Nitrogen-doped pyrolytic carbon films as highly electrochemically active electrodes.

Nitrogen-doped Pyrolytic Carbon (N-PyC) films were employed as an electrode material in electrochemical applications. PyC was grown by via non-catalysed chemical vapour deposition and subsequently functionalised via exposure to ammonia-hydrogen plasma. The electrochemical properties of the N-PyC films were investigated using the ferri/ferro-cyanide and hexaamine ruthenium(III) chloride redox probes. Exceptional electron transfer properties were observed and quantified for the N-PyC compared to the as-grown films. X-ray photoelectron spectroscopy confirmed the presence of nitrogen in edge plane graphitic configurations and the surface of the N-PyC was investigated using scanning electron microscopy and atomic force microscopy. The excellent electrochemical performance of the N-PyC, in addition to its ease of preparation, renders this material ideal for applications in electrochemical sensing.

DMF-exfoliated graphene for electrochemical NADH detection.

The electrochemical detection of NADH is of considerable interest because it is required as a cofactor in a large number of dehydrogenase-based biosensors. However, the presence of oxygenated functionalities on the electrode often causes fouling due to the adsorption of the oxidised form, NAD(+). Here we report an electroanalytical NADH sensor based on DMF-exfoliated graphene. The latter is shown to have a very low oxygen content, facilitating the exceptionally stable and sensitive detection of this important analyte.

Immobilized enzyme-single-wall carbon nanotube composites for amperometric glucose detection at a very low applied potential.

The behaviour of support electrodes modified with randomly dispersed single-wall carbon nanotube meshes containing adsorbed glucose oxidase with respect to amperometric glucose detection at a low potential is demonstrated.

The Stability Challenge on the Pathway to Low and Ultra-Low Platinum Loading for Oxygen Reduction in Fuel Cells.

We report the influence of catalyst loading on rates of platinum degradation in acidic electrolyte at room temperature. A piezoelectric printer is used to deposit spotted arrays of a commercially available catalyst comprised of Pt nanoparticles on a porous carbon support. The kinetically controlled oxygen reduction reaction (ORR) activity at different loadings is measured using an electrochemical scanning flow cell (SFC), and found to be quite stable over the range of loadings studied. This behaviour, however, contrasts sharply with rates of both transient and quasi-steady-state platinum dissolution. These are shown using downstream inductively coupled plasma mass spectrometry (ICP-MS) analytics, to increase as loading becomes lower. This dichotomy between activity and stability has direct implications for the development of improved catalyst materials, as well as for the achievement of current targets for reduced loadings of noble metals for fuel cells and other energy storage devices.

Dissolution of Platinum in the Operational Range of Fuel Cells.

One of the most important practical issues in low-temperature fuel-cell catalyst degradation is platinum dissolution. According to the literature, it initiates at 0.6-0.9 VRHE, whereas previous time- and potential-resolved inductively coupled plasma mass spectrometry (ICP-MS) experiments, however, revealed dissolution onset at only 1.05 VRHE. In this manuscript, the apparent discrepancy is addressed by investigating bulk and nanoparticulated catalysts. It is shown that, given enough time for accumulation, traces of platinum can be detected at potentials as low as 0.85 VRHE. At these low potentials, anodic dissolution is the dominant process, whereas, at more positive potentials, more platinum dissolves during the oxide reduction after accumulation. Interestingly, the potential and time dissolution dependence is similar for both types of electrode. Dissolution processes are discussed with relevance to fuel-cell operation and plausible dissolution mechanisms are considered.

Gas phase controlled deposition of high quality large-area graphene films.

A gas phase controlled graphene synthesis resembling a CVD process that does not critically depend on cooling rates is reported. The controllable catalytic CVD permits high quality large-area graphene formation with deft control over the thickness from monolayers to thick graphitic structures at temperatures as low as 750 degrees C.