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Influences on Subsurface Plutonium and Americium Migration

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Influences on Subsurface Plutonium and Americium Migration. / Emerson, H.P.; Pearce, C.I.; Delegard, C.H. et al.
In: ACS Earth and Space Chemistry, Vol. 5, No. 2, 18.02.2021, p. 279-294.

Research output: Contribution to Journal/MagazineJournal articlepeer-review

Harvard

Emerson, HP, Pearce, CI, Delegard, CH, Cantrell, KJ, Snyder, MMV, Thomas, M-L, Gartman, BN, Miller, MD, Resch, CT, Heald, SM, Plymale, AE, Reilly, DD, Saslow, SA, Neilson, W, Murphy, S, Zavarin, M, Kersting, AB & Freedman, VL 2021, 'Influences on Subsurface Plutonium and Americium Migration', ACS Earth and Space Chemistry, vol. 5, no. 2, pp. 279-294. https://doi.org/10.1021/acsearthspacechem.0c00277

APA

Emerson, H. P., Pearce, C. I., Delegard, C. H., Cantrell, K. J., Snyder, M. M. V., Thomas, M.-L., Gartman, B. N., Miller, M. D., Resch, C. T., Heald, S. M., Plymale, A. E., Reilly, D. D., Saslow, S. A., Neilson, W., Murphy, S., Zavarin, M., Kersting, A. B., & Freedman, V. L. (2021). Influences on Subsurface Plutonium and Americium Migration. ACS Earth and Space Chemistry, 5(2), 279-294. https://doi.org/10.1021/acsearthspacechem.0c00277

Vancouver

Emerson HP, Pearce CI, Delegard CH, Cantrell KJ, Snyder MMV, Thomas ML et al. Influences on Subsurface Plutonium and Americium Migration. ACS Earth and Space Chemistry. 2021 Feb 18;5(2):279-294. Epub 2021 Feb 4. doi: 10.1021/acsearthspacechem.0c00277

Author

Emerson, H.P. ; Pearce, C.I. ; Delegard, C.H. et al. / Influences on Subsurface Plutonium and Americium Migration. In: ACS Earth and Space Chemistry. 2021 ; Vol. 5, No. 2. pp. 279-294.

Bibtex

@article{974ef89617da4dd9916bfb846f563685,
title = "Influences on Subsurface Plutonium and Americium Migration",
abstract = "Plutonium (Pu) has been released to the environment worldwide, including approximately 1.85 × 1015 Bq (200 kg) of Pu from process waste solutions to unconfined soil structures at the Hanford Site in Washington State. The subsurface mobility of Pu is influenced by complex interactions with sediments, groundwater, and any co-contaminants within the waste stream. Previous investigations at Hanford have shown that Pu exists as discrete PuO2 particles forming before or after disposal, as secondary solid phases formed from waste interactions with sediments as adsorbed/incorporated species, and/or as dissolved species. In this research, new evidence is presented for the existence of PuO2, PuO2-Bi2O3 composites, and particles from burnt Pu metal in near-surface sediments where Pu-laden acidic process waste was disposed to sediments. Pu and americium (Am) L3 X-ray absorption spectroscopy and density functional theory suggest that, in larger, more crystalline PuO2 particles, Am formed from radioactive decay is retained in the PuIVO2 structure as AmIV. The Pu and Am that were disposed of in an acidic waste stream have since migrated deeper into the subsurface with detection to at least 37 meters below ground surface. In contrast, Pu deposited near the ground surface from neutral pH waste is found to be homogeneously distributed and relatively immobile. Groundwater extractions performed on contaminated sediments indicate that both Pu and Am are recalcitrant, with Am being fractionally less extractable than Pu on a molar basis. These results suggest that the more mobile fraction of Am has migrated from the near-surface and may be present in the deeper sediments as a different phase than Pu. From these results, it is suggested that Pu and Am deposited from acidic wastes were initially mobile and became significantly less mobile as wastes were neutralized within the soil profile. {\textcopyright}",
keywords = "americium, autoradiography, fate and transport, Hanford Site, plutonium, X-ray absorption spectroscopy",
author = "H.P. Emerson and C.I. Pearce and C.H. Delegard and K.J. Cantrell and M.M.V. Snyder and M.-L. Thomas and B.N. Gartman and M.D. Miller and C.T. Resch and S.M. Heald and A.E. Plymale and D.D. Reilly and S.A. Saslow and W. Neilson and S. Murphy and M. Zavarin and A.B. Kersting and V.L. Freedman",
year = "2021",
month = feb,
day = "18",
doi = "10.1021/acsearthspacechem.0c00277",
language = "English",
volume = "5",
pages = "279--294",
journal = "ACS Earth and Space Chemistry",
publisher = "American Chemical Society",
number = "2",

}

RIS

TY - JOUR

T1 - Influences on Subsurface Plutonium and Americium Migration

AU - Emerson, H.P.

AU - Pearce, C.I.

AU - Delegard, C.H.

AU - Cantrell, K.J.

AU - Snyder, M.M.V.

AU - Thomas, M.-L.

AU - Gartman, B.N.

AU - Miller, M.D.

AU - Resch, C.T.

AU - Heald, S.M.

AU - Plymale, A.E.

AU - Reilly, D.D.

AU - Saslow, S.A.

AU - Neilson, W.

AU - Murphy, S.

AU - Zavarin, M.

AU - Kersting, A.B.

AU - Freedman, V.L.

PY - 2021/2/18

Y1 - 2021/2/18

N2 - Plutonium (Pu) has been released to the environment worldwide, including approximately 1.85 × 1015 Bq (200 kg) of Pu from process waste solutions to unconfined soil structures at the Hanford Site in Washington State. The subsurface mobility of Pu is influenced by complex interactions with sediments, groundwater, and any co-contaminants within the waste stream. Previous investigations at Hanford have shown that Pu exists as discrete PuO2 particles forming before or after disposal, as secondary solid phases formed from waste interactions with sediments as adsorbed/incorporated species, and/or as dissolved species. In this research, new evidence is presented for the existence of PuO2, PuO2-Bi2O3 composites, and particles from burnt Pu metal in near-surface sediments where Pu-laden acidic process waste was disposed to sediments. Pu and americium (Am) L3 X-ray absorption spectroscopy and density functional theory suggest that, in larger, more crystalline PuO2 particles, Am formed from radioactive decay is retained in the PuIVO2 structure as AmIV. The Pu and Am that were disposed of in an acidic waste stream have since migrated deeper into the subsurface with detection to at least 37 meters below ground surface. In contrast, Pu deposited near the ground surface from neutral pH waste is found to be homogeneously distributed and relatively immobile. Groundwater extractions performed on contaminated sediments indicate that both Pu and Am are recalcitrant, with Am being fractionally less extractable than Pu on a molar basis. These results suggest that the more mobile fraction of Am has migrated from the near-surface and may be present in the deeper sediments as a different phase than Pu. From these results, it is suggested that Pu and Am deposited from acidic wastes were initially mobile and became significantly less mobile as wastes were neutralized within the soil profile. ©

AB - Plutonium (Pu) has been released to the environment worldwide, including approximately 1.85 × 1015 Bq (200 kg) of Pu from process waste solutions to unconfined soil structures at the Hanford Site in Washington State. The subsurface mobility of Pu is influenced by complex interactions with sediments, groundwater, and any co-contaminants within the waste stream. Previous investigations at Hanford have shown that Pu exists as discrete PuO2 particles forming before or after disposal, as secondary solid phases formed from waste interactions with sediments as adsorbed/incorporated species, and/or as dissolved species. In this research, new evidence is presented for the existence of PuO2, PuO2-Bi2O3 composites, and particles from burnt Pu metal in near-surface sediments where Pu-laden acidic process waste was disposed to sediments. Pu and americium (Am) L3 X-ray absorption spectroscopy and density functional theory suggest that, in larger, more crystalline PuO2 particles, Am formed from radioactive decay is retained in the PuIVO2 structure as AmIV. The Pu and Am that were disposed of in an acidic waste stream have since migrated deeper into the subsurface with detection to at least 37 meters below ground surface. In contrast, Pu deposited near the ground surface from neutral pH waste is found to be homogeneously distributed and relatively immobile. Groundwater extractions performed on contaminated sediments indicate that both Pu and Am are recalcitrant, with Am being fractionally less extractable than Pu on a molar basis. These results suggest that the more mobile fraction of Am has migrated from the near-surface and may be present in the deeper sediments as a different phase than Pu. From these results, it is suggested that Pu and Am deposited from acidic wastes were initially mobile and became significantly less mobile as wastes were neutralized within the soil profile. ©

KW - americium

KW - autoradiography

KW - fate and transport

KW - Hanford Site

KW - plutonium

KW - X-ray absorption spectroscopy

U2 - 10.1021/acsearthspacechem.0c00277

DO - 10.1021/acsearthspacechem.0c00277

M3 - Journal article

VL - 5

SP - 279

EP - 294

JO - ACS Earth and Space Chemistry

JF - ACS Earth and Space Chemistry

IS - 2

ER -