Vertical distribution of <Superscript>210</Superscript>Pb and <Superscript>226</Superscript>Ra and their activity ratio in marine sediment core of the East Malaysia coastal waters

Marine sediment cores were collected from two stations at East Malaysia coastal waters on June 2004. Activity concentrations of ²¹⁰Pb in sediment core were ranged from 11 Bqkg⁻¹ to 84 Bqkg⁻¹ dry wt. for SR 01 and 4 Bqkg⁻¹ to 66 Bqkg⁻¹ dry wt. for SB 03. Meanwhile, activity concentrations of ²²⁶Ra in sediment core were varied significantly depending on the sampling location of SR 01 and SB 03 with ranged 17–26 Bqkg⁻¹ dry wt. and 8–11 Bqkg⁻¹ dry wt., respectively. The activity ratios of ²¹⁰Pb/²²⁶Ra were no significantly different at all sampling stations with an average of 1.78. Refer to the entire results; the activities of ²¹⁰Pb and ²²⁶Ra were higher at station SR 01 than station SB 03, but contrast with ratio of ²¹⁰Pb/²²⁶Ra. The reasons of different ²¹⁰Pb and ²²⁶Ra activity concentration and distribution of their ratios were strictly related to their half lives, environment origin, potential sources and behavior.     

Vertical inventories and fluxes of <Superscript>210</Superscript>Pb, <Superscript>228</Superscript>Ra and <Superscript>226</Superscript>Ra at southern South China Sea and Malacca Straits

Inventories and fluxes of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were determined in sediment cores collected at nine stations covering of the southern South China Sea and Malacca Straits with the thickness of water column between 42 and 83 m depth. The inventories of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were calculated range from 0.15–2.55 Bq cm⁻², 0.05–0.40 Bq cm⁻² and 6.83–83.63 Bq cm⁻², meanwhile the fluxes ranged from 0.005–0.079 Bq cm⁻² yr⁻¹, 0.009–0.048 Bq cm⁻² yr⁻¹ and 0.003–0.037 Bq cm⁻² yr⁻¹, respectively. The results show that the highest inventories and fluxes for ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were found at station WC 01 and EC 05. Because there are additional sources of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra, where water transport will brings more dissolved isotopes, influence of the transportation and deposition of suspended particles, fast rate of regeneration and greater production of those radionuclides and others.     

<Superscript>210</Superscript>Pb and <Superscript>137</Superscript>Cs dating of sediments from Zigetang Lake,Tibetan Plateau

Zigetang Lake located in the central Tibetan Plateau was selected for the purpose of understanding of recent sedimentation rates. Based on ¹³⁷Cs dating marker, the sediment rate was 0.077 cm·yr⁻¹. The sedimentation rate was calculated to be 0.071 cm·yr⁻¹ and 0.029 g·cm⁻²·yr⁻¹ on the basis of ²¹⁰Pb CIC model. ²¹⁰Pb CRS model was also used for understanding of recent sedimentation change. The sediment accumulation rates for the CRS model ranged from 0.022 to 0.038 g·cm⁻²·yr⁻¹ with an irregular high value of 0.12 g·cm⁻²·yr⁻¹ around 1932 at Zigetang Lake core in the past eighty years.     

Comparison of analytical methods used to determine <Superscript>235</Superscript>U, <Superscript>238</Superscript>U and <Superscript>210</Superscript>Pb from sediment samples by alpha,beta and gamma spectrometry

An intercomparison of the methodology (alpha, beta and gamma spectrometry) used for ²³⁸U, ²³⁵U and ²¹⁰Pb determination was carried out based on 38 sediment samples. The activity range of the samples varied from 10–700 Bq/kg for ²¹⁰Pb, 1–35 Bq/kg for ²³⁵U and 10–800 Bq/kg for ²³⁸U. Results obtained using the three methods were not statistically different at high activity levels, but agreement between the results decreased at lower sample activity levels. For ²¹⁰Pb, the smallest difference was found between alpha and gamma spectrometry. A good correlation between results from alpha and gamma spectrometry was observed over the whole activity range. In beta spectrometry, the results were slightly higher than those obtained by alpha or gamma spectrometry due to the impurity of ²²⁸Ra. In ²³⁸U analysis, good correspondence was observed between ²³⁸U determined by gamma and alpha spectrometry, particularly at higher ²³⁸U activity concentrations over 100 Bq/kg. In ²³⁵U analysis, attention needs to be paid to interference from ²²⁶Ra and its reduction.     

Atmospheric deposition fluxes of <Superscript>7</Superscript>Be, <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po at Xiamen,China

The atmospheric deposition fluxes of ⁷Be, ²¹⁰Pb and ²¹⁰Po at Xiamen were measured. The samples were collected from March 2004 to April 2005 and the sampling period was one month. The ⁷Be and ²¹⁰Pb activity were measured using HPGe γ-spectrometer after concentration using Fe(OH)₃ co-precipitation method. The ²¹⁰Po was counted with an α-spectrometer after the sample was digested and spontaneous plated onto a silver planchet. At Xiamen, the atmospheric deposition fluxes of ⁷Be varied between 0.11 and 2.93 Bq·m⁻²·d⁻¹ and the average was 1.64 Bq·m⁻²·d⁻¹; ²¹⁰Pb fluxes varied between 0.04 and 0.85 Bq·m⁻²·d⁻¹, and the average was 0.51 Bq·m⁻²·d⁻¹; ²¹⁰Po fluxes varied between 0.002 and 0.133 Bq·m⁻²·d⁻¹, and the average was 0.061 Bq·m⁻²·d⁻¹. There were positive correlations between the deposition fluxes of ⁷Be, ²¹⁰Pb or ²¹⁰Po and the amount of precipitation. The residence time of aerosols varied between 6.0 and 54.0 days with a mean of 27.1 days, which were calculated by ²¹⁰Po/²¹⁰Pb fluxes ratios.     

Intertidal mangrove mudflat <Superscript>240+239</Superscript>Pu signatures,confirming a <Superscript>210</Superscript>Pb geochronology on the southeastern coast of Brazil

A sediment core was taken to determine if sediment accumulation rates could be conducted using ^240+239Pu signatures in the coastal mangrove mudflats of southeastern Brazil. The results from this study show that ^240+239Pu fallout activities are sufficient and well preserved in the coastal sediments of this region. Sediment accumulation rates determined from the ^240+239Pu signatures were 4.4 mm/year and 4.1 from ²¹⁰Pb (CIC) method. A sediment mixing coefficient rate was calculated using chlorophyll-a profile (9.5 cm²).     

Distribution of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb in riverine environs of coastal Karnataka

The concentrations of ²¹⁰Po and ²¹⁰Pb have been measured in soil, sediment and rock samples collected from major rivers of coastal Karnataka, viz. Kali, Sharavathi and Netravathi. The activity of ²¹⁰Po and ²¹⁰Pb in the samples were separated by radiochemical methods and the activity was counted using ZnS(Ag) alpha-counter. The activity ratio of ²¹⁰Po and ²¹⁰Pb and the dependence of organic matter content on the activity of these radionuclides were studied.     

Distributions of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb radioactivity in the intermediate layer of the northwestern North Pacific

The distributions of ²¹⁰Po and ²¹⁰Pb in the intermediate layer (400–2000 m) of the northwestern North Pacific were determined to elucidate the export flux of particulate matter. ²¹⁰Po generally showed depletion relative to ²¹⁰Pb in the intermediate layer, suggesting that ²¹⁰Po was scavenged by particles. Because the removal rate constants of ²¹⁰Po in the western region were higher than those in the eastern region and this trend coincided with that of the particle fluxes in the surface layer, the export production in the surface layer was assumed to influence the particle flux in the intermediate layer of the northwestern North Pacific.     

Measurements of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb in total diet samples: Estimate of dietary intakes of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb for Japanese

To estimate the dietary intakes of ²¹⁰Pb and ²¹⁰Po for the Japanese adults and their annual effective doses, ²¹⁰Pb and ²¹⁰Po were measured for 240 daily diet samples collected at two locations of Ishikawa Prefecture in Japan over three years by duplicate portion studies. No appreciable differences in intake rates of ²¹⁰Pb and ²¹⁰Po and their ²¹⁰Po/²¹⁰Pb ratios were seen among the years in each district, and between the two districts. The intake rates evaluated using 240 diet samples were 0.20 Bq/d/p for ²¹⁰Pb and 0.61 Bq/d/p for ²¹⁰Po as a median, respectively. Annual effective doses of ²¹⁰Pb and ²¹⁰Po for Japanese adults were estimated to be 0.050 and 0.053 mSv/y, respectively.     

Disequilibrium of dissolved <Superscript>234</Superscript>U/<Superscript>238</Superscript>U and <Superscript>210</Superscript>Po/<Superscript>210</Superscript>Pb in Greek rivers

For the first time, a radiological study for the dissolved ²³⁸U, ²³⁴U, ²¹⁰Pb and ²¹⁰Po was held in major Greek rivers across the country. ²³⁴U/²³⁸U activity ratios are above one in all samples and ²¹⁰Po/²¹⁰Pb activity ratios are respectively below the unit indicating the disequilibrium in the samples. Quite satisfactory correlations were observed among ²³⁴U and ²³⁸U as well as among ²¹⁰Po and ²¹⁰Pb values. Uranium isotopes were separated by ion exchange and electroplated on stainless steel plates. ²¹⁰Po was spontaneously deposited on nickel plates, while ²¹⁰Pb was indirectly determined through the ingrowth of ²¹⁰Po. The sources were measured by a-spectrometry.     

<Superscript>206</Superscript>Pb/<Superscript>207</Superscript>Pb ratios in dry deposit samples from the Metropolitan Zone of Mexico Valley

²⁰⁶Pb/²⁰⁷Pb isotope ratios of dry deposit samples in the Metropolitan Zone of Mexico Valley (MZMV) were determined and correlated with some contemporary environmental material such as gasoline, urban dust, etc., as possibile pollution sources, the latter presenting different signatures ²⁰⁶Pb/²⁰⁷Pb ratios were determined in samples “as is” by ICP-MS, using an Elan-6100. A standard material NIST-981 was used to monitor accuracy and to correct mass fractionation. The calculated enrichment factors of lead (taking rubidium as a conservative endogenous element) show its anthropogenic origin with percentages higher than 97.65%. ²⁰⁶Pb/²⁰⁷Pb ratio in dry deposit samples ranges from 0.816 to a maximum of 1.154, following a normal distribution. Arithmetic mean was 0.9967±0.0864 lower than those of possible pollution sources: 1.1395±0.0165 for gasoline, 1.071±0.008 for industrially derived lead and, for the more radiogenic natural soil and urban dust values ranging from 1.2082±0.022 to 1.211±0.108. The possible origin of lead in gasoline used prior to 1960 is discussed.     

Assessment of <Superscript>210</Superscript>Po in foodstuffs consumed in Korea

²¹⁰Po in the daily diet in Korea was analyzed and the ingestion dose from an intake of ²¹⁰Po was estimated by considering the dietary habit of a Korean person. The ²¹⁰Po concentrations of a leafy vegetable (0.36 Bq·kg⁻¹ for lettuce) in the terrestrial food were higher than those of grain, whereas Chinese cabbage had a lesser ²¹⁰Po concentration (0.019 Bq·kg⁻¹). The ²¹⁰Po concentration of the animal product was similar to those detected in the grain and vegetable. The ²¹⁰Po concentrations in the shell and crustaceous were high from 19.1 to 33.0 Bq·kg⁻¹, however, its value fell in the overall range of the reported values. The effective dose from ²¹⁰Po for an adult from the Korean population was about 269.4 μSv·y⁻¹. Nearly 80% of the ingestion dose from the intake of ²¹⁰Po was attributed to the consumption of seafood. It suggests that the marine food ingestion is a critical pathway for natural ²¹⁰Po to the Korean population.     

Radiofluorination of 2-fluoropyridines by isotopic exchange with [<Superscript>18</Superscript>F]fluoride

In homoaromatic systems, isotopic exchange (¹⁸F/¹⁹F) was previously (J Label Compd Radiopharm 18(12):1721–1730 [2], J Chem Soc Perkin Trans 1(3):295–298 [3]) proven to be advantageous, yet in general specific activity is thought to be low. For heteroaromatic systems, in particular, very few examples are published regarding the ¹⁸F-labelling of 2-substituted pyridines (J Label Compd Radiopharm 42:975–985 [9]). Therefore, in 2-fluoropyridines, we decided to study the ¹⁸F labelling by isotopic exchange (¹⁸F/¹⁹F). The radiochemical yield for 2-fluoropyridine was 90 ± 2%. Even if 2-fluoropyridine was substituted by an electron-donating group such as a methyl or a methoxy group, radiochemical yields were 80 ± 1 and 78 ± 1%, respectively. Although in benzenes, these substituents are known to decrease nucleophilic substitutions by ¹⁸F-Fluoride significantly. Moreover, by choosing appropriate concentrations of 2-fluoropyridines, reasonably high specific activities up to 10 GBq/μmol were obtained.     

Mixing of atmospheric <Superscript>210</Superscript>Pb and <Superscript>7</Superscript>Be and <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr fission products in four characteristic soil types

Depth distribution of atmospheric ²¹⁰Pb and ⁷Be and ⁹⁰Sr and ¹³⁷Cs fission products was measured in two types of aeolian soils (desert dust and volcanic ash), irrigated paddy soil and strongly acidic soil. The depth dependence of ²¹⁰Pb, ⁷Be and ¹³⁷Cs show that these radionuclides have been diffused as solid soil particles in surface soil layers. In aeolian soil layers, about 50% of ⁹⁰Sr were diffused in surface soil layer and the remaining 50% had penetrated to deeper layers. The half of the fission particles containing ⁹⁰Sr were shown to have decomposed over the past 35 years.     

Behavior of <Superscript>7</Superscript>Be and <Superscript>210</Superscript>Pb deposited via rainwater on a coniferous forest,a broad-leaved forest,and grassland

Fall water, stem flow water and falling litter in a coniferous forest (C. japonica) and a broad-leaved forest (L. edulis), and rainwater on a grassland near the forests were collected, and their ⁷Be and ²¹⁰Pb contents were measured. The average residence times of ⁷Be and ²¹⁰Pb in the forest crowns were calculated from the balances of their radionuclides, those in the forest crown of C. japonica were 88 days for ⁷Be and 9.2 years for ²¹⁰Pb, and those in the forest crown of L. edulis were 52 days and <1 year, respectively.     

Improvements on the method for determining of <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po in lead

An improved method is proposed to determine the content of ²¹⁰Pb in lead using ²¹⁰Po measured by alpha-ray spectrometry. This improved method, which is based on radiochemical separation by DDTC–toluene extraction, employs EDTA and citrate as masking reagents for the lead ions. To selectively extract polonium from an alkaline solution, the pH dependency was examined using a liquid scintillation counting method. And pH 9 was chosen as an extraction condition. Then ²¹⁰Po was electrodeposited on a stainless steel disk, and the chemical recovery was followed by ²⁰⁹Po tracer. The effectiveness of the new method was validated by the agreement with the analytical results from five samples as determined by gamma-ray spectrometry.     

Quantification of measurement uncertainty in the sequential determination of <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po by liquid scintillation counting and alpha-particle spectrometry

Methodologies for the quantification of measurement uncertainties associated with the determination of ²¹⁰Pb- and ²¹⁰Po-specific activities by liquid scintillation counting (LSC) and alpha-particle spectrometry are presented, and are demonstrated using the soil reference material IAEA-326. Major contributors to the combined uncertainty associated with the measurement result of ²¹⁰Pb were the uncertainties of net count rates in the ²¹⁰Pb energy region of the sample spectrum and in the ²¹⁰Bi energy region of the blank spectrum. The predominant sources of uncertainty in the measurement of ²¹⁰Po were the uncertainties of net count rates in the regions of interest of ²⁰⁹Po and ²¹⁰Po. The relative standard uncertainty of ²¹⁰Po exponentially increases with the time interval between the sampling date and the separation date of Po, and this effect is strongly dependent on the ²¹⁰Po/²¹⁰Pb activity ratio. When the specific activity of ²¹⁰Pb is much higher than that of ²¹⁰Po in the sample, the relative standard uncertainty of the ²¹⁰Po determination increases significantly within a short time interval between the sampling date (or reference date) and the separation date of Po in samples.     

Variation of <Superscript>231</Superscript>Pa, <Superscript>230</Superscript>Th and <Superscript>231</Superscript>Pa<Subscript>ex</Subscript>/<Superscript>230</Superscript>Th<Subscript>ex</Subscript> in surface sediments of the Sabah–Sarawak coastal waters

Protactinium and thorium activities were measured in eight surface sediment taken in 2004 to determine effectiveness scavenging of ²³¹Pa at Sabah–Sarawak coastal waters. The result found that activity ratios of ²³¹Pa_ex/²³⁰Th_ex were ranged from 0.07 to 0.13 at all sampling stations. The high ²³¹Pa_ex/²³⁰Th_ex activity ratio than the production ratio of 0.093 in seawater at station SR 01, SR 02, SR 04, SB 02 and SB 05, revealed that ²³¹Pa is effectively removed from the water column into the sediment in comparison with ²³⁰Th at those stations. Low percentage of ²³⁰Th_ex (90–95%) in comparison with ²³¹Pa_ex at all stations can be attributed to less efficiently scavenged of ²³⁰Th onto particles prior deposited at the marine sediment bed.     

Determination of <Superscript>3</Superscript>H, <Superscript>226</Superscript>Ra, <Superscript>222</Superscript>Rn and <Superscript>238</Superscript>U in Austrian ground- and drinking water

Screening measurements for ³H, ²²⁶Ra, ²²²Rn and ²³⁸U in ground water were performed within a ground- and drinking water project in Austria. The aim of this project is to get an overview of the distribution of natural radionuclide activity concentration levels in ground water bodies. In some cases this water is used for drinking water abstraction. In this paper methods and results of the screening measurements are presented. Regions with high activity concentrations were identified and in these regions further investigation for ²²⁸Ra, ²¹⁰Pb and ²¹⁰Po will be conducted.     

Novel methodology for the study of mercury methylation and reduction in sediments and water using <Superscript>197</Superscript>Hg radiotracer

Mercury tracers are powerful tools that can be used to study mercury transformations in environmental systems, particularly mercury methylation, demethylation and reduction in sediments and water. However, mercury transformation studies using tracers can be subject to error, especially when used to assess methylation potential. The organic mercury extracted can be as low as 0.01% of the endogenous labeled mercury, and artefacts and contamination present during methylmercury (MeHg) extraction processes can cause interference. Solvent extraction methods based on the use of either KBr/H₂SO₄ or HCl were evaluated in freshwater sediments using ¹⁹⁷Hg radiotracer. Values obtained for the ¹⁹⁷Hg tracer in the organic phase were up to 25-fold higher when HCl was used, which is due to the coextraction of ¹⁹⁷Hg²⁺ into the organic phase during MeHg extraction. Evaluations of the production of MeHg gave similar results with both MeHg extraction procedures, but due to the higher Hg²⁺ contamination of the controls, the uncertainty in the determination was higher when HCl was used. The Hg²⁺ contamination of controls in the HCl extraction method showed a nonlinear correlation with the humic acid content of sediment pore water. Therefore, use of the KBr/H₂SO₄ method is recommended, since it is free from these interferences. ¹⁹⁷Hg radiotracer (T _1/2 = 2.673 d) has a production rate that is about 50 times higher than that of ²⁰³Hg (T _1/2 = 46.595 d), the most frequently used mercury radiotracer. Hence it is possible to obtain a similar level of performance to ²⁰³Hg when it is used it in short-term experiments and produced by the irradiation of ¹⁹⁶Hg with thermal neutrons, using mercury targets with the natural isotopic composition. However, if the 0.15% natural abundance of the ¹⁹⁶Hg isotope is increased, the specific activity of the ¹⁹⁷Hg tracer can be significantly improved. In the present work, ¹⁹⁷Hg tracer was produced from mercury 51.58% enriched in the ¹⁹⁶Hg isotope, and a 340-fold increase in specific activity with respect to natural mercury targets was obtained. When this high specific activity tracer is employed, mercury methylation and reduction experiments with minimum mercury additions are feasible. Tracer recovery in methylation experiments (associated with Me¹⁹⁷Hg production from ¹⁹⁷Hg²⁺ spike, but also with Hg²⁺ contamination and Me¹⁹⁷Hg artefacts) with marine sediments was about 0.005% g⁻¹ WS (WS: wet sediment) after 20 h incubation with mercury additions of 0.05 ng g⁻¹ WS, which is far below natural mercury levels. In this case, the amount of Hg²⁺ reduced to Hg⁰ (expressed as the percent ¹⁹⁷Hg⁰ recovered with respect to the ¹⁹⁷Hg²⁺ added) varied from 0.13 to 1.6% g⁻¹ WS. Me¹⁹⁷Hg production from ¹⁹⁷Hg²⁺ spike after 20 h of incubation of freshwater sediment ranged from 0.02 to 0.13% g⁻¹ WS with mercury additions of 2.5 ng g⁻¹ WS, which is also far below natural levels. ¹⁹⁷Hg⁰ recoveries were low, 0.0058 ± 0.0013% g⁻¹ WS, but showed good reproducibility in five replicates. Me¹⁹⁷Hg production from ¹⁹⁷Hg²⁺ spiked in freshwater samples ranged from 0.1 to 0.3% over a period of three days with mercury additions of 10 ng L⁻¹. A detection limit of 0.05% for Me¹⁹⁷Hg production from ¹⁹⁷Hg²⁺ spike was obtained in seawater in a 25 h incubation experiment with mercury additions of 12 ng L⁻¹.