Nagasaki sediments reveal that long-term fate of plutonium is controlled by select organic matter moieties

Lin, Peng; Xu, Chen; Kaplan, Daniel I.; Chen, Hongmei; Yeager, Chris M.; Wang, Xing; Sun, Luni; Schwehr, Kathleen A.; Yamazaki, Hideo; Saito‐Kokubu, Yoko; Hatcher, Patrick G.; Santschi, Peter H.

doi:10.1016/j.scitotenv.2019.04.375

Cited by 13 publications

(19 citation statements)

References 42 publications

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“…NOM is commonly found associated with Fe(III) oxides in surface water and groundwater, − and their interactions can control the speciation and transport of Pu depending on colloidal properties of NOM–Fe. ,, For example, under oxic conditions, citric acid, humic acid (HA), and fulvic acid (FA) were found to increase Pu adsorption onto Fe(III) oxides at low pH by forming ternary Pu(IV)–NOM–Fe(III) oxide complexes. , Furthermore, these NOM–Fe colloids have been shown to serve as geochemical nanocarriers, either facilitating or reducing the overall transport of Pu in surface water depending on their particle transport properties. ,− Chen et al studied the mobility of Pu in soil-groundwater suspensions and found that Pu(IV) formed mobile colloids with NOM, while Pu(V) sorbed more readily to prevailing solid clay mineral surfaces . During seasonal mixing events and associated transient redox conditions, transport of NOM–Fe(II) colloids from groundwater to surface water can result in the formation of NOM–Fe(III) oxide colloids and generation of hydroxyl radicals. , …”

Section: Introductionmentioning

confidence: 99%

“…34 NOM is commonly found associated with Fe(III) oxides in surface water and groundwater, 35−37 colloidal properties of NOM−Fe. 12,38,39 For example, under oxic conditions, citric acid, humic acid (HA), and fulvic acid (FA) were found to increase Pu adsorption onto Fe(III) oxides at low pH by forming ternary Pu(IV)−NOM−Fe(III) oxide complexes. 12,38 Furthermore, these NOM−Fe colloids have been shown to serve as geochemical nanocarriers, either facilitating or reducing the overall transport of Pu in surface water depending on their particle transport properties.…”

Section: Introductionmentioning

confidence: 99%

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Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Pan

Jiao

Kersting

et al. 2021

Environ. Sci. Technol.

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Plutonium (Pu) redox and complexation processes in the presence of natural organic matter and associated iron can impact the fate and transport of Pu in the environment. We studied the fate of Pu(IV) in the presence of humic acid (HA) and Fe(II) upon reaction with H2O2 that may be generated by photochemical and other reactions. A portion of Pu(IV) was oxidized to Pu(V/VI), which is primarily ascribed to the generation of reactive intermediates from the oxidation of Fe(II) and Fe(II)–HA complexes by H2O2. The kinetics of Pu(IV) oxidation is pH-dependent and can be described by a model that incorporates Pu redox kinetics with published HA-modified Fenton reaction kinetics. At pH 3.5, the presence of HA slowed Pu(IV) oxidation, while at pH 6, HA accelerated Pu(IV) oxidation in the first several hours followed by a reverse process where the oxidized Pu(V/VI) was reduced back to Pu(IV). Analysis of Pu-associated particle size suggests that Pu oxidation state is a major driver in its complexation with HA and formation of colloids and heteroaggregates. Our results revealed the H2O2-driven oxidation of Pu(IV)–HA–Fe(II) colloids with implications to the transient mobilization of Pu(V/VI) in organic-rich redox transition zones.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Pan

Jiao

Kersting

et al. 2021

Environ. Sci. Technol.

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“…The influence of organic substances on plutonium migration has been discussed in other works (Zhao et al, 2011 ; Santschi et al, 2017 ; Lin et al, 2019 ). In the NNSS vadose zone, the water that was collected in a tunnel system had plutonium predominantly as an aqueous species, which was not bound with colloids (Zhao et al, 2011 ).…”

Section: Plutoniummentioning

confidence: 88%

“…Another example of the influence of organic matter on the behavior of Pu was found in the Nishiyama reservoir (Nagasaki, Japan) (Lin et al, 2019 ). Nagasaki is the only city in the world where a Pu bomb was exploded.…”

Section: Plutoniummentioning

confidence: 99%

Speciation of Uranium and Plutonium From Nuclear Legacy Sites to the Environment: A Mini Review

2020

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The row of 15 chemical elements from Ac to Lr with atomic numbers from 89 to 103 are known as the actinides, which are all radioactive. Among them, uranium and plutonium are the most important as they are used in the nuclear fuel cycle and nuclear weapon production. Since the beginning of national nuclear programs and nuclear tests, many radioactively contaminated nuclear legacy sites, have been formed. This mini review covers the latest experimental, modeling, and case studies of plutonium and uranium migration in the environment, including the speciation of these elements and the chemical reactions that control their migration pathways.

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“…The sequential extraction method (Figure ) of 239+240 Pu was used to separate soil into different fractions for the study of the dominant factors, which hindered 239+240 Pu migration in soil. ,,,, NH 2 OHCl was used to reduce/dissolve the Fe/Mn-oxides fraction, as well as Pu in the NOM Fe/Mn‑oxide fraction was obtained after separating the supernatant solutions. H 2 O 2 was used to oxidize other organic matter fractions.…”

Section: Methodsmentioning

confidence: 99%

Sequential Extraction of ^239+240Pu and the Vertical Distribution of ^239+240Pu, ¹³⁷Cs, and Heavy Metals in Chang-Bai Mountains’ Grassland Soil

Guan

Wang

Jing

et al. 2022

ACS Earth Space Chem.

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To establish a 239+240 Pu, 137 Cs, and heavy metal reference soil site in Northeast China, three grassland soil cores were collected from the Lao-Ye-Ling Mountain, which is a branch of the Chang-Bai Mountains. The activities were in the range of 0.041−2.752 mBq/g for 239+240 Pu and in the range of 0.2−57.6 mBq/g for 137 Cs. The 240 Pu/ 239 Pu atomic ratios were 0.161−0.186, showing that 239+240 Pu in the study area originated from the global fallout. Also, 239+240 Pu, 137 Cs, and excess 210 Pb were enriched in the surface soil. The convective−dispersion equation model provided the lower apparent dispersion coefficients (D) and apparent convection velocities (v) for both 239+240 Pu and 137 Cs. The soil erosion rate in this study area was estimated by an erosion model, which was lower than that in the other area of Northeast China. 239+240 Pu in the different soil fractions was analyzed by a sequential extraction method, and the result showed that 239+240 Pu was mainly adsorbed by Fe/Mn oxides and their associated organic matter (NOM Fe/Mn-oxides fraction). Except for Fe, all other heavy metals from the anthropogenic source were enriched in the surface soil. The pollution level of heavy metals in this study area was lower. In general, the alpine grassland soil of the Lao-Ye-Ling Mountain can be used as a reference soil site to study environmental pollution and soil erosion and provided some reference baselines for future multidisciplinary studies in Northeast Asia.

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Nagasaki sediments reveal that long-term fate of plutonium is controlled by select organic matter moieties

Cited by 13 publications

References 42 publications

Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Speciation of Uranium and Plutonium From Nuclear Legacy Sites to the Environment: A Mini Review

Sequential Extraction of ^239+240Pu and the Vertical Distribution of ^239+240Pu, ¹³⁷Cs, and Heavy Metals in Chang-Bai Mountains’ Grassland Soil

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Nagasaki sediments reveal that long-term fate of plutonium is controlled by select organic matter moieties

Cited by 13 publications

References 42 publications

Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Plutonium Redox Transformation in the Presence of Iron, Organic Matter, and Hydroxyl Radicals: Kinetics and Mechanistic Insights

Speciation of Uranium and Plutonium From Nuclear Legacy Sites to the Environment: A Mini Review

Sequential Extraction of 239+240Pu and the Vertical Distribution of 239+240Pu, 137Cs, and Heavy Metals in Chang-Bai Mountains’ Grassland Soil

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Product

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Sequential Extraction of ^239+240Pu and the Vertical Distribution of ^239+240Pu, ¹³⁷Cs, and Heavy Metals in Chang-Bai Mountains’ Grassland Soil