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Andrew J deMello

Publications and source records attributed to Andrew J deMello.

10 recordsLinked to original sources

A microfluidic system for evaluation of antioxidant capacity based on a peroxyoxalate chemiluminescence assay.

A microfluidic system incorporating chemiluminescence detection is reported as a new tool for measuring antioxidant capacity. The detection is based on a peroxyoxalate chemiluminescence (PO-CL) assay with 9,10-bis-(phenylethynyl)anthracene (BPEA) as the fluorescent probe and hydrogen peroxide as the oxidant. Antioxidant plugs injected into the hydrogen peroxide stream result in inhibition of the CL emission which can be quantified and correlated with antioxidant capacity. The PO-CL assay is performed in 800-microm-wide and 800-microm-deep microchannels on a poly(dimethylsiloxane) (PDMS) microchip. Controlled injection of the antioxidant plugs is performed through an injection valve. Of the plant-food based antioxidants tested, beta-carotene was found to be the most efficient hydrogen peroxide scavenger (SAHP of 3.27x10(-3) micromol-1 L), followed by alpha-tocopherol (SAHP of 2.36x10(-3) micromol-1 L) and quercetin (SAHP of 0.31x10(-3) micromol-1 L). Although the method is inherently simple and rapid, excellent analytical performance is afforded in terms of sensitivity, dynamic range, and precision, with RSD values typically below 1.5%. We expect our microfluidic devices to be used for in-the-field antioxidant capacity screening of plant-sourced food and pharmaceutical supplements.

Anthracenes↗

Integrated thin-film polymer/fullerene photodetectors for on-chip microfluidic chemiluminescence detection.

We report the use of solution-processed thin-film organic photodiodes for microscale chemiluminescence. The active layer of the photodiodes comprised a 1 : 1 blend by weight of the conjugated polymer poly(3-hexylthiophene) [P3HT] and [6,6]-phenyl-C(61)-butyric acid-methylester [PCBM]--a soluble derivative of C(60). The devices had an active area of 1 mm x 1 mm, and a broad-band response from 350 to 700 nm, with an external quantum efficiency of more than 50% between 450 and 550 nm. The photodiodes have a simple layered structure that permits facile integration with planar chip-based systems. To evaluate the suitability of the organic devices as integrated detectors for microscale chemiluminescence, a peroxyoxalate based chemiluminescence reaction (PO-CL) was monitored within a poly(dimethyl-siloxane) (PDMS) microfluidic device. Quantitation of hydrogen peroxide indicated excellent linearity and yielded a detection limit of 10 microM, comparable with previously reported results using micromachined silicon microfluidic chips with integrated silicon photodiodes. The combination of organic photodiodes with PDMS microfluidic chips offers a means of creating compact, sensitive and potentially low-cost microscale CL devices with wide-ranging applications in chemical and biological analysis and clinical diagnostics.

Dimethylpolysiloxanes↗

A one-step protocol for the chemical derivatisation of glass microfluidic devices.

A simple and robust derivatisation system for glass and silica microdevices is described. The device surface is coated in a one-step treatment with a highly cross-linked polystyrene/divinylbenzene/allylsiloxane copolymer. The surface derivatisation is highly resistant to solvents, acids, bases and oxidising or reducing agents.

Glass↗

A method for rapid reaction optimisation in continuous-flow microfluidic reactors using online Raman spectroscopic detection.

An extremely rapid tool for continuous flow synthetic process optimisation is described. A microfluidic reaction system operating in continuous flow is used in conjunction with confocal Raman microscopy to afford rapid molecule synthesis and product quantitation. Accordingly, the approach allows for rapid reaction optimisation within a continuous flow system. Specifically, the catalytic oxidation of isopropyl alcohol (IPA) to acetone using tetra-N-propylammonium perruthanate (TPAP)/N-methylmorpholine N-oxide (NMO) in a radial interdigitated micromixer is studied as a model reaction system. The composition of the reaction effluent can be determined with great facility and information relating to catalyst/co-oxidant ratios, catalyst turnovers and reaction endpoints extracted. Specifically, variation of catalyst and co-oxidant volumetric flow rates between 0 and 50 microL min(-1) is used to vary reactant concentrations, define reaction residence times and control product conversions between 0 and 100%. The rapid nature of the system allows chemical information to be gathered and utilised on a sub-minute timescale.

Journal Article↗

Thin-film polymer light emitting diodes as integrated excitation sources for microscale capillary electrophoresis.

We report the use of a thin-film polymer light emitting diode as an integrated excitation source for microfabricated capillary electrophoresis. The polyfluorene-based diode has a peak emission wavelength of 488 nm, an active area of 40 microm x 1000 microm and a thickness of similar 2 mm. The simple layer-by-layer deposition procedures used to fabricate the polymer component allow facile integration with planar chip-based systems. To demonstrate the efficacy of the approach, the polyfluorene diode is used as an excitation source for the detection of fluorescent dyes separated on-chip by electrophoresis. Using a conventional confocal detection system the integrated pLED is successfully used to detect fluorescein and 5-carboxyfluorescein at concentrations as low as 10(-6) M with a mass detection limit of 50 femtomoles. The drive voltages required to generate sufficient emission from the polymer diode device are as low as 3.7 V.

Biosensing Techniques↗

Integrated on-chip derivatization and electrophoresis for the rapid analysis of biogenic amines.

We demonstrate the monolithic integration of a chemical reactor with a capillary electrophoresis device for the rapid and sensitive analysis of biogenic amines. Fluorescein isothiocyanate (FITC) is widely employed for the analysis of amino-group containing analytes. However, the slow reaction kinetics hinders the use of this dye for on-chip labeling applications. Other alternatives are available such as o-phthaldehyde (OPA), however, the inferior photophysical properties and the UV lambdamax present difficulties when using common excitation sources leading to a disparity in sensitivity. Consequently, we present for the first time the use of dichlorotriazine fluorescein (DTAF) as a superior in situ derivatizing agent for biogenic amines in microfluidic devices. The developed microdevice employs both hydrodynamic and electroosmotic flow, facilitating the creation of a polymeric microchip to perform both precolumn derivatization and electrophoretic analysis. The favorable photophysical properties of the DTAF and its fast reaction kinetics provide detection limits down to 1 nM and total analysis times (including on-chip mixing and reaction) of <60 s. The detection limits are two orders of magnitude lower than current limits obtained with both FITC and OPA. The optimized microdevice is also employed to probe biogenic amines in real samples.

Biogenic Amines↗

In-column field-amplified sample stacking of biogenic amines on microfabricated electrophoresis devices.

A novel method for performing in-column field-amplified sample stacking (FASS) in chip-based electrophoretic systems is presented. The methodology involves the use of a narrow sample channel (NSC) injector. NSC injectors allow sample plugs to be introduced directly into the separation channel, and subsequent stacking and separation can proceed without any need for leakage control. More importantly, stacking and separation occur in a single step negating the requirement for complex channel geometries and voltage switching to control sample plugs during the stacking procedure. The chip is composed of six paralleled systems. Using the NSC injector design, the number of reservoirs in the multiplexed chip is reduced to N + 2, where N is the number of paralleled systems. This design feature radically reduces the complexity in chip structures and associated chip operation. The approach is applied to the analysis of fluorescently labelled biogenic amines affording detection at concentrations down to 20 pM.

Biogenic Monoamines↗

Solution-phase electroluminescence.

We report emissive devices exhibiting electroluminescence in the solution phase. The principle operating mechanism for these devices--direct electronic carrier injection from the electrodes into the carrier bands of the dissolved polymer--resembles that of a conventional solid-state organic light-emitting diode and is distinct from the solvent-mediated electrochemical devices recently reported by Chang et al.

Journal Article↗