Spatial and temporal variations of 14C in Fucus spp. in Swedish coastal waters.

Carbon-14 (14C) dominates the collective effective dose from globally dispersed long-lived radionuclides produced by and released from the nuclear power industry. Literature data on the discharge of 14C to the marine environment from nuclear power plants (NPPs) and its dispersion in the marine ecosystem are sparse. The local marine 14C background must be determined before the 14C enrichment in the marine environment from a NPP can be estimated. This is not trivial since marine activity concentrations of 14C vary spatially, partly due to long-range transport of 14C from other anthropogenic sources. We have analysed 14C in samples of several species of brown algae (Fucus spp.) collected at 45 sites along the Swedish coast in 2020. At sites remote from NPPs, the 14C activity concentrations per unit mass of carbon (here expressed as Fraction Modern, F14C) were significantly higher on the west coast than on the east coast (F14C up to about 1.10 in Skagerrak, and about 1.01, close to atmospheric levels, in the Baltic Sea and the Gulf of Bothnia). On the west coast, F14C showed a strong correlation with salinity, both of which increased towards the north. This indicates that 14C is carried from other anthropogenic sources (e.g. from the nuclear fuel reprocessing plants at La Hague and Sellafield). The highest value of F14C observed was close to the Ringhals NPP on the west coast, F14C ≈ 1.3, which is higher than expected in the terrestrial environment of this NPP. We also report on temporal variations of F14C in Fucus spp. collected at Särdal on the Swedish west coast during the period 1967-2020. The values of F14C in the Särdal marine samples collected after the 1990s are clearly higher than F14C in clean air CO2, indicating contributions of 14C of anthropogenic origin.

Human Atherosclerotic Plaque Progression Is Dependent on Apoptosis According to Bomb-Pulse 14C Dating.

Individuals with rapidly progressing atherosclerotic plaques are at higher risk of experiencing acute complications. Currently, we lack knowledge regarding factors in human plaque that cause rapid progression. Using the 14C bomb-pulse dating method, we assessed the physical age of atherosclerotic plaques and which biological processes were associated with rapidly progressing plaques. Interestingly, increased apoptosis was the main component associated with a young physical plaque age, reflecting rapid plaque progression. Our findings in combination with recent advances in imaging techniques could guide future diagnostic imaging strategies to identify rapidly progressing plaques or therapeutic targets, halting plaque progression.

In vivo measurement of pre-operational spallation source workers: baseline body burden levels and detection limits of relevant gamma emitters using high-resolution gamma spectrometry.

As a measure to prepare for long-term internal dose monitoring of workers at the European Spallation Source (ESS) in Lund, Sweden, operated by the European Research Infrastructure Consortium (ERIC), as well as to enhance emergency preparedness against accidental releases, a series of in vivo measurements were conducted using a high-resolution HPGe detector with a 123% relative efficiency (1.332 MeV). This study describes the whole-body counting set-up, calibration procedure, and subsequent validation measurements using conventional NaI(Tl)-scanning-bed geometry on a selection of workers from the ESS. Detection limits for the relevant gamma emitters 7Be, 172Hf, and 182Ta were determined to be 65 Bq, 130 Bq, and 22 Bq, respectively, using a 2400 s acquisition time. The baseline measurements suggest that care must be taken to ensure that the fluctuations in the presence of radon daughters 214Bi and 214Pb are minimised by, for example, ensuring a minimum air exchange between the measuring room and the ambient air, and by demanding that the measured subjects change clothes and shower before measurement. Furthermore, in a monitoring program for internal doses to spallation source workers, the presence of radionuclides originating from non-work-related sources (such as 226Ra from private water wells or 137Cs from intakes of Chernobyl contaminated foodstuffs), or radionuclides from previous work history (such as 60Co within the nuclear power industry), must be considered.

Extending the scope of dispersive liquid-liquid microextraction for trace analysis of 3-methyl-1,2,3-butanetricarboxylic acid in atmospheric aerosols leading to the discovery of iron(III) complexes.

3-Methyl-1,2,3-butanetricarboxylic acid (MBTCA) is a secondary organic aerosol and can be used as a unique emission marker of biogenic emissions of monoterpenes. Seasonal variations and differences in vegetation cover around the world may lead to low atmospheric MBTCA concentrations, in many cases too low to be measured. Hence, an important tool to quantify the contribution of terrestrial vegetation to the loading of secondary organic aerosol may be compromised. To meet this challenge, a dispersive liquid-liquid microextraction (DLLME) method, known for the extraction of hydrophobic compounds, was extended to the extraction of polar organic compounds like MBTCA without compromising the efficiency of the method. The extraction solvent was fine-tuned using tri-n-octyl phosphine oxide as additive. A multivariate experimental design was applied for deeper understanding of significant variables and interactions between them. The optimum extraction conditions included 1-octanol with 15% tri-n-octyl phosphine oxide (w/w) as extraction solvent, methanol as dispersive solvent, 25% NaCl dissolved in 5 mL sample (w/w) acidified to pH 2 using HNO3, and extraction time of 15 min. A limit of detection of 0.12 pg/m3 in air was achieved. Furthermore, unique complexation behavior of MBTCA with iron(III) was found when analyzed with ultra-high-performance liquid chromatography coupled with electrospray ionization-quadrupole time-of-flight mass spectrometry (UHPLC-ESI-QToF). A comprehensive overview of this complexation behavior of MBTCA was examined with systematically designed experiments. This newly discovered behavior of MBTCA will be of interest for further research on organometallic photooxidation chemistry of atmospheric aerosols. Graphical abstract a) Additive assisted DLLME and MBTCA complexes with Fe(III), b) A good quality figure is attached in ppt format to facilitate editable objects.

Towards the isolation and estimation of elemental carbon in atmospheric aerosols using supercritical fluid extraction and thermo-optical analysis.

Air-starved combustion of biomass and fossil fuels releases aerosols, including airborne carbonaceous particles, causing negative climatic and health effects. Radiocarbon analysis of the elemental carbon (EC) fraction can help apportion sources of its emission, which is greatly constrained by the challenges in isolation of EC from organic compounds in atmospheric aerosols. The isolation of EC using thermo-optical analysis is however biased by the presence of interfering compounds that undergo pyrolysis during the analysis. EC is considered insoluble in all acidic, basic, and organic solvents. Based on the property of insolubility, a sample preparation method using supercritical CO2 and methanol as co-solvent was developed to remove interfering organic compounds. The efficiency of the method was studied by varying the density of supercritical carbon dioxide by means of temperature and pressure and by varying the methanol content. Supercritical CO2 with 10% methanol by volume at a temperature of 60 °C, a pressure of 350 bar and 20 min static mode extraction were found to be the most suitable conditions for the removal of 59 ± 3% organic carbon, including compounds responsible for pyrolysis with 78 ± 16% EC recovery. The results indicate that the method has potential for the estimation and isolation of EC from OC for subsequent analysis methods and source apportionment studies.

Direct association between diet and the stability of human atherosclerotic plaque.

Mediterranean diet has been suggested to explain why coronary heart disease mortality is lower in southern than northern Europe. Dietary habits can be revealed by isotope ratio mass spectrometry (IRMS) measurement of carbon (δ(13)C) and nitrogen (δ(15)N) in biological tissues. To study if diet is associated with human plaque stability, atherosclerotic plaques from carotid endarterectomy on 56 patients (21 Portuguese and 35 Swedish) were analysed by IRMS and histology. Plaque components affecting rupture risk were measured. Swedish plaques had more apoptosis, lipids and larger cores, as well as fewer proliferating cells and SMC than the Portuguese, conferring the Swedish a more rupture-prone phenotype. Portuguese plaques contained higher δ(13)C and δ(15)N than the Swedish, indicating that Portuguese plaques were more often derived from marine food. Plaque δ(13)C correlated with SMC and proliferating cells, and inversely with lipids, core size, apoptosis. Plaque δ(15)N correlated with SMC and inversely with lipids, core size and apoptosis. This is the first observational study showing that diet is reflected in plaque components associated with its vulnerability. The Portuguese plaques composition is consistent with an increased marine food intake and those plaques are more stable than those from Swedish patients. Marine-derived food is associated with plaque stability.

Bomb-pulse 14C analysis combined with 13C and 15N measurements in blood serum from residents of Malmö, Sweden.

The (14)C content of 60 human blood serum samples from residents of Malmö (Sweden) in 1978, obtained from a biobank, has been measured to estimate the accuracy of (14)C bomb-pulse dating. The difference between the date estimated using the Calibomb software and sampling date varied between -3 ± 0.4 and +0.2 ± 0.5 years. The average age deviation of all samples was -1.5 ± 0.7 years, with the delay between production and consumption of foodstuffs being probably the dominating cause. The potential influence of food habits on the (14)C date has been evaluated using stable isotope δ(13)C and δ(15)N analysis and information about the dietary habits of the investigated individuals. Although the group consisting of lacto-ovo vegetarians and vegans (pooled group) was not completely separated from the omnivores in a stable isotopic trophic level diagram, this analysis proved to add valuable information on probable dietary habits. The age deviation of the sampling date from the respective Calibomb date was found strongly correlated with the δ(13)C values, probably due to influence from marine diet components. For the omnivore individuals, there were indications of seasonal effects on δ(13)C and the age deviation. No significant correlation was found between the age deviation and the δ(15)N values of any dietary group. No influence of sex or year of birth was found on neither the (14)C nor the δ(13)C and δ(15)N values of the serum samples. The data were also divided into two groups (omnivores and pooled group), based on the level of δ(15)N in the samples. The consumption of high δ(15)N-valued fish and birds can be responsible for this clustering.

Short communication: Dating components of human atherosclerotic plaques.

RATIONALE: Atherosclerotic plaques that give rise to acute clinical symptoms are typically characterized by degradation of the connective tissue and plaque rupture. Experimental studies have shown that mechanisms to repair vulnerable lesions exist, but the rate of remodeling of human plaque tissue has not been studied. OBJECTIVE: In the present study, we determined the biological age of different components of advanced human atherosclerotic plaques by analyzing tissue levels of (14)C released into the atmosphere during the nuclear weapons tests in the late 1950s and early 1960s. METHODS AND RESULTS: Atherosclerotic plaques were obtained from 10 patients (age 46 to 80 years) undergoing carotid surgery. Different regions of the plaques were dissected and analyzed for (14)C content using accelerator mass spectrometry. At the time of surgery, the mean biological age of the cap region was 6.4+/-3.2 years, which was significantly lower than that of the shoulder region (12.9+/-3.0 years, P<0.01), the interface toward the media (12.4+/-3.3 years, P<0.01), and the core (9.8+/-4.5 years, P<0.05). Analysis of proliferative activity and rate of apoptosis showed no signs of increased cellular turnover in the cap, suggesting that the lower (14)C content reflected a more recent time of formation. CONCLUSIONS: These results show that the turnover time of human plaque tissue is very long and may explain why regression of atherosclerotic plaque size rarely is observed in cardiovascular intervention trials.

The use of hair as an indicator of occupational 14C contamination.

This paper presents a study in which the specific activity of (14)C in hair has been investigated as an easily determined bio-indicator of the integrated (14)C exposure (over several months). The study includes 28 Swedish workers handling (14)C-labelled compounds, or working in a (14)C-enriched environment. Hair samples from personnel at a Swedish nuclear power plant showed very low levels of (14)C contamination, if any. In contrast, personnel at the investigated research departments showed (14)C levels in hair of up to 60% above the natural specific activity of (14)C. Much higher levels, up to 80 times the natural specific activity of (14)C, were found in hair from individuals working at a pharmaceutical research laboratory. This contamination was, however, not solely an internal contamination. There were indications that most of the (14)C in the hair originated from airborne (14)C-compounds, which were adsorbed onto the hair. The difficulties in removing this external (14)C contamination prior to analysis are discussed, as are the possibilities of using accelerator mass spectrometry to analyse various types of samples for retrospective dose assessment.

14CO2 dispersion around two PWR nuclear power plants in Brazil.

Atmospheric air samples were taken within 3 km from power plants encompassing five different distances and wind directions. Samples were taken between 2002 and 2005 aiming to evaluate the environmental (14)C enrichment due to the operation of Brazilian nuclear power plants. The sampling system consisted of a pump connected to a trapping column filled with a 3M NaOH solution. The trapped CO(2) was analyzed for (14)C by using a single stage accelerator mass spectrometry (SSAMS). All sampling sites revealed measurable (14)C excess values. The maximum excesses were of 15 and 14 mBq/m(3) for sampling sites placed at NE of the power plants, which is the main wind direction in the area. The mean excesses values were 12 mBq/m(3) to the NE direction, 8 mBq/m(3) to the E, 10 mBq/m(3) to the N, 8 mBq/m(3) to the WNW and 7 mBq/m(3) to the W direction (increasing distances from NE to W). Compared to other Light Water Reactors (LWR) data, these means' values are significantly higher than the average worldwide reported value of 3 mBq/m(3). Available data indicate that the observed values are not related to (14)C emission by the power plants vent stack. Other factors, such as topography, seem to have an important role because it affects wind dispersion thus favoring (14)C accumulation in the sampled area. Moreover, the high elevations around the power plants enhance the chances to measure high values of (14)C since the plume can be intercepted before it is drawn to the ground. Modeling of the plume has shown that its dispersion does not follow a Gaussian model and that agreement between atmospheric CO(2) and vegetation (14)C activities occurs only for sampling sites placed at NE of the power plants.

(14)C, delta(13)C and total C content in soils around a Brazilian PWR nuclear power plant.

Nuclear power plants release (14)C during routine operation mainly as airborne gaseous effluents. Because of the long half-life (5730 years) and biological importance of this radionuclide (it is incorporated in plant tissue by photosynthesis), several countries have monitoring programs in order to quantify and control these emissions. This paper compares the activity of (14)C in soils taken within 1km from a Brazilian nuclear power plant with soils taken within a reference area located 50km away from the reactor site. Analyses of total carbon, delta(13)C and (137)Cs were also performed in order to understand the local soil dynamics. Except for one of the profiles, the isotopic composition of soil organic carbon reflected the actual forest vegetation present in both areas. The (137)Cs data show that the soils from the base of hills are probably allocthonous. The (14)C measurements showed that there is no accumulation due to the operation of the nuclear facility, although excess (14)C was found in the litter taken in the area close to power plant. This indicates that the anthropogenic signal observed in the litter fall has not been transferred yet to the soil. This study is part of an extensive research programme in which other samples including air, vegetation and gaseous effluents (taken in the vent stack of the Brazilian nuclear power reactors Angra I and II) were also analyzed. The present paper aimed to evaluate how (14)C emissions from the nuclear power plant are transferred and stored by soils present in the surroundings of the reactor site. This is the first study concerning anthropogenic (14)C in soils in Brazil.

Characterization of 14C in Swedish light water reactors.

This paper presents the results of a 4-y investigation of 14C in different waste streams of both boiling water reactors (BWRs) and pressurized water reactors (PWRs). Due to the potential impact of 14C on human health, minimizing waste and releases from the nuclear power industry is of considerable interest. The experimental data and conclusions may be implemented to select appropriate waste management strategies and practices at reactor units and disposal facilities. Organic and inorganic 14C in spent ion exchange resins, process water systems, ejector off-gas and replaced steam generator tubes were analyzed using a recently developed extraction method. Separate analysis of the chemical species is of importance in order to model and predict the fate of 14C within process systems as well as in dose calculations for disposal facilities. By combining the results of this investigation with newly calculated production rates, mass balance assessments were made of the 14C originating from production in the coolant. Of the 14C formed in the coolant of BWRs, 0.6-0.8% was found to be accumulated in the ion exchange resins (core-specific production rate in the coolant of a 2,500 MWth BWR calculated to be 580 GBq GW(e)(-1) y(-1)). The corresponding value for PWRs was 6-10% (production rate in a 2,775 MWth PWR calculated to be 350 GBq GW(e)(-1) y(-1)). The 14C released with liquid discharges was found to be insignificant, constituting less than 0.5% of the production in the coolant. The stack releases, routinely measured at the power plants, were found to correspond to 60-155% of the calculated coolant production, with large variations between the BWR units.

14C content in vegetation in the vicinities of Brazilian nuclear power reactors.

(14)C specific activities were measured in grass samples collected around Brazilian nuclear power reactors. The specific activity values varied between 227 and 299 Bq/kg C. Except for two samples which showed (14)C specific activities 22% above background values, half of the samples showed background specific activities, and the other half had a (14)C excess of 1-18%. The highest specific activities were found close to the nuclear power plants and along the main wind directions (NE and NNE). The activity values were found to decrease with increasing distance from the reactors. The unexpectedly high (14)C excess values found in two samples were related to the local topography, which favors (14)C accumulation and limits the dispersion of the plume. The results indicate a clear (14)C anthropogenic signal within 5 km around the nuclear power plants which is most prominent along northeastwards, the prevailing wind direction.

Low-level occupational 14C contamination--results from a pilot study.

This paper presents a pilot study in which specific activities of 14C in hair and urine from 11 radiation workers handling 14C-containing substances have been measured using accelerator mass spectrometry. Varying degrees of contamination were revealed: up to 63% excess in hair and 400% excess in urine. Although the 14C excess reported in this study would result in low effective doses, it would be of interest to monitor the situation at other workplaces with potentially higher risks of contamination. Simultaneous measurements of 14C in hair and urine with additional random measurements of 14C in faeces and exhaled air could provide a means of improving dose estimates for workers handling different types of 14C-containing substances.

Long-term biokinetics and radiation exposure of patients undergoing 14C-glycocholic acid and 14C-xylose breath tests.

The (14)C-glycocholic acid and (14)C-xylose breath tests are clinically used for the diagnosis of intestinal diseases, such as bacterial overgrowth in the small intestine. The two tests have in earlier studies been thoroughly evaluated regarding their clinical value, but due to the long physical half-life of (14)C and the limited biokinetic and dosimetric data, which are available for humans, several hospitals have been restrictive in their use. The aim of this study was to investigate the long-term biokinetics and dosimetry of the two (14)C compounds in patients and volunteers, using the highly sensitive accelerator mass spectrometry (AMS) technique. Eighteen (18) subjects were included, 9 for each compound. The (14)C content in samples from exhaled air, urine, and, for some subjects, also feces were analyzed with both liquid scintillation counting (LSC) and AMS. The results from the glycocholic acid study showed that, up to 1 year after the administration, 67%+/-6% (mean+/-standard deviation) of the administered activity was recovered in exhaled air, 2.4%+/-0.4% was found in urine, and 7.6% (1 subject) in feces. In the xylose study, the major part was found in the urine (66%+/-2%). A significant part was exhaled (28%+/-5%), and the result from an initial 72-hour stool collection from 2 of the subjects showed that the excretion by feces was insignificant. The absorbed dose to various organs and tissues and the effective dose were calculated by using biokinetic models, based on a combination of experimental data from the present study and from earlier reports. In the glycocholic acid study, the highest absorbed dose was received by the colon (1.2 mGy/MBq). In the xylose study, the adipose tissue received 0.8 mGy/MBq. The effective dose was estimated to 0.5 (glycocholic acid) and 0.07 mSv/MBq (xylose). Thus, from a radiation protection point of view, we see no need for restrictions in using the two (14)C-labeled radiopharmaceuticals on adults with the activities normally administered (0.07-0.4 MBq).

Assessment of the environmental contamination with long-lived radionuclides around an operating RBMK reactor station.

The presence of man-made gamma emitting radionuclides in the region within 32km radius of the Ignalina NPP/Lithuania has been investigated during the period 2001-2004, prior to the closure of the first of the two operating RBMK 1500-type reactors. Gamma spectrometric measurements of various terrestrial and aquatic plants as well as of soil samples showed moderate environmental contamination with the fission product (137)Cs and with the neutron activation products (60)Co and (54)Mn. Traces of the activation products (65)Zn and (110m)Ag were found in the nearest vicinity of the NPP. Activity concentrations were inhomogeneously distributed in the area of interest. Moss and algae samples showed the highest uptake of radionuclides. In addition to the gamma spectrometric measurements, the levels of (14)C were determined in the same bio-indicator samples using accelerator mass spectrometry.

Biokinetics and radiation dosimetry for patients undergoing a glycerol tri[1-14C]oleate fat malabsorption breath test.

The glycerol tri[1-14C]olein test for fat malabsorption was carried out in two male volunteers and measurements of the loss of 14C in expired air, urine and faeces and the retention of 14C in biopsy samples of abdominal fat were made using accelerator mass spectrometry. Exhalation accounted for 73% and 55% of the administered activity and could be described by three-component exponential functions with halftimes of about 1h, 2 days and 150 days, respectively. Urinary excretion accounted for 24% of the administered activity, almost all during the first 24h after administration; about 2% was excreted in the faeces in 48h. The halftime of retention of 14C in fat ranged from 137 to 620 days. Absorbed dose calculations indicate that for a normal adult the largest dose, 1.5-7.0mGy/MBq is received by the adipose tissue, and that the effective dose is 0.3-0.5mSv/MBq. It is concluded that no restrictions need to be placed on radiation safety grounds on the administration of 0.05-0.1MBq 14C-triolein for the triolein breath test.