Development and application of mass spectrometric techniques for ultra-trace determination of 236U in environmental samples-A review

Bu, Wenting; Zheng, Jian; Ketterer, Michael E.; Hu, Sheng; Uchida, Shunsuke; Wang, Xiaolin

doi:10.1016/j.aca.2017.09.029

Cited by 37 publications

(25 citation statements)

References 161 publications

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“…Unlike Pu, U is also naturally présent in the environment with two primordial isotopes (238U and 235U) and one radiogenic isotope (234U) originating from the 238U-decay. Moreover, these isotopes are relatively abundant in soils and sediment, with the U concentration being 6 to 9 orders of magnitude higher than that of Pu (Bu et al, 2017). On the contrary, the 236U isotope has an extremely low abundance in natural-occurring U present in environmental samples (<10-13).…”

Section: Pu and U Source Term Signaturesmentioning

confidence: 98%

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

et al. 2019

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Section: Pu and U Source Term Signaturesmentioning

confidence: 98%

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

et al. 2019

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“…The mean 236 U/ 238 U isotope ratio level in Earth crust is 10 -14 -10 -13 . 1 However, anthropogenic 236 U was globally deposited on Earth surface through atmospheric nuclear weapon tests leading to a characteristic 236 U/ 238 U isotope ratio of 10 -8 -10 -9 in most environmental samples. [2][3][4][5][6][7][8][9] In addition, anthropogenic 236 U was locally released into the environment in the vicinity of nuclear fuel reprocessing facilities or after nuclear power plant accidents, with 236 U/ 238 U isotope ratio signatures above 10 -9 .…”

Section: Introductionmentioning

confidence: 99%

“…[10][11][12][13][14][15] In uranium ore, high uranium concentrations associated with high neutron flux lead to a higher production of 236 U with 236 U/ 238 U isotope ratios with a typical signature of about 10 -10 . 1,[16][17][18][19][20][21][22][23] In the case of Uores the main sources of neutrons are: (i) (α, n) reactions, with light elements and (ii) spontaneous and neutron-induced fission of 238 U and 235 U respectively. 17 This high isotopic contrast between the sources makes 236 U/ 238 U isotope ratios a relevant tracer for uranium source identification in the environment.…”

Section: Introductionmentioning

confidence: 99%

Pushing Limits of ICP–MS/MS for the Determination of Ultralow ²³⁶U/²³⁸U Isotope Ratios

et al. 2020

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Determination of uranium isotope ratios is of great expedience for assessing its origin in environmental samples. In particular, the 236 U/ 238 U isotope ratio provides a powerful tool to discriminate between the different sources of uranium (uranium ore, geochemical background and uranium from anthropogenic activities). However, in the environment, this ratio is typically below 10 -8 . This low abundance of 236 U and the presence in large excess of major isotopes (mainly 238 U and 235 U) complicates the accurate detection of 236 U signal by mass spectrometry and thus highly sensitive analytical instruments providing high abundance sensitivity are required. This work pushes the limits of triple quadrupole-based ICP-MS technology for accurate detection of 236 U/ 238 U isotope ratios down to 10 -10 , which is so far mainly achievable by AMS. Coupled with an efficient desolvating module, N 2 O was used as the reaction gas in the collision reaction cell of the ICP-MS/MS. This configuration allows a significant decrease of the uranium polyatomic interferences ( 235 UH + ions) and an accurate determination of low 236 U/ 238 U isotope ratios. This new methodology was successfully validated through measurements of certified reference material from 10 -7 to 10 -9 and then through comparisons with AMS measurement results for ratios down to 10 -10 . This is the first time that 236 U/ 238 U isotope ratios as low as 10 -10 were determined by ICP-MS/MS. The possibility of measuring low 236 U/ 238 U isotope ratios can offer a large variety of geochemical applications in particular for the determination of uranium sources in the environment. ASSOCIATED CONTENT Supporting InformationDemonstration of Eq. 1 and Eq. 2. and a figure on the influence of the 235 UH + interference on the measurement of 236 U/ 238 U isotope ratio for a given hydride formation rate.

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“…Even though a small amount (about 35 kg in total) of 236 U is produced naturally in the Earth's surface environments, 236 U is (by mass) the largest secondary product created in nuclear reactors, estimated totally to be an order of 10 6 kg 1 . 236 U is a sensitive tracer of deliberate or accidental leakage from the nuclear fuel/waste cycle [2][3][4][5] . The known sources of reactor 236 U, i.e., deliberate releases from the two European reprocessing plants at La Hague, France (LH) and Sella eld, UK (SF) since 1950s, can be traced throughout the North Atlantic and the Arctic water currents 6 .…”

Section: Introductionmentioning

confidence: 99%

“…The known sources of reactor 236 U, i.e., deliberate releases from the two European reprocessing plants at La Hague, France (LH) and Sella eld, UK (SF) since 1950s, can be traced throughout the North Atlantic and the Arctic water currents 6 . Emissions from other known sources of reactor 236 U, e.g., the Spring eld nuclear facility and the Fukushima accident, are negligible 5,7 .…”

Section: Introductionmentioning

confidence: 99%

A previously unknown source of reactor radionuclides in the Baltic Sea, identified by 233, 236, 238U and 127, 129I multi-fingerprinting

Qiao¹,

Zhang²,

Steier³

et al. 2020

Preprint

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We present the first application of multi-isotopic fingerprints (i.e., 236U/238U, 233U/236U, 236U/129I and 129I/127I) for the discovery of unrevealed radioactive sources. Our data indicate that, besides the reactor signature from the two European reprocessing plants and global fallout signature, there must be a previously undiscovered additional reactor 236U source in the Baltic Sea. This reactor 236U may come from unreported discharges from nuclear research facilities in Sweden, or it may come from accidental leakage from disposal of spent nuclear fuel on the Baltic seafloor, either reported or unreported. Such leakage would indicate potential problems with the safety of seafloor disposal, and may be accompanied by leakage of other radionuclides. The results demonstrate the high sensitivity of the multi-isotopic tracer systems, especially the newly accessible 233U/236U signature, to distinguish environmental emissions of unrevealed historical or present radioactive releases for nuclear safeguard and emergency preparedness, as well as tracing environmental processes from the releasing sites.

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Development and application of mass spectrometric techniques for ultra-trace determination of 236U in environmental samples-A review

Cited by 37 publications

References 161 publications

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

Pushing Limits of ICP–MS/MS for the Determination of Ultralow ²³⁶U/²³⁸U Isotope Ratios

A previously unknown source of reactor radionuclides in the Baltic Sea, identified by 233, 236, 238U and 127, 129I multi-fingerprinting

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Development and application of mass spectrometric techniques for ultra-trace determination of 236U in environmental samples-A review

Cited by 37 publications

References 161 publications

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

Pushing Limits of ICP–MS/MS for the Determination of Ultralow 236U/238U Isotope Ratios

A previously unknown source of reactor radionuclides in the Baltic Sea, identified by 233, 236, 238U and 127, 129I multi-fingerprinting

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Pushing Limits of ICP–MS/MS for the Determination of Ultralow ²³⁶U/²³⁸U Isotope Ratios