Environmental radioactivity

The environmental radioactivity page is devoted to the subject of radioactive materials in the Human Environment. While some isotopes are only found on earth as a result of human activity (e.g. ⁹⁰Sr and ⁹⁹Tc), and some isotopes are only present due to natural processes (e.g. ⁴⁰K), a few isotopes are present as a result of both natural processes and human activities (e.g. tritium). The concentration and location of some natural isotopes (such as ²³⁸U) can be affected by human activity. For more details of uranium and radium please see Uranium in the environment and radium in the environment.

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Overview

A review of the subject has been published by SCOPE in the report SCOPE 50 Radioecology after chernobyl. This report has seven main subsections.

• Sources of radioactivity
• Case-studies of Significant Radioactive Releases (man made)
• Atmospheric Pathways
• Terrestrial Pathways
• Radionuclide Aquatic Pathways
• Behaviour and Decontamination of Artificial Radionuclides in the Urban Environment
• Dosimetry and the Assessment of Environmental Effects of Radiation Exposure
• Appendices
• References and Bibliography

Background level in soils

Radioactivity is present everywhere (and has been since the formation of the earth). According to the IAEA, one kilogram of soil typically contains the following amounts of the following three natural radioisotopes 370 Bq ⁴⁰K (typical range 100-700 Bq), 25 Bq ²²⁶Ra (typical range 10-50 Bq), 25 Bq ²³⁸U (typical range 10-50 Bq) and 25 Bq ²³²Th (typical range 7-50 Bq).^[1] These values are average values and some soils may varry greatly from these norms.

Sea and river silt

A recent report on the sava river in serbia suggests that many of the river silts contain about 100 Bq kg^-1 of natural radioisotopes (²²⁶Ra, ²³²Th and ²³⁸U).^[2] Also according to the United Nations the normal concentration of uranium in soil is 300 μg kg^-1 to 11.7 mg kg^-1.^[3]. It is well known that some plants are able to absorb and concentrate metals within their tissues (see hyperaccumulators for further detail) and it is known that iodine was first isolated from seaweed in France which suggests that seaweed is an iodine hyperaccumulator.

For instance Busby quotes Garland et al. 1989 who reported the plutonium activity in Welsh inter tidal sediments which suggests that the closer a site is to Sellafield the higher the concentration of plutonium in the silt is. Some relationship can be seen but the scatter of points is large (R² = 0.3683) if the data is fitted to an exponential line.

Man-made

The additional radioactivity in the biosphere caused by human activity due to the releases of man-made radioactivity and of Naturally Occurring Radioactive Materials (NORM} can be divided into several classes.

1. Normal licensed releases which occur during the regular operation of a plant or process handling man-made radioactive materials.
   • For instance the release of ⁹⁹Tc from a nuclear medicine department of a hospital which occurs when a person given a Tc imaging agent expels the agent.
2. Releases of man-made radioactive materials which occur during an industrial or research accident.
   • For instance the Chernobyl accident.
3. Releases which occur as a result of military activity.
   • For example a nuclear weapons test.
4. Releases which occur as a result of a crime.
   • For example the Goiânia accident where thieves, unaware of its radioactive content, stole some medical equipment and as a result a number of people were exposed to radiation.
5. Releases of Naturally Occurring Radioactive Materials (NORM) as a result of mining etc.
   • For example the release of the trace quantities of Uranium and Thorium in coal, when it is burned in power stations

This subject tends to be emotive and controversial, for instance The Low Level Radiation Campaign has a very different view from that held by BNFL.

Farming and the transfer to humans of deposited radioactivity

Just because a radioisotope lands on the surface of the soil, does not mean it will enter the human food chain. After release into the environment radioactive materials can reach humans in a range of different routes, and the chemistry of the element usually dictates the most likely route.

Cows

Jiří Hála's textbook (Radioactivity, Ionizing Radiation and Nuclear Energy, ISBN 807302053X explains how cattle only pass a minority of the strontium, cesium, plutonium and americium they ingest to the humans who consume milk and meat. For instance, for milk if the cow has a daily intake of 1000 Bq of the following isotopes then the milk will have the following activities.

• ⁹⁰Sr, 2 Bq dm^-3
• ¹³⁷Cs, 5 Bq dm^-3
• ²³⁹Pu, 0.001 Bq dm^-3
• ²⁴¹Am, 0.001 Bq dm^-3

Soil

Jiří Hála's textbook states that soils vary greatly in their ability to bind radioisotopes, the clay particles and humic acids can alter the distribution of the isotopes between the soil water and the soil. The distribution coefficient K_d is the ratio of the soil's radioactivity (Bq g^-1) to that of the soil water (Bq ml^-1). If the radioactivity is tightly bonded to by the minerals in the soil then less radioactivity can be absorbed by crops and grass growing in the soil.

• Cs-137 K_d = 1000
• Pu-239 K_d = 10000 to 100000
• Sr-90 K_d = 80 to 150
• I-131 K_d = 0.007 to 50

The trinity test

One dramatic source of man-made radioactivity is a nuclear weapons test. The glassy trinitite formed by the first atom bomb contains radioisotopes formed by neutron activation and nuclear fission. In addition some natural radioisotopes are present. A recent paper (P.P. Parekh, T.M. Semkow, M.A. Torres, D.K. Haines, J.M. Cooper, P.M. Rosenberg and M.E. Kitto, Jorunal of Environmental Radioactivity, 2006, 85, 103-120) reports the levels of long lived radioisotopes in the trinitite. The trinitite was formed from feldspar and quartz which were melted by the heat. Two samples of trinitite were used, the first (left hand side bars) was taken from between 40 and 65 meters of ground zero while the other sample was taken from further away from the ground zero point.

The ¹⁵²Eu and ¹⁵⁴Eu was mainly formed by the neutron activation of the europium in the soil, it is clear that the level of radioactivity for these isotopes is highest where the neutron dose to the soil was larger. Some of the ⁶⁰Co is generated by activation of the cobalt in the soil, but some was also generated by the activation of the cobalt in the steel (100 foot) tower. This ⁶⁰Co from the tower would have been scattered over the site reducing the difference in the soil levels.

The ¹³³Ba and ²⁴¹Am are due to the neutron activation of barium and plutonium inside the bomb. The barium was present in the form of the nitrate in the chemical explosives used while the plutonium was the fissile fuel used.

The ¹³⁷Cs level is higher in the sample which was further away from the ground zero point– this is thought to be because the precursors to the ¹³⁷Cs (¹³⁷I and ¹³⁷Xe) and the cesium to a lesser degree are volatile. The natural radioisotopes in the glass are about the same in both locations.

Activation products

The action of neutrons on stable isotopes can form radioisotopes, for instance the neutron bombardment (neutron activation) of nitrogen-14 forms carbon-14. This radioisotope can be released from the nuclear fuel cycle, this is the radioisotope responsible for the majority of the dose experienced by the population as a result of the activities of the nuclear power industry. For a discussion of the physics of neutron activation see Neutron activation analysis.

Nuclear bomb tests have increased the specific activity of carbon, whereas the use of fossil fuels has decreased it. See the page on Radiocarbon dating for further details.

Fission products

See fission products for more detail, two sources of these radioisotopes is nuclear fallout from atomic bombs and nuclear accidents such as chernobyl. For a good paper about the isotropic signature of the local bomb fallout from a ground burst see T. Imanaka, S. Fukutani, M. Yamamoto, A. Sakaguchi and M. Hoshi, J. Radiation Research, 2006, 47, Suppl A121-A127.

Discharges from plants within the nuclear fuel cycle introduce fission products to the environment, the releases from nuclear reprocessing plants tend to be medium to longlived radioisotopes, this is because the nuclear fuel is allowed to cool for several years before being dissolved in the nitric acid. The releases from nuclear reactor accidents and bomb detonations will contain a greater amount of the shortlived radioisotopes (when the amounts are expressed in activity {Bq}).

Short lived

An example of a shortlived fission product is Iodine-131, this can also be formed as an activation product by the neutron activation of tellurium.

In both bomb fallout and a release from a power reactor accident, the shortlived isotopes cause the dose rate on day one to be much higher than that which will be experienced at the same site many days later. This holds true even if no attempts at decontamination are made. In the graphs below, the total gamma dose rate and the share of the dose due to each main isotope released by the chernobyl accident are shown.

Medium lived

The classic example is ¹³⁷Cs, the cesium is released in bomb fallout and from the nuclear fuel cycle. A paper has been written on the radioactivity found in oysters found in the Irish Sea, these were found by gamma spectroscopy to contain ¹⁴¹Ce, ¹⁴⁴Ce, ¹⁰³Ru, ¹⁰⁶Ru, ¹³⁷Cs, ⁹⁵Zr and ⁹⁵Nb. In addition a zinc activation product (⁶⁵Zn) was found, this is thought to be due to the corrosion of magnox fuel cladding in cooling ponds.^[4] It is likely that the modern releases of all these isotopes from Windscale is smaller.

An important part of the Chernobyl release was the cesium-137, this isotope is responsible for much of the long term (at least one year after the fire) external exposure which has occurred at the site. Also the cesium isotopes in the fallout have had an effect on farming.

A good source of data on the subject of cesium in chernobyl fallout exists at [2], this is the Ukrainian Research Institute for Agricultural Radiology.

A great deal of cesium was released during the Goiânia accident where a radioactive source (made for medical use) was stolen and then smashed open during an attempt to convert it into scrap metal. The accident could have been stopped at several stages; first, the last legal owners of the source failed to make arrangements for the source to be stored in a safe and secure place; and second, the scrap metal workers who took it did not recognise the markings which indicated that it was a radioactive object.

P. Soudek, Š. Valenová, Z. Vavříková and T. Vaněk, Journal of Environmental Radioactivity, 2006, 88, 236-250 report details of the uptake of ⁹⁰Sr and ¹³⁷Cs into sunflowers grown under hydroponic conditions. The cesium was found in the leaf veins, in the stem and in the apical leaves. It was found that 12% of the cesium entered the plant, and 20% of the strontium. This paper also reports details of the effect of potassium, ammonium and calcium ions on the uptake of the radioisotopes.

Cesium binds tightly to clay minerals such as illite and montmorillonite; hence it remains in the upper layers of soil where it can be accessed by plants with shallow roots (such as grass). Hence grass and mushrooms can carry a considerable amount of ¹³⁷Cs which can be transferred to humans through the food chain. One of the best countermeasures in dairy farming against ¹³⁷Cs is to mix up the soil by deeply ploughing the soil. This has the effect of putting the ¹³⁷Cs out of reach of the shallow roots of the grass, hence the level of radioactivity in the grass will be lowered. Also after a nuclear war or serious accident the removal of top few cm of soil and its burial in a shallow trench will reduce the long term gamma dose to humans due to ¹³⁷Cs as the gamma photons will be attenuated by their passage through the soil. The more remote the trench is from humans and the deeper the trench is the better the degree of protection which will be afforded to the human population.

In livestock farming an important countermeasure against ¹³⁷Cs is to feed to animals a little prussian blue. This iron potassium cyanide compound acts as an ion-exchanger. The cyanide is so tightly bonded to the iron that it is safe for a human to eat several grams of prussian blue per day. The prussian blue reduces the biological half life (different from the nuclear half life) of the cesium. The physical or nuclear half life of ¹³⁷Cs is about 30 years. This is a constant which can not be changed but the biological half life is not a constant. It will change according to the nature and habits of the organism for which it is expressed. Cesium in humans normally has a biological half life of between one and four months. An added advantage of the prussian blue is that the cesium which is stripped from the animal in the droppings is in a form which is not available to plants. Hence it prevents the cesium from being recycled. The form of prussian blue required for the treatment of humans or animals is a special grade. Attempts to use the pigment grade used in paints have not been successful.

Long lived

A pair of good examples would be iodine-129 and Tc-99.

Plutonium and the other actinides

In popular culture plutonium is credited with being the ultimate threat to life and limb which is wrong; while ingesting plutonium is not likely to be good for one's health, other radioisotopes such as radium are more toxic to humans. Regardless, the introduction of the transuranium elements such as plutonium into the environment should be avoided wherever possible. Currently the activities of the nuclear reprocessing industry have been subject to great debate as one of the fears of those opposed to the industry is that large amounts of plutonium will be either mismanaged or released into the environment. In the past one of the biggest releases of plutonium into the environment has been nuclear bomb testing.

• Those tests in the air scattered some plutonium over the entire globe; this great dilution of the plutonium has resulted in the threat to each exposed person being very small as each person is only exposed to a very small amount.
• The underground tests tend to form molten rock which rapidly cools and seals in the actinides so rendering them unable to move, again the threat to humans is small unless the site of the test is dug up.
• The safety trials where bombs were subject to simulated accidents pose the greatest threat to people; some areas of land used for such experiments (conducted in the open air) have not been fully released for general use despite in one case an extensive decontamination.

For further details see actinides in the environment.

Natural

Activation products from cosmic rays

Cosmogenic isotopes (or cosmogenic nuclides) are rare isotopes created when a high-energy cosmic ray interacts with the nucleus of an in situ atom. These isotopes are produced within earth materials such as rocks or soil, in Earth's atmosphere, and in extraterrestrial items such as meteorites. By measuring cosmogenic isotopes, scientists are able to gain insight into a range of geological and astronomical processes. There are both radioactive and stable cosmogenic isotopes. These radioisotopes such as tritium, carbon-14 and phosphorus-32.

Production modes

Here is a list of radioisotopes formed by the action of cosmic rays on the atomosphere, the list also contains the production mode of the isotope. These data were obtained from the SCOPE50 report, see table 1.9 of chapter 1.

Transfer to ground

The level of beryllium-7 in the air is related to the sun spot cycle, as radiation from the sun forms this radioisotope in the atmosphere. The rate at which it is transferred from the air to the ground is controlled in part by the weather.

Applications in geology listed by isotope

Applications of dating

Because cosmogenic isotopes have long half-lives (anywhere from thousands to millions of years), scientists find them useful for geologic dating. Cosmogenic isotopes are produced at or near the surface of the Earth, and thus are commonly applied to problems of measuring ages and rates of geomorphic and sedimentary events and processes.

Specific applications of cosmogenic isotopes include:

• exposure dating of earth surfaces, including glacially-scoured bedrock, fault scarps, landslide debris
• burial dating of sediment, bedrock, ice
• measurement of steady-state erosion rates
• absolute dating of organic matter (radiocarbon dating)
• absolute dating of water masses, measurement of groundwater transport rates
• absolute dating of meteorites, lunar surfaces

Methods of measurement for the long lived isotopes

To measure cosmogenic isotopes produced within solid earth materials, such as rock, samples are generally first put through a process of mechanical separation. The sample is crushed and desirable material, such as a particular mineral (quartz in the case of Be-10), is separated from non-desirable material by using a density separation in a heavy liquid medium such as LST (lithium sodium tungstate).

The sample is then dissolved, a common isotope carrier added (Be-9 carrier in the case of Be-10), and the aqueous solution is purified down to an oxide or other pure solid.

Finally, the ratio of the rare cosmogenic isotope to the common isotope is measured using accelerator mass spectrometry. The original concentration of cosmogenic isotope in the sample is then calculated using the measured isotopic ratio, the mass of the sample, and the mass of carrier added to the sample.

References about cosmogenic isotope dating

• Gosse, John C., and Phillips, Fred M. (2001). "Terrestrial in situ cosmogenic nuclides: Theory and application". Quaternary Science Reviews 20, 1475-1560.
• Granger, Darryl E., Fabel, Derek, and Palmer, Arthur N. (2001). "Pliocene-Pleistocene incision of the Green River, Kentucky, determined from radioactive decay of cosmogenic 26Al and 10Be in Mammoth Cave sediments". Geological Society of America Bulletin 113 (7), 825-836.

Radium and Radon from the decay of long lived actinides

Radium and radon are in the environment because they are decay products of uranium and thorium. For further details about thorium see actinides in the environment, for further details of uranium see uranium in the environment while for further details about radium and radon please see radium in the environment.

The radon (²²²Rn) released into the air decays to ²¹⁰Pb and other radioisotopes, the levels of ²¹⁰Pb can be measured. The rate of deposition of this radioisotope is dependent on the weather. Here is a graph of the deposition rate observed in Japan.^[5]

Uranium-lead dating

The uranium-lead radiometric dating scheme is one of the oldest available, as well as one of the most highly respected. It has been refined to the point that the error in dates of rocks about three billion years old is no more than two million years.

Uranium-lead dating is usually performed on the mineral zircon (ZrSiO₄), though it can be used on other materials. Zircon incorporates uranium atoms into its crystalline structure as substitutes for zirconium, but strongly rejects lead. It has a high blocking temperature, is resistant to mechanical weathering and is chemically inert. Zircon also forms multiple crystal layers during metamorphic events, which each may record an isotopic age of the event. These can be dated by a SHRIMP ion microprobe.

One of its advantages is that any sample provides two clocks, one based on uranium-235's decay to lead-207 with a half-life of about 703 million years, and one based on uranium-238's decay to lead-206 with a half-life of about 4.5 billion years, providing a built-in crosscheck that allows accurate determination of the age of the sample even if some of the lead has been lost.

For further details see radiometric dating and exponential decay.

References

Further reading

Radioactivity, Ionizing Radiation and Nuclear Energy, by J. Hala and J.D. Navratil