Europium(III) Meets Etidronic Acid (HEDP): A Coordination Study Combining Spectroscopic, Spectrometric, and Quantum Chemical Methods

Author:

Heller Anne12ORCID,Senwitz Christian12,Foerstendorf Harald3ORCID,Tsushima Satoru34ORCID,Holtmann Linus5ORCID,Drobot Björn3ORCID,Kretzschmar Jerome3ORCID

Affiliation:

1. Chair of Radiochemistry/Radioecology, Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01062 Dresden, Germany

2. Central Radionuclide Laboratory, Radiation Protection Office, Technische Universität Dresden, 01062 Dresden, Germany

3. Institute of Resource Ecology, Helmholtz-Zentrum Dresden-Rossendorf, 01328 Dresden, Germany

4. International Research Frontiers Initiative (IRFI), Institute of Innovative Research, Tokyo Institute of Technology, Tokyo 152-8550, Japan

5. Institute of Radioecology and Radiation Protection, Leibniz Universität Hannover, 30419 Hannover, Germany

Abstract

Etidronic acid (1-Hydroxyethylidene-1,1-diphosphonic acid, HEDP, H4L) is a proposed decorporation agent for U(VI). This paper studied its complex formation with Eu(III), an inactive analog of trivalent actinides, over a wide pH range, at varying metal-to-ligand ratios (M:L) and total concentrations. Combining spectroscopic, spectrometric, and quantum chemical methods, five distinct Eu(III)−HEDP complexes were found, four of which were characterized. The readily soluble EuH2L+ and Eu(H2L)2− species with log β values of 23.7 ± 0.1 and 45.1 ± 0.9 are formed at acidic pH. At near-neutral pH, EuHL0s forms with a log β of ~23.6 and, additionally, a most probably polynuclear complex. The readily dissolved EuL− species with a log β of ~11.2 is formed at alkaline pH. A six-membered chelate ring is the key motif in all solution structures. The equilibrium between the Eu(III)–HEDP species is influenced by several parameters, i.e., pH, M:L, total Eu(III) and HEDP concentrations, and time. Overall, the present work sheds light on the very complex speciation in the HEDP–Eu(III) system and indicates that, for risk assessment of potential decorporation scenarios, side reactions of HEDP with trivalent actinides and lanthanides should also be taken into account.

Funder

German Federal Ministry of Education and Research

German Federal Ministry for the Environment, Nature Conversation, Nuclear Safety and Consumer Protection

Publisher

MDPI AG

Subject

Chemistry (miscellaneous),Analytical Chemistry,Organic Chemistry,Physical and Theoretical Chemistry,Molecular Medicine,Drug Discovery,Pharmaceutical Science

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