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Inorganic materials for pertechnetate detection and management


EMSL Project ID
47928

Abstract

One of the DOE-EM current challenges is to meet regulatory requirements for near term technetium (Tc) disposal due to excess Tc in DOE waste streams. Design of novel Tc separation and immobilization technologies requires detailed knowledge of Tc speciation, partitioning, retention, and transport in DOE flow sheets or within groundwater and soils. This in turn necessitates availability of reliable in situ measuring capability able to discriminate between Tc species in different oxidation state. In an effort to address the need for a selective detection and monitoring of pertechnetate (TcO4-) and lower valent Tc species in ground water and tank waste solutions, we propose to develop an economic solid-state colorimetric sensor. It is based on a square-planar transition metal sensor material promising for rapid in situ detection of TcO4- without cumbersome instrumentation or highly involving and time-consuming laboratory analysis. Our preliminary experimental results demonstrated that the proposed Pt sensing materials selectively uptake TcO4- resulting in changes of their structure and physical properties and thus generating unique colorimetric/luminescent response. In the similar system but based on the different Pt complex, ClO4- was detected at 0.1 ppb concentration in the presence of several interfering anions including chloride, bromide, carbonate, sulfate, phosphate, and others. We hypothesize that similar complex compounds possessing analogous molecular structure can be used for the design of novel inorganic sequestration agents highly selective for TcO4-. The applied approach can be generalized for the selective detection of other anions.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
Status
Closed

Team

Principal Investigator

Tatiana Levitskaia
Institution
Pacific Northwest National Laboratory

Team Members

Leigh Lin
Institution
Defense Nuclear Facilities Safety Board

Mary Leonard
Institution
Pacific Northwest National Laboratory

William Connick
Institution
University of Cincinnati

Sayandev Chatterjee
Institution
Pacific Northwest National Laboratory

Amity Andersen
Institution
Environmental Molecular Sciences Laboratory

Niranjan Govind
Institution
Pacific Northwest National Laboratory

Related Publications

Chatterjee S, AE Norton, MK Edwards, JM Peterson, D taylor, SA Bryan, A Andersen, N Govind, TE Albrecht-Schmitt, W Connick, and TG Levitskaia. 2015. "Highly Selective Colorimetric and Luminescence Response of a Square-Planar Platinum(II) Terpyridyl Complex to Aqueous TcO4?." Inorganic Chemistry 54(20):9914-9923. doi:10.1021/acs.inorgchem.5b01664
Chatterjee S., M.S. Fujimoto, N.L. Canfield, M.R. Elmore, D.W. Olson, E.C. Buck, and M.A. Conroy, et al. 2019. "An Electrochemical Technique for Controlled Dissolution of Zirconium Based Components of Light Water Reactors." RSC Advances 9, no. 4:1869-1881. PNNL-SA-140123. doi:10.1039/C8RA08693A
Levitskaia TG, S Chatterjee, N Pence, J Romero, T Varga, MH Engelhard, Y Du, L Kovarik, BW Arey, ME Bowden, and ED Walter. 2016. "Inorganic Tin Aluminophosphate Nanocomposite for Reductive Separation of Pertechnetate." Environmental Science: Nano 3(2):1003-1013. doi:10.1039/C6EN00130K