Spectroelectrochemical Sensors: New Polymer Films for Improved Sensitivity
The selectivity of an optical sensor can be improved by combining optical detection with electrochemical oxidation or reduction of the target analyte to change its spectral properties. The changing signal can distinguish the analyte from interferences with similar spectral properties that would otherwise interfere. The analyte is detected by measuring the intensity of the electrochemically modulated signal. In one form this spectroelectrochemical sensor consists of an optically transparent electrode (OTE) coated with a film that preconcentrates the target analyte. The OTE functions as an optical waveguide for attenuated total reflectance (ATR) spectroscopy, which detects the analyte by absorption. Sensitivity relies in part on a large change in molar absorptivity between the two oxidation states used for electrochemical modulation of the optical signal. A critical part of the sensor is the ion selective film. It should preconcentrate the analyte and exclude some interferences. At the same time the film must not interfere with the electrochemistry or the optical detection. Therefore, since the debut of the sensor’s concept one major focus of our group has been developing appropriate films for different analytes. Here we report the development of a series of quaternized poly(vinylpyridine)-co-styrene (QPVP-co-S) anion exchange films for use in spectroelectrochemical sensors to enable sensitive detection of target anionic analytes in complex samples. The films were either 10% or 20% styrene and were prepared with varying degrees of quaternized pyridine groups, up to 70%. Films were characterized with respect to thickness with spectroscopic ellipsometry, degree of quaternization with FTIR, and electrochemically and spectroelectrochemically using the anions ferrocyanide and pertechnetate.
- Research Organization:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1345463
- Report Number(s):
- PNNL-SA-105075; 24491a; KP1504010
- Country of Publication:
- United States
- Language:
- English
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