Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry

Michael E. Ketterer, Bridgette R. Watson, Gerald Matisoff, Christopher G. Wilson

Research output: Contribution to journalArticle

42 Citations (Scopus)

Abstract

Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu. and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into ∼2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 μL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 μg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in ∼6 h of instrumental measurement time, are in agreement with a γ spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 ± 0.02 and 47.8 ± 0.8 Bq/kg, respectively; inventories were 108 ± 2 Bq/m2 239+240Pu and 2710 ± 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.

Original languageEnglish (US)
Pages (from-to)1307-1311
Number of pages5
JournalEnvironmental Science and Technology
Volume36
Issue number6
DOIs
StatePublished - Mar 15 2002

Fingerprint

Inductively coupled plasma mass spectrometry
Sediments
mass spectrometry
plasma
fallout
sediment
sediment core
chronology
radionuclide
Fallout
anion
Atoms
Ion exchangers
isotope
Time measurement
Radioisotopes
Isotopes
Pneumatics
Anions
Negative ions

ASJC Scopus subject areas

  • Environmental Engineering
  • Environmental Science(all)
  • Environmental Chemistry

Cite this

Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry. / Ketterer, Michael E.; Watson, Bridgette R.; Matisoff, Gerald; Wilson, Christopher G.

In: Environmental Science and Technology, Vol. 36, No. 6, 15.03.2002, p. 1307-1311.

Research output: Contribution to journalArticle

@article{f9e333c3cb3b407eab635457c75befb1,
title = "Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry",
abstract = "Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu. and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into ∼2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 μL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 μg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in ∼6 h of instrumental measurement time, are in agreement with a γ spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 ± 0.02 and 47.8 ± 0.8 Bq/kg, respectively; inventories were 108 ± 2 Bq/m2 239+240Pu and 2710 ± 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.",
author = "Ketterer, {Michael E.} and Watson, {Bridgette R.} and Gerald Matisoff and Wilson, {Christopher G.}",
year = "2002",
month = "3",
day = "15",
doi = "10.1021/es010826g",
language = "English (US)",
volume = "36",
pages = "1307--1311",
journal = "Environmental Science & Technology",
issn = "0013-936X",
publisher = "American Chemical Society",
number = "6",

}

TY - JOUR

T1 - Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry

AU - Ketterer, Michael E.

AU - Watson, Bridgette R.

AU - Matisoff, Gerald

AU - Wilson, Christopher G.

PY - 2002/3/15

Y1 - 2002/3/15

N2 - Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu. and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into ∼2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 μL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 μg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in ∼6 h of instrumental measurement time, are in agreement with a γ spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 ± 0.02 and 47.8 ± 0.8 Bq/kg, respectively; inventories were 108 ± 2 Bq/m2 239+240Pu and 2710 ± 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.

AB - Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu. and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into ∼2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 μL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 μg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in ∼6 h of instrumental measurement time, are in agreement with a γ spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 ± 0.02 and 47.8 ± 0.8 Bq/kg, respectively; inventories were 108 ± 2 Bq/m2 239+240Pu and 2710 ± 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.

UR - http://www.scopus.com/inward/record.url?scp=0037086198&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0037086198&partnerID=8YFLogxK

U2 - 10.1021/es010826g

DO - 10.1021/es010826g

M3 - Article

VL - 36

SP - 1307

EP - 1311

JO - Environmental Science & Technology

JF - Environmental Science & Technology

SN - 0013-936X

IS - 6

ER -