Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Deblonde, Gauthier J.-P.; Morrison, Keith; Mattocks, Joseph A.; Cotruvo, Joseph A.; Zavarin, Mavrik; Kersting, Annie B.

doi:10.1021/acs.est.3c06033

Title: Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Journal Article · 27 October 2023 · Environmental Science and Technology

DOI: https://doi.org/10.1021/acs.est.3c06033 · OSTI ID:2274879

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Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate; Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute
Pennsylvania State University, University Park, PA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute

Minor actinides are major contributors to the long-term radiotoxicity of nuclear fuels and other radioactive wastes. Here in this context, understanding their interactions with natural chelators and minerals is key to evaluating their transport behavior in the environment. The lanmodulin family of metalloproteins is produced by ubiquitous bacteria and Methylorubrum extorquens lanmodulin (LanM) was recently identified as one of nature’s most selective chelators for trivalent f-elements. Herein, we investigated the behavior of neptunium, americium, and curium in the presence of LanM, carbonate ions, and common minerals (calcite, montmorillonite, quartz, and kaolinite). We show that LanM’s aqueous complexes with Am(III) and Cm(III) remain stable in carbonate-bicarbonate solutions. Furthermore, the sorption of Am(III) to these minerals is strongly impacted by LanM, while Np(V) sorption is not. With calcite, even a submicromolar concentration of LanM leads to a significant reduction in the Am(III) distribution coefficient (K_d, from >10⁴ to ~10² mL/g at pH 8.5), rendering it even more mobile than Np(V). Thus, LanM-type chelators can potentially increase the mobility of trivalent actinides and lanthanide fission products under environmentally relevant conditions. Monitoring biological chelators, including metalloproteins, and their biogenerators should therefore be considered during the evaluation of radioactive waste repository sites and the risk assessment of contaminated sites.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344; SC0021007

OSTI ID:: 2274879

Report Number(s):: LLNL--JRNL-852053; 1077894

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 49 Vol. 57; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Enhanced rare-earth separation with a metal-sensitive lanmodulin dimer Mattocks, Joseph A.; Jung, Jonathan J.; Lin, Chi-Yun Nature, Vol. 618, Issue 7963 https://doi.org/10.1038/s41586-023-05945-5	journal	May 2023
Sorption of Cm(III) and Eu(III) onto clay minerals under saline conditions: Batch adsorption, laser-fluorescence spectroscopy and modeling Schnurr, Andreas; Marsac, Rémi; Rabung, Thomas Geochimica et Cosmochimica Acta, Vol. 151 https://doi.org/10.1016/j.gca.2014.11.011	journal	February 2015
Plutonium Co-precipitation with Calcite Balboni, Enrica; Smith, Kurt F.; Moreau, Liane M. ACS Earth and Space Chemistry, Vol. 5, Issue 12 https://doi.org/10.1021/acsearthspacechem.1c00181	journal	November 2021
Americium Runde, Wolfgang H.; Schulz, Wallace W. The Chemistry of the Actinide and Transactinide Elements https://doi.org/10.1007/1-4020-3598-5_8	book	January 2007
The Carbonate Complexation of the Am(III) Ion Meinrath, G.; Kim, J. I. ract, Vol. 52-53, Issue 1 https://doi.org/10.1524/ract.1991.5253.1.29	journal	January 1991
Uptake of Cm(III) and Eu(III) by Calcium Silicate Hydrates: A Solution Chemistry and Time-Resolved Laser Fluorescence Spectroscopy Study Tits, Jan; Stumpf, Thorsten; Rabung, Thomas Environmental Science & Technology, Vol. 37, Issue 16 https://doi.org/10.1021/es030020b	journal	August 2003
The Role of Transferrin in Actinide(IV) Uptake: Comparison with Iron(III) Jeanson, Aurélie; Ferrand, M.; Funke, Harald Chemistry - A European Journal, Vol. 16, Issue 4 https://doi.org/10.1002/chem.200901209	journal	January 2010
Fate of actinides in the presence of humic substances under conditions relevant to nuclear waste disposal Moulin, Valerie; Moulin, Christophe Applied Geochemistry, Vol. 10, Issue 5 https://doi.org/10.1016/0883-2927(95)00029-1	journal	September 1995
Use of rare‐earth elements in the phyllosphere colonizer Methylobacterium extorquens PA1 Ochsner, Andrea M.; Hemmerle, Lucas; Vonderach, Thomas Molecular Microbiology, Vol. 111, Issue 5 https://doi.org/10.1111/mmi.14208	journal	February 2019
Determination of affinities of lanthanide-binding proteins using chelator-buffered titrations Mattocks, Joseph A.; Tirsch, Jonathan L.; Cotruvo, Jr., Joseph A. Methods in Enzymology https://doi.org/10.1016/bs.mie.2021.01.044	book	January 2021
Neptunium and Plutonium Solubilities in a Yucca Mountain Groundwater Efurd, D. Wes; Runde, Wolfgang; Banar, Joe C. Environmental Science & Technology, Vol. 32, Issue 24 https://doi.org/10.1021/es980591h	journal	December 1998
Plutonium Oxidation and Subsequent Reduction by Mn(IV) Minerals in Yucca Mountain Tuff Powell, Brian A.; Duff, Martine C.; Kaplan, Daniel I. Environmental Science & Technology, Vol. 40, Issue 11 https://doi.org/10.1021/es052353+	journal	May 2006
Uranium Uptake by Hectorite and Montmorillonite: A Solution Chemistry and Polarized EXAFS Study Schlegel, Michel L.; Descostes, Michael Environmental Science & Technology, Vol. 43, Issue 22 https://doi.org/10.1021/es902001k	journal	October 2009
Incorporation of Np(V) and U(VI) in carbonate and sulfate minerals crystallized from aqueous solution Balboni, Enrica; Morrison, Jessica M.; Wang, Zheming Geochimica et Cosmochimica Acta, Vol. 151 https://doi.org/10.1016/j.gca.2014.10.027	journal	February 2015
A Catalytic Role of XoxF1 as La3+-Dependent Methanol Dehydrogenase in Methylobacterium extorquens Strain AM1 Nakagawa, Tomoyuki; Mitsui, Ryoji; Tani, Akio PLoS ONE, Vol. 7, Issue 11 https://doi.org/10.1371/journal.pone.0050480	journal	November 2012

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