Impact of electron charge transfer and pH on the transformation of uranium-organic complexes

GEOC 175

Gary P. Halada and Charlotte Eng. Department of Materials Science and Engineering; and the Center for Environmental Molecular Science, Stony Brook University, Stony Brook, NY 11794-2275
The stability of uranium-organic complexes is extremely important in development of environmental remediation technologies and in understanding the transport and fate of contaminants in the environment. The stability of the complexes is affected by electron transfer reactions caused by bacterial activity and by redox reactions with other compounds in soil, groundwater and environmental corrosion products. Changes in pH, and hence the oxidizing or reducing character of the local environment, also have profound effects on uranium-organic complexes. An excellent way to understand the stability and bioavailability of such complexes is with electrochemical techniques, such as cyclic voltametry and potentiodynamic analysis. Though these techniques provide information on kinetics of electron transfer and reduction of complexes, they provide no information on the structure of the products formed, and, hence, interpretation of the data is extremely difficult. Through a unique in situ combination of electrochemical analysis and Raman spectroscopy with quantum mechanical molecular modeling using Density Functional Theory, the redox-driven transformation of uranium-organic complexes, primarily involving aromatic structures, is studied.