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ucin1052761078.pdf (11.27 MB)
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Abstract Header
DEVELOPMENT OF A REMOTE SPECTROELECTROCHEMICAL SENSOR FOR TECHNETIUM AS PERTECHNETATE
Author Info
MONK, DAVID JAMES
Permalink:
http://rave.ohiolink.edu/etdc/view?acc_num=ucin1052761078
Abstract Details
Year and Degree
2003, PhD, University of Cincinnati, Arts and Sciences : Chemistry.
Abstract
Subsurface contamination by technetium (Tc) is of particular concern in the monitoring, characterization, and remediation of underground nuclear waste storage tanks, processing areas, and associated surroundings at the Hanford Site and other U.S. DOE sites nationwide. The concern over this radioactive element arises for two reasons. First, its most common isotope,
99
Tc, has an extremely long lifetime of 2.15 x 10
5
years. Second, it’s most common chemical form in environmental conditions, pertechnetate (TcO
4
-
), exhibits very fast migration through soils and readily presents itself to any nearby aquifer. Standard procedures of sampling and analysis in a laboratory prove to be slow and costly in the case of subsurface contamination by radioactive materials. It is highly desirable to develop sensors for these materials that possess the capability of either
in-situ
or on-site placement for continuous monitoring or immediate analysis of collected samples. These sensors need to possess adequate detection limit and selectivity, rapid response, reversibility (many measurements with one sensor), the ability to perform remotely, and ruggedness. This dissertation describes several areas of the continued work toward a sensor for
99
Tc as TcO
4
-
. Research initially focused on developing spectroelectrochemical instrumentation and a disposable sensing element, engineered to address the need to perform remote measurements. The instrument was then tested using samples containing
99
Tc, resulting in the development of ancillary equipment and techniques to address concerns associated with performing experiments on radioactive materials. In these tests, the electrochemistry of TcO
4
-
was demonstrated to be irreversible. Electrochemical reduction of TcO
4
-
on a bare or polymer modified electrode resulted in the continuous build up of technetium oxide (TcO
2
) on the elect rode surface. This TcO
2
formed in visual quantities in these films during electrochemistry, and proved to be non-ideal for spectroelectrochemical sensing. In the most recent work described, the development of metal templating techniques using complexes synthesized with rhenium (Re) was investigated as one means to circumvent this irreversibility. In an extension of the metal templating research, custom ligands were being designed which will impart structural rigidity and fluorescence to the template complexes, to facilitate selectivity and sensitivity at levels previously unprecedented for optical techniques.
Committee
DR. THOMAS RIDGWAY (Advisor)
Pages
263 p.
Keywords
spectroelectrochemistry
;
instrumentation
;
sensors
;
technetium
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Citations
MONK, D. J. (2003).
DEVELOPMENT OF A REMOTE SPECTROELECTROCHEMICAL SENSOR FOR TECHNETIUM AS PERTECHNETATE
[Doctoral dissertation, University of Cincinnati]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1052761078
APA Style (7th edition)
MONK, DAVID.
DEVELOPMENT OF A REMOTE SPECTROELECTROCHEMICAL SENSOR FOR TECHNETIUM AS PERTECHNETATE.
2003. University of Cincinnati, Doctoral dissertation.
OhioLINK Electronic Theses and Dissertations Center
, http://rave.ohiolink.edu/etdc/view?acc_num=ucin1052761078.
MLA Style (8th edition)
MONK, DAVID. "DEVELOPMENT OF A REMOTE SPECTROELECTROCHEMICAL SENSOR FOR TECHNETIUM AS PERTECHNETATE." Doctoral dissertation, University of Cincinnati, 2003. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1052761078
Chicago Manual of Style (17th edition)
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Document number:
ucin1052761078
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Copyright Info
© 2003, all rights reserved.
This open access ETD is published by University of Cincinnati and OhioLINK.