Impact of Natural Organic Matter on Plutonium Vadose Zone Migration from an NH4Pu(V)O2CO3(s) Source

Melody Maloubier; Hilary Emerson; Kathryn Peruski; Annie B. Kersting; Mavrik Zavarin; Philip M. Almond; Daniel I. Kaplan; Brian A. Powell

doi:10.1021/acs.est.9b05651

Impact of Natural Organic Matter on Plutonium Vadose Zone Migration from an NH₄Pu(V)O₂CO₃(s) Source

Melody Maloubier, Hilary Emerson, Kathryn Peruski, Annie B. Kersting, Mavrik Zavarin, Philip M. Almond, Daniel I. Kaplan, Brian A. Powell

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

We investigated the influence of natural organic matter (NOM) on the behavior of Pu(V) in the vadose zone through a combination of the field lysimeter and laboratory studies. Well-defined solid sources of NH₄Pu(V)O₂CO₃(s) were placed in two 5-L lysimeters containing NOM-amended soil collected from the Savannah River Site (SRS) or unamended vadose zone soil and exposed to 3 years of natural South Carolina, USA, meteorological conditions. Lysimeter soil cores were removed from the field, used in desorption experiments, and characterized using wet chemistry methods and X-ray absorption spectroscopy. For both lysimeters, Pu migrated slowly with the majority (>95%) remaining within 2 cm of the source. However, without the NOM amendment, Pu was transported significantly farther than in the presence of NOM. Downward Pu migration appears to be influenced by the initial source oxidation state and composition. These Pu(V) sources exhibited significantly greater migration than previous studies using Pu(IV) or Pu(III) sources. However, batch laboratory experiments demonstrated that Pu(V) is reduced by the lysimeter soil in the order of hours, indicating that downward migration of Pu may be due to cycling between Pu(V) and Pu(IV). Under the conditions of these experiments, NOM appeared to both enhance reduction of the Pu(V) source as well as Pu sorption to soils. This indicates that NOM will tend to have a stabilizing effect on Pu migration under SRS vadose zone field conditions.

Original language	English
Pages (from-to)	2688-2697
Number of pages	10
Journal	Environmental Science and Technology
Volume	54
Issue number	5
DOIs	https://doi.org/10.1021/acs.est.9b05651
State	Published - Mar 3 2020
Externally published	Yes

Funding

This research is funded by the Office of Biological and Environmental Research of the U.S. Department of Energy as part of the Subsurface Biogeochemical Research Program under Work Proposal Number SCW1053, Subsurface Biogeochemistry of Actinides. SRNL personnel also received support through contract DE-AC09-08SR22470 with the DOE. XAS experiments were conducted at the Stanford Synchrotron Radiation Laboratory (Beamline 11.2), which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. We thank Dr. Dai (LLNL) for TEM analysis.

Funders	Funder number
U.S. Department of Energy	DE-AC09-08SR22470, SCW1053
Office of Science
Basic Energy Sciences	DE-AC02-76SF00515
Biological and Environmental Research

Access to Document

10.1021/acs.est.9b05651

Cite this

@article{f76555fe82be49c0bfb31df7bff75227,

title = "Impact of Natural Organic Matter on Plutonium Vadose Zone Migration from an NH4Pu(V)O2CO3(s) Source",

abstract = "We investigated the influence of natural organic matter (NOM) on the behavior of Pu(V) in the vadose zone through a combination of the field lysimeter and laboratory studies. Well-defined solid sources of NH4Pu(V)O2CO3(s) were placed in two 5-L lysimeters containing NOM-amended soil collected from the Savannah River Site (SRS) or unamended vadose zone soil and exposed to 3 years of natural South Carolina, USA, meteorological conditions. Lysimeter soil cores were removed from the field, used in desorption experiments, and characterized using wet chemistry methods and X-ray absorption spectroscopy. For both lysimeters, Pu migrated slowly with the majority (>95%) remaining within 2 cm of the source. However, without the NOM amendment, Pu was transported significantly farther than in the presence of NOM. Downward Pu migration appears to be influenced by the initial source oxidation state and composition. These Pu(V) sources exhibited significantly greater migration than previous studies using Pu(IV) or Pu(III) sources. However, batch laboratory experiments demonstrated that Pu(V) is reduced by the lysimeter soil in the order of hours, indicating that downward migration of Pu may be due to cycling between Pu(V) and Pu(IV). Under the conditions of these experiments, NOM appeared to both enhance reduction of the Pu(V) source as well as Pu sorption to soils. This indicates that NOM will tend to have a stabilizing effect on Pu migration under SRS vadose zone field conditions.",

author = "Melody Maloubier and Hilary Emerson and Kathryn Peruski and Kersting, {Annie B.} and Mavrik Zavarin and Almond, {Philip M.} and Kaplan, {Daniel I.} and Powell, {Brian A.}",

note = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = mar,

day = "3",

doi = "10.1021/acs.est.9b05651",

language = "English",

volume = "54",

pages = "2688--2697",

journal = "Environmental Science and Technology",

issn = "0013-936X",

publisher = "American Chemical Society",

number = "5",

}

TY - JOUR

T1 - Impact of Natural Organic Matter on Plutonium Vadose Zone Migration from an NH4Pu(V)O2CO3(s) Source

AU - Maloubier, Melody

AU - Emerson, Hilary

AU - Peruski, Kathryn

AU - Kersting, Annie B.

AU - Zavarin, Mavrik

AU - Almond, Philip M.

AU - Kaplan, Daniel I.

AU - Powell, Brian A.

PY - 2020/3/3

Y1 - 2020/3/3

N2 - We investigated the influence of natural organic matter (NOM) on the behavior of Pu(V) in the vadose zone through a combination of the field lysimeter and laboratory studies. Well-defined solid sources of NH4Pu(V)O2CO3(s) were placed in two 5-L lysimeters containing NOM-amended soil collected from the Savannah River Site (SRS) or unamended vadose zone soil and exposed to 3 years of natural South Carolina, USA, meteorological conditions. Lysimeter soil cores were removed from the field, used in desorption experiments, and characterized using wet chemistry methods and X-ray absorption spectroscopy. For both lysimeters, Pu migrated slowly with the majority (>95%) remaining within 2 cm of the source. However, without the NOM amendment, Pu was transported significantly farther than in the presence of NOM. Downward Pu migration appears to be influenced by the initial source oxidation state and composition. These Pu(V) sources exhibited significantly greater migration than previous studies using Pu(IV) or Pu(III) sources. However, batch laboratory experiments demonstrated that Pu(V) is reduced by the lysimeter soil in the order of hours, indicating that downward migration of Pu may be due to cycling between Pu(V) and Pu(IV). Under the conditions of these experiments, NOM appeared to both enhance reduction of the Pu(V) source as well as Pu sorption to soils. This indicates that NOM will tend to have a stabilizing effect on Pu migration under SRS vadose zone field conditions.

AB - We investigated the influence of natural organic matter (NOM) on the behavior of Pu(V) in the vadose zone through a combination of the field lysimeter and laboratory studies. Well-defined solid sources of NH4Pu(V)O2CO3(s) were placed in two 5-L lysimeters containing NOM-amended soil collected from the Savannah River Site (SRS) or unamended vadose zone soil and exposed to 3 years of natural South Carolina, USA, meteorological conditions. Lysimeter soil cores were removed from the field, used in desorption experiments, and characterized using wet chemistry methods and X-ray absorption spectroscopy. For both lysimeters, Pu migrated slowly with the majority (>95%) remaining within 2 cm of the source. However, without the NOM amendment, Pu was transported significantly farther than in the presence of NOM. Downward Pu migration appears to be influenced by the initial source oxidation state and composition. These Pu(V) sources exhibited significantly greater migration than previous studies using Pu(IV) or Pu(III) sources. However, batch laboratory experiments demonstrated that Pu(V) is reduced by the lysimeter soil in the order of hours, indicating that downward migration of Pu may be due to cycling between Pu(V) and Pu(IV). Under the conditions of these experiments, NOM appeared to both enhance reduction of the Pu(V) source as well as Pu sorption to soils. This indicates that NOM will tend to have a stabilizing effect on Pu migration under SRS vadose zone field conditions.

UR - http://www.scopus.com/inward/record.url?scp=85081129341&partnerID=8YFLogxK

U2 - 10.1021/acs.est.9b05651

DO - 10.1021/acs.est.9b05651

M3 - Article

C2 - 31942795

AN - SCOPUS:85081129341

SN - 0013-936X

VL - 54

SP - 2688

EP - 2697

JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 5

ER -

Impact of Natural Organic Matter on Plutonium Vadose Zone Migration from an NH₄Pu(V)O₂CO₃(s) Source

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this