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Perspective

210Po in the Environment: Reassessment of Dose to Humans

by
Saif Uddin
1,*,
Scott W. Fowler
2,† and
Montaha Behbehani
1
1
Environment Pollution and Climate Program, Kuwait Institute for Scientific Research, Safat 13109, Kuwait
2
School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000, USA
*
Author to whom correspondence should be addressed.
†
Present address: Institute Bobby, 8 Allée des Orangers, 06320 Cap d’Ail, France.
Sustainability 2023, 15(2), 1674; https://doi.org/10.3390/su15021674
Submission received: 3 December 2022 / Revised: 11 January 2023 / Accepted: 12 January 2023 / Published: 15 January 2023
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Abstract

:
Significant efforts have been made by the International Commission on Radiological Protection (ICRP) to establish a reliable basis of equivalent and effective doses due to radionuclides. The ICRP over years has been updating the dose coefficients to include recent developments and make it more realistic. This perspective highlights some issues that warrant updating the methodology used for estimating 210Po dose to humans. The need to underpin these dose coefficients with ever-increasing literature has encouraged us to share the observation on the significant loss of 210Po due to seafood cooking, considering the loss due to cooking warrants changing the factor for the dose from seafood ingestion. Most dose assessment approaches use whole-body concentration, while most 210Po is present in the liver and digestive system that often are not part of the edible portion. The other factor is the extremely high 210Po concentration in aerosols as a result of coal and oil-fired power plants, forest fires, and volcanic activities, especially in the inhalable fraction. The 210Po/210Pb concentration ratio in the Gulf was observed to be between 1.6 and 1.9 in contrast to the 0.1 ratio observed in non-impacted areas. This reassessment of the inhalation dose is also relevant globally due to increasing incidences of forest fires where a much higher than 0.1 210Po/210Pb ratio is expected and will result in a significant inhalation dose.

1. Introduction

There has been considerable interest in polonium ever since its discovery in 1898. There are forty three isotopes of polonium and all of which are radioactive [1]. Seven of these isotopes are naturally occurring, of which 210Po is the longest lived with a 138.4-day half life [2]. 210Po is one of the most toxic naturally occurring radioactive material (NORM) due to its high specific activity of 1.66 × 1014 Bq g−1 [1]. The toxicity of 210Po can be appreciated from the fact that the lethal dose for humans is ~10 µg [3]. The main source of 210Po and its progeny in the environment is 238U. The average concentration of uranium in earth is about 2.8 ppm of which 99.284% is 238U. The exhalation of 222Rn from the soil due to natural decay of 238U is a major source of 210Po in the atmosphere [4,5]. Other conspicuous natural sources of 210Po in the environment are volcanic eruptions, forest fires [6,7], and atmospheric dust [5], while fossil fuel production and burning [5,8], effluent and tailings from uranium mining, phosphate fertilizer, and coal fired power plants are the major artificial sources. There was an incident of a 42 TBq 210Po release from a nuclear power plant fire in Sellafield, United Kingdom in 1957 [9]. 210Po is also artificially produced by irradiating 209Bi with thermal neutrons to obtain 210Bi, which decays to 210Po.
The overriding interest in 210Po assessment emanates from the fact that over 90% of the natural radiation dose received by living organisms comes from 210Po ingestion and inhalation [10,11]. The initial assessment on 210Po dose indicated that 78.1% of total 210Po intake is from the ingestion of food, 17.1% from cigarette smoke, 4.2% from water and 0.6% from air inhalation [12]. These estimates have been updated and revised in a recently developed biokinetic model developed following the mysterious death of Mr. Alexander Litvinenko, and it was concluded that the daily committed effective dose range from ingestion ranges between 2.1 × 10−3–1.7 × 10−2 mSv and 5.5 × 10−2–4.5 × 10−1 mSv by inhalation [13]. The United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) estimates suggest that the average natural radiation dose received by humans on earth is 2.4 mSv y−1 [14] of which 52% is from internal radiation, 20% from external terrestrial radiation, 16% due to cosmic radiation, and 12% from ingestion. Details of likely 210Po dose from seafood ingestion and aerosol inhalation are discussed in this perspective, and that should provide insight on whether the dose estimates and significant pathways need reassessment.

2. 210Po Levels in Environment

There is a consensus that 238U in earth’s crust is the source of 210Pb and 210Po in environment. There is significant variation in uranium concentration in different geologic formations, with 0.1 mg kg−1 in some basalts to 6.1 mg kg−1 in some granites, and a maximum of 300 mg kg−1 in phosphates and up to 1250 mg kg−1 in some shale formations. In an ideal condition 210Pb and 210Po are more or less in secular equilibrium with 238U. However, due to various geological and geomorphological processes, this equilibrium is disturbed mainly due to decay of uranium and release of 222Rn from soils into the atmosphere. The 210Pb and 210Po are very close to secular equilibrium in top soils, with considerable spatial variation globally. Several studies have reported 210Po concentrations of 2–22000 Bq kg−1 (DW) [15,16,17,18,19,20,21,22,23,24] in surface soil with significant spatial distribution. A significant quantity of 210Po is known to be added by fracking waste from the oil industry [25].
In addition to 222Rn exhalation from soil into the atmosphere, there are other significant pathways, e.g., volcanic eruptions, industrial activities, power plants (coal and oil fired), forest fires, and fossil fuel burning [4,26,27,28,29,30,31,32]. Investigations by such researchers have found the oil industry and power and desalination plants reliant on fossil fuel to be a significant source of 210Po for the atmosphere [5] in those regions. Due to their particle reactive nature, 210Po and 210Pb quickly attach to the particles in atmosphere and are scavenged and deposited in terrestrial and marine areas due to wet and dry deposition. The 210Pb and 210Po deposited over these areas becomes incorporated into various plants due to uptake by roots or foliar uptake by leaves [9,33]. Carvalho et al. [9] provided a detailed summary of the activity concentration of 210Po in terrestrial plants and they vary both spatially and with plant type, with the lowest values in vegetables, fruits, and trees in Portugal, and the highest levels in lichens in the United Kingdom.
There are umpteen studies over last 5–6 decades that have looked at 210Pb and 210Po levels in organisms (animals). 210Pb is commonly retained in bones while 210Po is located in soft tissues, with the highest concentrations in liver > kidney > meat [34,35,36,37]. Both 210Pb and 210Po have been extensively studied in marine biota [38,39,40,41,42,43,44,45,46,47,48,49,50,51,52]. Elevated levels of 210Po in most marine biota are considered a potent route of enhanced radiation dose to humans consuming seafood [26,46,53,54,55].
Being particle reactive, significant amounts of 210Pb and 210Po are associated with suspended particulate matter in the aquatic environment. In the marine environment, higher concentrations of 210Po and 210Pb are observed at depth due both to the release of 226Ra from the oceanic sea floor and the downward flux of phytoplankton and zooplankton debris, such as zooplankton molts, carcasses and fecal pellets.

3. 210Po Dose to Humans

210Po is a highly radiotoxic naturally occurring radioisotope with a specific activity of 166 TBq g−1. The International Commission on Radiological Protection (ICRP) has stipulated the fractional intestinal uptake as 50%. Seafood ingestion is considered a significant route of 210Po dose to humans [14]. Reports show that intake via inhalation is much smaller than ingestion [56], even at uranium milling facilities [57]. The International Atomic Energy Agency (IAEA) under its coordinated research project “Sources of Radioactivity in the Marine Environment and Their Relative Contributions to Overall Dose Assessment from Radioactivity (MARDOS)” suggested two methods for dose estimation from seafood ingestion [58]. The dose estimates using Method 1 use the activity concentration of 210Po in water (for 1990) for different fishing areas and applies recommended concentration factors which are equivalent to 1.5 × 10−4 CwFc for fish and 3.2 × 10−3 CwFc for shellfish. For Method 2, the doses were estimated using IAEA estimated concentrations in fish and shellfish (for 1990), equivalent to 7.6 × 10−8 CbFc for fish and 1.1 × 10−7 CbFc for shellfish, where Cw is concentration in water, Cb is concentration in edible part of the biota, and Fc is the catch from the FAO fishing area in kg yr−1. It is reported that ingestion is the main route of Po reaching the gastrointestinal tract, being absorbed in plasma and distributed to soft tissues, with accumulation in the liver and kidneys [56,59]. Table 1 presents annual 210Po ingestion in different countries. The graphical depiction is presented in Figure 1.

4. Need for an Improved Dose Estimate

For a realistic dose assessment, it was highlighted way back in 1995 to consider the effect of cooking on levels of 210Po and 210Pb in seafood [72]. It was only in 2018–2019 that an assessment of 210Po loss in cooked seafood was published by this group which showed a significant loss of 210Po in cooked seafood [68]. The 210Po loss in fish varies between 14% and 58%, with significant variation among the fish studied, with no difference in most fish between the way they were cooked. The wet weight (wwt) concentration ranged from 0.73 to 50.9 mBq g−1 for uncooked edible tissue; 0.43 to 46.3 mBq g−1 for grilled; 0.38 to 44.3 mBq g−1 for boiled fish muscle. The 210Po concentrations in fish stock varied between 0.05 and 3.84 mBq g−1. The 210Po concentration in whole shrimp varied between 68.6 and 484 mBq g−1 wwt (uncooked), 78.1 and 310 mBq g−1 wwt (grilled), 35.6 and 157 mBq g−1 wwt (boiled), and the stock range was 14.4 to 27.6 mBq g−1. The study also highlighted that the bulk of 210Po concentration is in the heptopancreas and digestive systems. Once the head was removed and shrimp were deveined, the highest 210Po concentrations of 25.1–79.7 mBq g−1 wwt were in uncooked shrimps, followed by grilled samples in which the concentrations were 19.4 and 59.1 mBq g−1 wwt, and boiled shrimp concentrations at 18.1–42.6 mBq g−1 wwt, and the lowest concentrations were in the stock where the 210Po was only 3.70 and 4.52 mBq g−1.
The reduction in 210Po concentration were more significant in shrimps where a 75% decrease in 210Po concentration was observed in deveined shrimps and 84% in cooked deveined shrimps than in uncooked whole shrimps. These results strongly confirm a significant loss of 210Po due to cooking. This finding elicits a discussion on reassessing how doses are estimated for humans ingesting seafood. The safe consumption advisories are based on the concentration in fresh seafood. With such losses due to cooking now known, they need to be factored in the dose models for determining realistic dose assessments and safe consumption limits for humans.
Another aspect that needs addressing is the inhalation dose, considering that the ICRP has made efforts to assess radiation dose, several publications have been produced over the years, the latest of them being ICRP Publication 119 [74,75]. The inhalation dose is based on the assumption of absorption scenarios classified as slow, moderate, and fast. The highest dose coefficient is for slow and is seven times higher than the fast scenario. The ICRP Publication 119 has provided inhalation dose coefficients for 1 µm and 5 µm particle sizes under moderate and fast absorption scenarios. The inhalation dose to workers for a 1 µm fast scenario was 6.0 × 10−7 Sv Bq−1 and for moderate is 3.0 × 10−6 Sv Bq−1; whereas for a 5 µm size fast scenario it was 7.1 × 10−7 Sv Bq−1 and for moderate is 2.2 × 10−6 Sv Bq−1. Compared to the inhalation dose, the ingestion dose coefficient was suggested to be 2.4 × 10−7 Sv Bq−1.
In some recent investigations, concentrations of 210Po were determined for size-fractionated aerosols in Kuwait. The results showed 91% of the aerosol load was in the inhalable size fraction with the 210Po/210Pb ratios between 1.2–1.9, much above typical activity Po/Pb ratios of <0.1 in areas free of anthropogenic inputs. The highest concentrations were found downwind of an industrial area that houses petroleum industries, a cement factory, and a power and desalination plant [5]. Due to sparse precipitation, often, the 210Pb and 210Po produced from 222Rn in atmosphere remains in aerosol. The dry deposition of this 210Po will be a more significant pathway in this case.
The volcanic gasses and the recurrent forest fires reported globally has destroyed about 1,207,649 Km2 forest between 2001 and 2019 [76]. The country-wise area is provided in Supplementary file S1; However significantly, forest fires are reported from Australia, Argentina, Brazil, Bolivia, Chile, China, Colombia, Congo, Indonesia, Madagascar, Mongolia, Mexico, Malaysia, Peru, Paraguay, Portugal, Russia, Spain, South Africa, and United States of America, which can be another significant source of atmospheric polonium. The 210Po/210Pb and 210Bi/210Pb ratios can be used for assessing the suspended particulate matter deposition rates and factored in for dose calculation [29,77]. The oil operations and coal-fired power plants are to be considered. In Kuwait, radon concentrations in air samples collected downwind from industrial areas associated with oil operations are in the 2523–131,618 Bq/m3 range [78]. Such levels could result in higher atmospheric 210Pb and 210Po concentrations and likely lead to higher inhalation exposure.
Given the higher concentration of 210Po in aerosol in oil producing countries, areas affected by forest fires and volcanic eruptions, and coal-fired power plants, the inhalation doses in these regions are likely to be much higher than the ingestion dose. Keeping in mind that a significant portion of polonium is lost due to cooking, we feel there is a definite need to reassess the ingestion and inhalation doses that humans and non-human terrestrial biota are receiving.

5. Discussion

The need for reassessing the dose from 210Po emanates from the fact that none of the currently applied approaches, i.e., ERICA (Environmental Risk from Ionising Contaminants: Assessment and Management), MARDOS-IAEA, and ICRP, take into account the 210Po losses due to cooking of seafood. Most of the 210Po concentrations used are whole-body concentrations; whereas studies have shown that the highest 210Po concentrations in marine biota are in the liver and digestive systems that are often removed before cooking, which will result in significantly lower 210Po in edible tissue. The methods proposed by MARDOS include the activity concentration of 210Po in water (for 1990) for different fishing areas and applying concentration factors equivalent to 1.5 × 10−4 CwFc for fish and 3.2 × 10−3 CwFc for shellfish, or the doses estimated using IAEA estimated concentrations in fish and shellfish, both of which are very coarse approximations.
The other very critical issue is the weight to be given to the 210Po inhalation dose. The growing amount of literature on high levels of 210Po in aerosol in the proximity of coal and oil-fired power plants, the oil industry, volcanic eruptions, and forest fires certainly warrants reconsideration of inhalation pathways in dose estimations. The increasing incidences of forest fires can result in significantly higher 210Po concentration in the atmosphere and rationalize the need to look at inhalation pathways more seriously. This perspective intends to open a discussion among groups interested in radioecology and risk assessment to refine and modify the current risk assessment tools.

6. Conclusions

Based on the information summarized in this perspective, we think there is an obvious need to reconsider how 210Po dose to humans is assessed. The ICRP is continuously updating the guidelines, with more and more regional data generated, much of which is summarized in the IAEA’s MARIS database. The fact that usually the highest concentrations of 210Po are in organs such as the liver, hepatopancreas, digestive system, and fecal matter, which are most often not part of the human diet, it will be prudent to consider a concentration in edible tissue only. Moreover, the significant loss of 210Po which takes place due to cooking is not presently accounted for in dose estimations. Unequivocal evidence of 210Po emanating from industrial sources and forest fires has not attracted due attention and can be a more significant pathway for 210Po dose to humans via inhalation. With recent developments, some countries in Europe are considering the utilization of coal to meet the energy demands which would further exacerbate 210Po emissions to the atmosphere. The recurrence of forest fires across the globe is also likely to add an unprecedented amount of 210Po to the atmosphere and likely result in a large dose contribution to humans. With the evidence provided in this communication, we wish to initiate a discussion within the current scenario on whether inhalation is a dominant pathway for the population living in regions impacted by forest fires and downwind of coal-fired power plants and oil operations, instead of only considering seafood ingestion which itself needs correction and refinement.

Supplementary Materials

The Following upporting information can be downloaded at: https://www.mdpi.com/article/10.3390/su15021674/s1, Table S1: Forest Area lost due to fires (2001 – 2019) in Km2.

Author Contributions

Conceptulization, S.U.; Writing the original draft, S.U., S.W.F. and M.B.; Reviewing and editing, S.U. and S.W.F. All authors have read and agreed to the published version of the manuscript.

Funding

There was no funding received for this study.

Informed Consent Statement

Not Applicable.

Data Availability Statement

All the data reported and used is duly referenced and will be made available on request.

Acknowledgments

The authors thank Mohammad Faizuddin of GGIS UAE for providing a graphical representation of the polonium ingestion data.

Conflicts of Interest

The authors declare no conflict of interest.

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Sustainability 15 01674 g001 550
Figure 1. 210Po ingestion rates globally (Data was obtained from Table 1).
Figure 1. 210Po ingestion rates globally (Data was obtained from Table 1).
Sustainability 15 01674 g001
Table
Table 1. Annual 210Po ingestion rates in different countries.
Table 1. Annual 210Po ingestion rates in different countries.
210Po Ingestion Rate (Bq y−1)LocationReferences
1351Alaska—Arctic dwellers[60]
18Buenos Aires, Argentina[61]
1351Canada—Arctic dwellers[62]
68–130China[14]
932Finland—Arctic dwellers[63]
260France[64]
40–62Germany[14,65]
145Greece[64]
20India[14]
126Italy[66]
175–252Japan[67]
37–347 Kuwait[68]
38Leningrad, erstwhile USSR[69]
796–3033Marshall Islands[70]
32–56 Poland[71]
299Portugal[72]
51Romania[14]
54Rostov-on-Don, erstwhile USSR[56]
310Spain[64]
28–44United Kingdom[14]
22United States of America[73]
540USSR—Arctic dweller
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Uddin, S.; Fowler, S.W.; Behbehani, M. 210Po in the Environment: Reassessment of Dose to Humans. Sustainability 2023, 15, 1674. https://doi.org/10.3390/su15021674

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Uddin S, Fowler SW, Behbehani M. 210Po in the Environment: Reassessment of Dose to Humans. Sustainability. 2023; 15(2):1674. https://doi.org/10.3390/su15021674

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Uddin, Saif, Scott W. Fowler, and Montaha Behbehani. 2023. "210Po in the Environment: Reassessment of Dose to Humans" Sustainability 15, no. 2: 1674. https://doi.org/10.3390/su15021674

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