Publikationsrepositorium - Helmholtz-Zentrum Dresden-Rossendorf

Our research aims at a better understanding of fundamental processes defining transport and accumulation of radiotoxic elements such as U, Np, Pu, Am, Cm, as well as Tc and Se. This requires knowledge of their mobility in the environment and of their (radio)ecological behavior. The results will help to develop biochemically and radiochemically founded risk assessment schemes, remediation procedures in areas affected by uranium mining, and help to assess the long-term safety of final disposal sites for nuclear waste in geologic formations.
Therefore, we apply solution- and solid-state NMR to various simple and complex systems. Occasionally, lanthanide ions, Ln(III), are used as non-radioactive, isoelectronic analogs for trivalent actinides, An(III). Radionuclide complexation by small molecules is studied for, e.g., citrate [1,2], glutathione (GSH/GSSG) [3,4], as well as 2-phosphonobutane-1,2,4,-tricarbox-ylate (PBTC) [5] and nitrilotriacetate (NTA) [6]. Selenium and (organo)borates were subject of NMR studies, too [7–9]. Comprehensive kinetic and thermodynamic studies were performed for water addition to PQQ, a redox cofactor in Ln(III)-dependent alcohol dehydrogenases [10]. Indicator molecules excreted from carrot cells or fungi upon treatment with uranium were identified also by NMR [11,12]. Furthermore, the bulk structure as well as the interaction of organics (e.g., gluconate, PBTC) and/or radionuclides with calcium (aluminate) silicate hydrate (C (A )S H) phases related to cementitious materials critical for nuclear waste disposal infrastructures were characterized by 13C, 31P, 27Al, and 29Si MAS NMR [13,14].

Literature:

[1] J. Kretzschmar et al., Chem. Commun. 2020, 56, 13133. [2] J. Kretzschmar et al., Inorg. Chem. 2021, 60, 7998. [3] J. Kretzschmar et al., Chem. Commun. 2018, 54, 8697. [4] J. Kretzschmar et al., Inorg. Chem. 2020, 59, 4244. [5] J. Kretzschmar et al., Molecules 2022, 27, 4067. [6] S. Friedrich et al., Molecules 2023, submitted. [7] J. Kretzschmar et al., Dalton Trans. 2015, 44, 10508. [8] J. Schott et al., Dalton Trans. 2014, 43, 11516. [9] J. Schott et al., Dalton Trans. 2015, 44, 11095. [10] N. Al Danaf et al., Phys. Chem. Chem. Phys., 2022, 24, 15397. [11] J. Jessat et al., J. Hazard. Mater. 2022, 439, 129520. [12] A. Wollenberg et al., J. Hazard. Mater. 2021, 411, 125068. [13] S. Dettmann et al., Front. Nucl. Eng. 2023, 2, 1124856. [14] K. Schmeide et al., in preparation.