produced) in the electrolyte. Firstly, oxygen consumption was investigated by both GOx and FAD-GDH in the presence of substrate. Relatively high electrocatalytic currents were obtained with both enzymes. O2 consumption was observed with immobilized GOx only, whilst O2 concentration remained stable for the FAD-GDH. Dissolved oxygen depletion effects on laccase electrode performances were investigated with both an oxidizing and a reducing electrode immersed in a single compartment. In the presence of glucose, dramatic decreases in cathodic currents were recorded when laccase electrodes were combined with a GOx-based electrode only. Furthermore, it appeared that the major loss of performance of the cathode was due to the increase of H2O2 concentration in the bulk solution induced laccase inhibition. 24 h stability experiments suggest that the use of O2-insensitive FAD-GDH as to obviate in situ peroxide production by GOx is effective. Open-circuit potentials of 0.66 ± 0.03 V and power densities of 122.2 ± 5.8 μW cm−2 were observed for FAD-GDH/laccase biofuel cells.
Co-reporter:Ross D. Milton, Jessica Baur, John R. Varcoe, Alfred E. Thumser and Robert C. T. Slade
Physical Chemistry Chemical Physics 2012 vol. 14(Issue 27) pp:9582-9585
Publication Date(Web):08 Jun 2012
DOI:10.1039/C2CP41651D
A glucose oxidase (GOd) bioelectrode exhibiting high performance, direct electron transfer (DET) has been prepared. Unprecedented redox peak current densities of 1 mA cm−2 were observed alongside a clear electrochemical response to glucose. This system shows potential as a low cost, high performance enzymatic bioelectrode.
Co-reporter:Xuee Wu, Feng Zhao, John R. Varcoe, Alfred E. Thumser, Claudio Avignone-Rossa, Robert C.T. Slade
Bioelectrochemistry 2009 Volume 77(Issue 1) pp:64-68
Publication Date(Web):November 2009
DOI:10.1016/j.bioelechem.2009.05.008
Conductive cellulose-multiwalled carbon nanotube (MWCNT) matrix with a porous structure and good biocompatibility has been prepared using a room temperature ionic liquid (1-ethyl-3-methylimidazolium acetate) as solvent. Glucose oxidase (GOx) was encapsulated in this matrix and thereby immobilized on a glassy carbon surface. The direct electron transfer and electrocatalysis of the encapsulated GOx has been investigated using cyclic voltammetry and chronoamperometry. The GOx exhibited a pair of stable, well defined and nearly symmetric reversible redox peaks. The experimental results also demonstrate that the immobilized GOx retains its biocatalytic activity toward the oxidation of glucose and therefore can be employed in a glucose biosensor. The results show that the bioelectrode modified by the cellulose-MWCNT matrix has potential for use in biosensors and other bioelectronics devices.
Co-reporter:Xuee Wu, Feng Zhao, John R. Varcoe, Alfred E. Thumser, Claudio Avignone-Rossa, Robert C.T. Slade
Biosensors and Bioelectronics 2009 Volume 25(Issue 2) pp:326-331
Publication Date(Web):15 October 2009
DOI:10.1016/j.bios.2009.07.011
The construction and characterization of a one-compartment fructose/air biological fuel cell (BFC) based on direct electron transfer is reported. The BFC employs bilirubin oxidase and d-fructose dehydrogenase adsorbed on a cellulose–multiwall carbon nanotube (MWCNT) matrix, reconstituted with an ionic liquid, as the biocathode and the bioanode for oxygen reduction and fructose oxidation reactions, respectively. The performance of the bioelectrode was investigated by chronoamperometric and cyclic voltammetric techniques in a standard three-electrode cell, and the polarization and long-term stability of the BFC was tested by potentiostatic discharge. An open circuit voltage of 663 mV and a maximum power density of 126 μW cm−2 were obtained in buffer at pH 5.0. Using this regenerated cellulose–MWCNT matrix as the immobilization platform, this BFC has shown a relatively high performance and long-term stability compared with previous studies.
Co-reporter:Feng Zhao, Nelli Rahunen, John R. Varcoe, Alexander J. Roberts, Claudio Avignone-Rossa, Alfred E. Thumser, Robert C.T. Slade
Biosensors and Bioelectronics 2009 Volume 24(Issue 7) pp:1931-1936
Publication Date(Web):15 March 2009
DOI:10.1016/j.bios.2008.09.030
A microbial fuel cell (MFC) has been developed for removal of sulfur-based pollutants and can be used for simultaneous wastewater treatment and electricity generation. This fuel cell uses an activated carbon cloth + carbon fibre veil composite anode, air-breathing dual cathodes and the sulfate-reducing species Desulfovibrio desulfuricans. 1.16 g dm−3 sulfite and 0.97 g dm−3 thiosulfate were removed from the wastewater at 22 °C, representing sulfite and thiosulfate removal conversions of 91% and 86%, respectively. The anode potential was controlled by the concentration of sulfide in the compartment. The performance of the cathode assembly was affected by the concentration of protons in the cation-exchanging ionomer with which the electrocatalyst is co-bound at the three-phase (air, catalyst and support) boundary.
Co-reporter:Feng Zhao, Nelli Rahunen, John R. Varcoe, Amreesh Chandra, Claudio Avignone-Rossa, Alfred E. Thumser and Robert C. T. Slade
Environmental Science & Technology 2008 Volume 42(Issue 13) pp:4971-4976
Publication Date(Web):June 3, 2008
DOI:10.1021/es8003766
By employing the sulfate-reducing bacterium Desulfovibrio desulfuricans we demonstrate the possibility of electricity generation in a microbial fuel cell (MFC) with concomitant sulfate removal. This approach is based on an in situ anodic oxidative depletion of sulfide produced by D. desulfuricans. Three different electrode materials, graphite foil (GF), carbon fiber veil (CFV), and high surface area activated carbon cloth (ACC), were evaluated for sulfide electrochemical oxidation. In comparison to CFV and GF electrodes, ACC was a superior material for sulfide adsorption and oxidation and showed significant potential for harvesting energy from sulfate-rich solutions in the form of electricity. Sulfate (3.03 g dm−3) was removed from a bacterial suspension, which represented 99% removal. A maximum power density of 0.51 mW cm−2 (normalized to geometric electrode area) was obtained with a one-chamber, air-breathing cathode and continuous flow MFC operated in batch mode at 22 °C.
Co-reporter:Amreesh Chandra, Alexander J. Roberts, Robert C.T. Slade
Solid State Communications 2008 Volume 147(3–4) pp:83-87
Publication Date(Web):July 2008
DOI:10.1016/j.ssc.2008.05.012
Synthesis and characterization of the tailored nanostructured vanadium molybdenum oxide (V xMo1−xOy) system is reported. TEM studies clearly show the formation of varying morphologies at vanadium and molybdenum rich ends. The effect of these differing morphologies on the surface area is presented. It is shown that compositions with x<0.40x<0.40 have electronic conductivity and a reduced contribution of ionic conductivity. Possible explanations for this observation are discussed. The VMO system shows promise for application as electrode materials in fields such as supercapacitors.
Co-reporter:Timothy N. Danks, Robert C. T. Slade and John R Varcoe
Journal of Materials Chemistry A 2003 vol. 13(Issue 4) pp:712-721
Publication Date(Web):26 Feb 2003
DOI:10.1039/B212164F
Vinylbenzyl chloride was grafted onto PVDF and FEP polymer films using radiation-grafting methodology. Subsequent reaction with trimethylamine and ion-exchange with potassium hydroxide yields alkaline anion-exchange membranes that are capable of conducting hydroxide ions; such membranes may be suitable for use in low temperature direct methanol fuel cells for portable devices. The PVDF based materials underwent an undesirable degradation and were found to be less suitable for this class of membrane. FEP-based materials exhibited superior structural stability, conductivities up to 0.02 S cm−1 at room temperature, and good retention of ion-exchange capacities when treated in water at 60 °C.
Co-reporter:A.M White, R.C.T Slade
Synthetic Metals 2003 Volume 139(Issue 1) pp:123-131
Publication Date(Web):8 August 2003
DOI:10.1016/S0379-6779(03)00039-0
Redox-composited polymers have been chemically fabricated via vapour transport of monomer and evaluated for potential use as electrodes within a solid-state supercapacitor. An in depth evaluation of membrane electrode assemblies (MEAs, capacitor devices without a casing) was carried out. MEAs were made by hot pressing of the electrodes onto a proton-conducting solid electrolyte membrane in a ‘sandwich’ configuration. The highest specific capacitance, specific energy and specific power values depend on the method of cell-to-cell comparison: the highest values per unit mass of MEA were with electrodes incorporating polypyrrole doped with 10-molybdo-2-vanadophosphoric acid and stored wet (specific capacitance, specific energy and specific power values: 7 F g−1, 0.5 W h kg−1 and 3.3 W kg−1); the highest values per unit mass of active polymer were for polypyrrole doped with 12-molybdosilicic acid (33.4 F g−1, 2.12 W h g−1 and 3.7 W kg−1).
Co-reporter:Timothy N. Danks, Robert C. T. Slade and John R. Varcoe
Journal of Materials Chemistry A 2002 vol. 12(Issue 12) pp:3371-3373
Publication Date(Web):26 Sep 2002
DOI:10.1039/B208627A
Vinylbenzyl chloride has been radiation grafted onto both PVDF and FEP fluoropolymer films; subsequent amination and ion-exchange to give the hydroxide ion forms yield anion-exchange membranes suitable for use in low temperature direct methanol fuel cells for portable applications.
Co-reporter:Amreesh Chandra, Alexander J. Roberts, Robert C.T. Slade
Solid State Communications (July 2008) Volume 147(3–4) pp:83-87
Publication Date(Web):1 July 2008
DOI:10.1016/j.ssc.2008.05.012
Synthesis and characterization of the tailored nanostructured vanadium molybdenum oxide (V xMo1−xOy) system is reported. TEM studies clearly show the formation of varying morphologies at vanadium and molybdenum rich ends. The effect of these differing morphologies on the surface area is presented. It is shown that compositions with x<0.40 have electronic conductivity and a reduced contribution of ionic conductivity. Possible explanations for this observation are discussed. The VMO system shows promise for application as electrode materials in fields such as supercapacitors.
Co-reporter:Ross D. Milton, Fabien Giroud, Alfred E. Thumser, Shelley D. Minteer and Robert C. T. Slade
Chemical Communications 2014 - vol. 50(Issue 1) pp:NaN96-96
Publication Date(Web):2013/10/29
DOI:10.1039/C3CC47689H
Mediator-less, direct electro-catalytic reduction of oxygen to water by bilirubin oxidase (Myrothecium sp.) was obtained on anthracene-modified, multi-walled carbon nanotubes. H2O2 was found to significantly and irreversibly affect the electro-catalytic activity of bilirubin oxidase, whereas similar electrodes comprised of laccase (Trametes versicolor) were reversibly inhibited.
Co-reporter:Ross D. Milton, Fabien Giroud, Alfred E. Thumser, Shelley D. Minteer and Robert C. T. Slade
Physical Chemistry Chemical Physics 2013 - vol. 15(Issue 44) pp:NaN19379-19379
Publication Date(Web):2013/10/08
DOI:10.1039/C3CP53351D
Hydrogen peroxide production by glucose oxidase (GOx) and its negative effect on laccase performance have been studied. Simultaneously, FAD-dependent glucose dehydrogenase (FAD-GDH), an O2-insensitive enzyme, has been evaluated as a substitute. Experiments focused on determining the effect of the side reaction of GOx between its natural electron acceptor O2 (consumed) and hydrogen peroxide (produced) in the electrolyte. Firstly, oxygen consumption was investigated by both GOx and FAD-GDH in the presence of substrate. Relatively high electrocatalytic currents were obtained with both enzymes. O2 consumption was observed with immobilized GOx only, whilst O2 concentration remained stable for the FAD-GDH. Dissolved oxygen depletion effects on laccase electrode performances were investigated with both an oxidizing and a reducing electrode immersed in a single compartment. In the presence of glucose, dramatic decreases in cathodic currents were recorded when laccase electrodes were combined with a GOx-based electrode only. Furthermore, it appeared that the major loss of performance of the cathode was due to the increase of H2O2 concentration in the bulk solution induced laccase inhibition. 24 h stability experiments suggest that the use of O2-insensitive FAD-GDH as to obviate in situ peroxide production by GOx is effective. Open-circuit potentials of 0.66 ± 0.03 V and power densities of 122.2 ± 5.8 μW cm−2 were observed for FAD-GDH/laccase biofuel cells.
Co-reporter:Ross D. Milton, Jessica Baur, John R. Varcoe, Alfred E. Thumser and Robert C. T. Slade
Physical Chemistry Chemical Physics 2012 - vol. 14(Issue 27) pp:NaN9585-9585
Publication Date(Web):2012/06/08
DOI:10.1039/C2CP41651D
A glucose oxidase (GOd) bioelectrode exhibiting high performance, direct electron transfer (DET) has been prepared. Unprecedented redox peak current densities of 1 mA cm−2 were observed alongside a clear electrochemical response to glucose. This system shows potential as a low cost, high performance enzymatic bioelectrode.