Single rhenium atoms on nanomagnetite: Probing the recharge process that controls the fate of rhenium in the environment
Understanding the redox transitions that control rhenium geochemistry is central to paleoredox and geochronology studies, as well as predicting the fate of chemically similar hazardous oxyanions in the environment such as pertechnetate. However, detailed mechanistic information regarding rhenium redox transitions in anoxic systems is scarce. Here, we performed a comprehensive laboratory study of rhenium redox transitions on variably oxidized magnetite nanoparticle surfaces. Through high-end spectroscopic and microscopic tools, we propose an abiotic transition pathway in which aqueous iron(II) ions in the presence of pure or preoxidized magnetite serve as an electron source to reduce rhenium(VII) to individual rhenium(IV) atoms or small polynuclear species on nanoparticle surfaces. Notably, iron(II) ions recharged preoxidized magnetite nanoparticles exhibit a maghemite core and a magnetite shell, challenging the traditional core-shell magnetite-maghemite model. This study provides a fundamental understanding of redox processes governing rhenium fate and transport in the environment and enables an improved basis for predicting its speciation in geochemical systems.
Authors
- Rong-Rong Ding (ORCID: https://orcid.org/0000-0001-8210-6172)
- Alexandre Gloter (ORCID: https://orcid.org/0000-0002-4813-3799)
- Elke Arenholz (ORCID: https://orcid.org/0000-0001-8152-6773)
- Yang Mu (ORCID: https://orcid.org/0000-0001-7338-7398)
- Carolina Guida (ORCID: https://orcid.org/0000-0002-3181-7860)
- Andreas C. Scheinost (ORCID: https://orcid.org/0000-0002-6608-5428)
- Laurent Charlet (ORCID: https://orcid.org/0000-0003-3669-7316)
- Kristina O. Kvashnina (ORCID: https://orcid.org/0000-0003-4447-4542)
- Alejandro Fernández-Martı́nez (ORCID: https://orcid.org/0000-0001-5073-9629)
- Carolyn I. Pearce (ORCID: https://orcid.org/0000-0003-3098-1615)
- Jean−Marc Grenèche (ORCID: https://orcid.org/0000-0001-7309-8633)
- Kevin M. Rosso (ORCID: https://orcid.org/0000-0002-8474-7720)
- Kaifeng Wang (ORCID: https://orcid.org/0000-0002-5076-8304)
Institutions
- University of Science and Technology of China (CN)
- Centre National de la Recherche Scientifique (FR)
- Pacific Northwest National Laboratory (US)
- Central Michigan University (US)
- Université Paris-Saclay (FR)
- Laboratoire de physique des Solides (FR)
- Geological Survey of Denmark and Greenland (DK)
- European Synchrotron Radiation Facility (FR)
- Universidad Nacional de Colombia (CO)
- Institut des Sciences de la Terre (FR)
- CAS Key Laboratory of Urban Pollutant Conversion (CN)
- Institut des Molécules et Matériaux du Mans (FR)
- Université Gustave Eiffel (FR)
- Institut de Recherche pour le Développement (FR)
- Université Savoie Mont Blanc (FR)
- Université Grenoble Alpes (FR)
Publication Details
- Journal
- Science Advances
- Published
- 2025-05-16
- DOI
- https://doi.org/10.1126/sciadv.adq3650
- Citations
- 6
- Primary Topic
- Advanced Nanomaterials in Catalysis
- Type
- article
- Field-Weighted Citation Impact
- 3.11