Designing a Spectroelectrochemical Sensor for Pertechnetate Applicable to Hanford and Other DOE Sites
EMSL Project ID
39193
Abstract
The general aim of our work currently funded by DOE (formerly by EMSP) is the design andimplementation of a new sensor technology that offers unprecedented levels of specificity needed for
analysis of the complex chemical mixtures found at DOE sites nationwide. This project involves a very
successful collaboration between scientists at the University of Cincinnati (UC) and several at the Pacific
Northwest National Laboratory (PNNL) and the Environmental Molecular Sciences Laboratory (EMSL).
The goal of the work described in this proposal is the continued development of a sensor for 99Tc that is
applicable to characterizing and monitoring the vadose zone and associated ground water. The single
focus of this proposal is pertechnetate, TcO4-, which is considered to be the dominant species in the
vadose zone and ground water. The sensor will have the capability for on-site monitoring, either by
immersion in subsurface water for continuous monitoring or for the immediate analysis of collected
samples. The project will build on the substantial progress of a well-established UC-PNNL collaboration
which provides the wide range of expertise needed for success: spectroscopy, electrochemistry, device
fabrication, thin film technology, synthetic inorganic chemistry, experience with Tc, and facilities for
handling radioactive isotopes. The sensor will consist of an innovative fluorescence-based
spectroelectrochemical configuration that we have developed under our EMSP grants: a waveguide with
an optically transparent electrode that is coated with a thin chemically-selective film. It is now absolutely
clear from our previous work that the fluorescence spectroelectrochemical sensor can reach limits of
detection of at least 10-12 M given even a low-to-moderate quantum yield fluorescent material. We find
this result very exciting since the limit of detection for an analogous Tc-based fluorescent species would
need to be about 10-10 M to reach regulatory limits.
Project Details
Project type
Exploratory Research
Start Date
2010-03-17
End Date
2011-03-20
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Chatterjee S, AS Del Negro, MK Edwards, B Twamley, JA Krause, and SA Bryan. 2010. "trans-K3[TcO2(CN)4]." Acta Crystallographica. Section E 66(8):i61 - i62. doi:10.1107/S1600536810028205
Chatterjee S, AS Del Negro, MK Edwards, SA Bryan, N Kaval, N Pantelic, LK Morris, WR Heineman, and CJ Seliskar. 2011. "Luminescence-Based Spectroelectrochemical Sensor for [Tc(dmpe)3]2+/+ (dmpe = 1,2-bis(dimethylphosphino)ethane) within a Charge-Selective Polymer Film." Analytical Chemistry 83(5):1766-1722. doi:10.1021/ac1030368
Chatterjee S, AS Del Negro, Z Wang, MK Edwards, SE Hightower, JA Krause, B Twamley, BP Sullivan, C Reber, C Reber, WR Heineman, CJ Seliskar, and SA Bryan. 2011. "Electronic and Molecular Structures of trans-Dioxotechnetium(V) Polypyridyl Complexes in Solid State." PNNL-SA-77269, Pacific Northwest National Laboratory, Richland, WA. [Unpublished]
Chatterjee S, SA Bryan, CJ Seliskar, and WR Heineman. 2013. "Three-Component Spectroelectrochemical Sensor Module for the Detection of Pertechnetate (TcO4-)." Reviews in Analytical Chemistry 32(3):209-224. doi:10.1515/revac-2013-0001