Comparison of Mobile Phone and CCD Cameras for Electrochemiluminescent Detection of Biogenic Amines.

Biogenic amines are an important and widely studied class of molecules due to their link to the physiological processes of food-related illnesses and histamine poisoning. Electrochemiluminescent (ECL) detection offers an inexpensive and portable analytical method of detection for biogenic amines when coupled with recent advancements in low-cost carbon-based electrodes and a smartphone camera. In this work, a mobile phone camera was evaluated against a piece of conventional instrumentation, the charge-coupled device, for the detection of ECL from the reaction of biogenic amines with the luminescent compound tris(2,2'-bipyridyl)ruthenium(II). Assisted by a 3D-printed light-tight housing, the mobile phone achieved limits of detection of 127, 425 and 421 µM for spermidine, putrescine, and histamine, respectively. The mobile phone's analytical figures of merit were lesser than the CCD camera but were still within the range to detect contamination. In an exploration of real-world samples, the mobile phone was able to determine the contents of amines in skim milk on par with that of a CCD camera.

Exploring carbon particle type and plasma treatment to improve electrochemical properties of stencil-printed carbon electrodes.

Stencil-printing conductive carbon inks has revolutionized the development of inexpensive, disposable and portable electrochemical sensors. However, stencil-printed carbon electrodes (SPCEs) typically suffer from poor electrochemical properties. While many surface pretreatments and modifications have been tested to improve the electrochemical activity of SPCEs, the bulk composition of the inks used for printing has been largely ignored. Recent studies of other carbon composite electrode materials show significant evidence that the conductive carbon particle component is strongly related to electrochemical performance. However, such a study has not been carried out with SPCEs. In this work, we perform a systematic characterization of SPCEs made with different carbon particle types including graphite particles, glassy carbon microparticles and carbon black. The relationship between carbon particle characteristics including particle size, particle purity, and particle morphology as well as particle mass loading on the fabrication and electrochemical properties of SPCEs is studied. SPCEs were plasma treated for surface activation and the electrochemical properties of both untreated and plasma treated SPCEs are also compared. SPCEs displayed distinct analytical utilities characterized through solvent window and double layer capacitance. Cyclic voltammetry (CV) of several standard redox probes, FcTMA+, ferri/ferrocyanide, and pAP was used to establish the effects of carbon particle type and plasma treatment on electron transfer kinetics of SPCEs. CV of the biologically relevant molecules uric acid, NADH and dopamine was employed to further illustrate the differences in sensing and fouling characteristics of SPCEs fabricated with different carbon particle types. SEM imaging revealed significant differences in the SPCE surface microstructures. This systematic study demonstrates that the electrochemical properties of SPCEs can be tuned and significantly improved through careful selection of carbon particle type and plasma cleaning with a goal toward the development of better performing electrochemical point-of-need sensors.

Disposable glassy carbon stencil printed electrodes for trace detection of cadmium and lead.

Cadmium (Cd) and lead (Pb) pollution is a significant environmental and human health concern, and methods to detect Cd and Pb on site are valuable. Stencil-printed carbon electrodes (SPCEs) are an attractive electrode material for point-of-care (POC) applications due to their low cost, ease of fabrication, disposability and portability. At present, SPCEs are exclusively formulated from graphitic carbon powder and conductive carbon ink. However, graphitic carbon SPCEs are not ideal for heavy metal sensing due to the heterogeneity of graphitic SPCE surfaces. Moreover, SPCEs typically require extensive modification to provide desirable detection limits and sensitivity at the POC, significantly increasing cost and complexity of analysis. While there are many examples of chemically modified SPCEs, the bulk SPCE composition has not been studied for heavy metal detection. Here, a glassy carbon microparticle stencil printed electrode (GC-SPE) was developed. The GC-SPEs were first characterized with SEM and cyclic voltammetry and then optimized for Cd and Pb detection with an in situ Bi-film plated. The GC-SPEs require no chemical modification or pretreatment significantly decreasing the cost and complexity of fabrication. The detection limits for Cd and Pb were estimated to be 0.46 µg L-1 and 0.55 µg L-1, respectively, which are below EPA limits for drinking water (5 µg L-1 Cd and 10 µg L-1 Pb) [1]. The reported GC-SPEs are advantageous with their low cost, ease of fabrication and use, and attractive performance. The GC-SPEs can be used for low-level metal detection at the POC as shown in the report herein.

Janus electrochemistry: Simultaneous electrochemical detection at multiple working conditions in a paper-based analytical device.

The simultaneous detection of multiple analytes from a single sample is a critical tool for the analysis of real world samples. However, this is challenging to accomplish in the field by current electroanalytical techniques, where tuning assay conditions towards a target analyte often results in poor selectivity and sensitivity for other species in the mixture. In this work, an electrochemical paper-based analytical device (ePAD) capable of performing simultaneous electrochemical experiments in different solution conditions on a single sample was developed for the first time. We refer to the system as a Janus-ePAD after the two-faced Greek god because of the ability of the device to perform electrochemistry on the same sample under differing solution conditions at the same time with a single potentiostat. In a Janus-ePAD, a sample wicks down two channels from a single inlet towards two discreet reagent zones that adjust solution conditions, such as pH, before flow termination in two electrochemical detection zones. These zones feature independent working electrodes and shared reference and counter electrodes, facilitating simultaneous detection of multiple species at each species' optimal solution condition. The device utility and applicability are demonstrated through the simultaneous detection of two biologically relevant species (norepinephrine and serotonin) and a common enzymatic assay product (p-aminophenol) at two different solution pH conditions. Janus-ePADs show great promise as an inexpensive and broadly applicable platform which can reduce the complexity and/or number of steps required in multiplexed analysis, while also operating under the optimized conditions of each species present in a mixture.

Ion release and in vitro enamel fluoride uptake associated with pit and fissure sealants containing microencapsulated remineralizing agents.

PURPOSE: To determine if pit-and-fissure sealants with microencapsulated remineralizing agents with sustained release of fluoride, calcium and phosphate ions could promote enamel fluoride uptake by demineralized tooth structure. METHODS: Sealants that contained 5 w/w% microcapsules with aqueous solutions of 5M Ca(NO3)2 or 0.8M NaF or 6.0M K2HPO4 or a mixture of all three were prepared. Ion release profiles were measured as a function of time. Enamel fluoride uptake by demineralized tooth structure was determined. RESULTS: Sustained release of fluoride, calcium and phosphate ions from a sealant was demonstrated. Fluoride uptake by demineralized enamel was significantly increased compared to a control sealant manufactured without microcapsules (P< 0.01). Bovine enamel that contained 2.2±2.1 µg F/g of enamel prior to exposure to a sealant without microcapsules had 2.3±0.5 after 90 days. Enamel exposed to sealant with 5w/% NaF microcapsules went from 3.5±3.5 µg F/g of enamel prior to exposure to 148±76 after 90 days. Enamel exposed to sealant with 2 w/w% NaF, 2 w/w% Ca(NO3)2 and 1 w/w% K2HPO4 microcapsules went from 1.7±0.7 µg F/g of enamel prior to exposure to 190±137 after 90 days. CLINICAL SIGNIFICANCE: Sealants with encapsulated remineralizing agents were capable of releasing biologically available fluoride, calcium, and phosphate ions. Incorporation of these microcapsules in pit and fissure sealants is a promising method for remineralization determined by enamel fluoride uptake measurements.

Ion release, fluoride charge of and adhesion of an orthodontic cement paste containing microcapsules.

OBJECTIVES: Dental materials capable of releasing calcium, phosphate and fluoride are of great interest for remineralization. Microencapsulated aqueous solutions of these ions in orthodontic cement demonstrate slow, sustained release by passive diffusion through a permeable membrane without the need for dissolution or etching of fillers. The potential to charge a dental material formulated with microencapsulated water with fluoride by toothbrushing with over the counter toothpaste and the effect of microcapsules on cement adhesion to enamel was determined. METHODS: Orthodontic cements that contained microcapsules with water and controls without microcapsules were brushed with over-the-counter toothpaste and fluoride release was measured. Adhesion measurements were performed loading orthodontic brackets to failure. Cements that contained microencapsulated solutions of 5.0M Ca(NO3)2, 0.8M NaF, 6.0MK2HPO4 or a mixture of all three were prepared. Ion release profiles were measured as a function of time. RESULTS: A greater fluoride charge and re-release from toothbrushing was demonstrated compared to a control with no microcapsules. Adhesion of an orthodontic cement that contained microencapsulated remineralizing agents was 8.5±2.5MPa compared to the control without microcapsules which was of 8.3±1.7MPa. Sustained release of fluoride, calcium and phosphate ions from cement formulated with microencapsulated remineralizing agents was demonstrated. CONCLUSIONS: Orthodontic cements with microcapsules show a release of bioavailable fluoride, calcium, and phosphate ions near the tooth surface while having the ability to charge with fluoride and not effect the adhesion of the material to enamel. Incorporation of microcapsules in dental materials is promising for promoting remineralization.