Department of Nuclear Physics

AMS and Radiation Physics Group University of Lund

RADIONUCLIDE CONCENTRATION IN FUELS AND ASH PRODUCTS FROM BIOFUEL HEATING PLANTS

Bengt Erlandsson Robert Hedvall Sren Mattsson

Department of Nuclear Physics Slvegatan 14 S-223 62 Lund Sweden

Repoit 02/95 LUNFD6/(NFFR-3067)/4-38/tt995) Lund"! 995

O 7

SSI P397.91

RADIONUCLIDE CONCENTRATION IN FUELS AND ASH PRODUCTS FROM BIOFUEL HEATING PLANTS

Redogrelse fr projekt SSI P 397.91 "Mtning av koncentrationen av radioaktiva mnen i biobrnslen och dessas restprodukter" Bengt Erlandsson, Dept. of Nuclear Physics, University of Lund, S-223 62 Lund, Sweden. Robert Hedvall^, Dept. of Radiation Physics, Lund, University of Lund, S-221 85 Lund, Sweden. Sren Mattsson, Dept. of Radiation Physics, Malm, University of Lund, S-214 01 Malm, Sweden.
#

) Present address: Studsvik Nuclear AB, S-611 82 Nykping, Sweden.

Lund December 1994

Contents

1. 2. 3. 4. 5.

Abstract Introduction Investigation sites Time scheme for sampling Instrumentation Results Enrichment factors Activity concentration and generated energy Relation between deposition and activity concentration in fuel The release of radioactive substances to the surroundings Concluding remarks References

6. 7.
8. 9. 10 11. 12.

3 4 5 6 7 7 8 9 10 11 12 14

1. Abstract The activity concentration of the radionuclides K-40, Ac-228, Pa-234, Mn-54, Co-60, Zr-95, Ru-106, Ag-110m, Sb-125, Cs-134, Cs-137 and Ce-144 have been investigated in peat, wood chips and ash products from 13 Swedish district heating plants during the winter seasons of 1986/87,1988/89,1989/90 and 1990/91. There is a significant decrease in the activity concentration of Cs-137 in the fuel which is especially pronounced between the first two seasons, 86/87 and 88/89 after the Chernobyl accident. In spite of the varying deposition of Cs-137 over the country it has been possible to give a relation between the activity concentration in the peat and wood chips as a function of the deposition. The Swedish biofuel heating plants of which 3540 are burning peat and 70-75 wood chips have been divided in three groups according to the activity concentration in the ash products. The mean Cs-137 concentration in ash and the total activity "produced" per year in Sweden have been calculated. The maximum concentration in air at ground level and the corresponding effective dose rate of inhaled Cs-137 as a function of the emission rates of flue gases from stacks with varying heights and during different weather conditions has been calculated.

2. Introduction
The use of biomass fuel has increased rapidly in Sweden during the last decade. After oil and coal, peat and wood chips are the most common fuels used in district heating plants. The energy production from peat burning was 1.1 TWh in 1986 and 3.2 TWh in 1992 and the energy production from wood chips was 3.1 TWh in 1986 and 5.1 TWh in 1992. The total energy production from the district heating plants was 46.9 TWh in 1986 and 47.7 TWh in 1992. Peat and wood chips have thus increased their part in the energy production from 9% to 17%. A total of 3500 kirr of peat land could easily be used in Sweden which equals 2000 TWh. K-40 and radionuclides belonging to the uranium and thorium series are the most prominent natural radionuclides in both peat, wood chips and straw. Fission products from nuclear weapons tests since the I950's are also found. After the Chernobyl accident in April 1986 the deposition of the caesium isotopes Cs-134 and Cs-137 has reached several hundreds of kBq/m^ in some areas of Sweden (SGAB, 1986). It is therefore of importance to decide if peat from contaminated bogs can be used as fuel without exposing workers handling the fuels or ash products or people living near to the plants to too high levels of external and internal radiation. In most cases the emission of radioactive material is a minor environmental problem compared with the emission of sulphur oxides, nitrogen oxides, metals and organic matter. Emissions of such compounds have been studied more thoroughly (Nilsson & Timm, 1983; Rudling & Lofroth, 1980; Pohjola et ai, 1985) than radionuclide emissions. The aim of this investigation is to measure the activity concentration of various radionuclides in the biofuels peat and wood and their enrichment in the combustion process. The activity balance of the radionuclides in the heating plants will also be analysed. The amount of Cs-134 and Cs-137 in ash products produced in power plants per year in Sweden will be calculated. Finally, a simple model will be applied for the calculation of the effective dose from inhalation of stack effluents to a group of persons living in the surroundings of the plant. There is also a component of external exposure. Other ways of increasing the body burden are for example ingestion of food products in areas effected by fall-out from stack emission or by leaching elements from deposits of fly-ash.

3. Investigation sites Samples of biofuel and ash products in the form of grab samples have been taken once a year from 13 heating plants in Sweden. The location of the heating plants is shown in Fig. 1. Their exact locations together with information whether the plant is burning peat or wood-chips are given in Table 1. Several of the heating plants are using fuel from places located up to 100 km from the plant, where the deposition of radio nuclides may be different from that of the plant site and may vary considerably. Therefore a more thorough description of each plant and the area from which the fuel is taken is necessary and will be given below. All deposition values given in the table refer to the total deposition as estimated from an airborne gamma ray survey (SGAB, 1986). It has also to be observed that the true deposition may be a factor of two larger or smaller than the estimated (Edvarson , 1991). 1. ngelholm The plant has two 15 MW boilers and burns both peat and wood.

The peat comes from bogs 110 km NE of ngelholm where the deposition of Cs-137 was 0-2 kBq/m^ and the wood chips from forests 17 km N of ngelholm where the deposition of Cs-137 was 2-3 kBq/m22. Vstervik The plant has one 20 MW boiler and burns wood chips from the

north-eastern parts of Smland and the south-eastern parts of stergtland. The deposition in these areas varied between 3-5 kBq/rrr for Cs-137. 3. Skvde The plant has one 18 MW boiler and burns wood chips from the

surroundings of Skvde, where the deposition was low, 0-2 kBq/irr for Cs-137. This plant is connected to the Regional hospital and is not giving information to the Swedish district heating association. 4. Eskilstuna The plant has one 50 MW boiler and bums wood ships from

forests within a radius of about 100 km to the north of Eskilstuna. In these parts the deposition varied between 10 and 60 kBq/m 2 for Cs-137. 5. Enkping The plant has two 5.8 MW boilers and burns wood chips from

forests within 100 km from Enkping. The deposition of Cs-137 varied from 10 to 60 kBq/m 2 in these areas.

6.

Sandviken

This plant has two 15 MW boilers and burns both peat and wood

chips. The peat comes from bogs about 30 km south of Sandviken, where the deposition of Cs-137 was between 40 and 80 kBq/m 2 (Hedvall & Erlandsson, 1992). 7. Hudiksvall The plant has one 35 MW boiler and bums peat from two bogs at

Ljusdal. The deposition of Cs-137 was 3-10 kBq/m 2 . 8. Hrnsand The plant has one 16 MW boiler and bums peat from bogs about
2

100 km NW of Hrnsand where the deposition was about 30 9. stersund

The plant has two 25 MW boilers and bums peat from Strmsund

100 km north-east of stersund, from Brcke 60 km south of stersund and from Hammarstrand 85 km east of stersund. In the first area the deposition of Cs-137 was 10 to 20 kBq/m 2 , in the second area 3 to 5 kBq/m2 and in the third 30-40 kBq/m 2 . 10. Ume The plant has one 30 MW boiler and burns peat from Trskmyran

about 35 km north of Ume, where the deposition of Cs-137 was 10 to 20 kBq/m 2 . 11. Skellefte The plant has one 25 MW boiler and burns peat and wood chips.

The peat comes from bogs at Rjnoret 50 km to the north of Skellefte, where the deposition of Cs-137 was 2 to 5 kBq/m 2 12. Boden The plant has two boilers, one 25 MW boiler for wood chips and

another 20 MW boiler for peat. Both wood chips and peat come from the surroundings of Boden where the deposition of Cs-137 was 0 to2 kBq/m 2 . 13. Gllivare The plant has one 20 MW boiler for peat. The peat comes from

bogs round Gllivare, where the deposition was 0 to 2 kBq/m . 4. Time scheme for sampling Samples in the form of grab samples have been taken during the winter seasons of 1986/87,1988/89,1989/90 and 1990/91. In Table 1 is given the month and year of the sampling.

5. Instrumentation The activity concentration of the various radionuciides in the samples was determined with a HPGe, or a Ge(Li) detector. The HPGe detector had a relative efficiency of 35.2% and a resolution of 1.78 keV (1.33 MeV). The Ge(Li) detector had an efficiency of 18% and a resolution of 1.88 keV (1.33 MeV). The detectors were placed in lead caves with wall thicknesses of 120-200 mm and the inside of the lead caves were also lined with 10 mm of copper. For the efficiency calibration an ionexchange resin method was used (Bjurman et al., 1987). The samples were first dried and homogenised and then packed into either 60,123, or 180 ml tubs which were placed close to the front of the detector. With this close geometry, summation effects from cascading gamma rays must be taken into consideration. Other difficulties in analysing the gamma ray spectra with interfering peaks were also taken into consideration. For further details see Hedvall & Erlandsson, (1992). 6. Results The activity concentration for the following radionuciides has been measured: K-40, Ac-228, Pa-234, Mn-54, Co-60, Zr-95, Ru-106, Ag-110m, Sb-125, Cs-134, Cs-137 and Ce-144. The first three are naturally occurring and the others are well known from the Chernobyl fallout. Cs-137 does not entirely come from the Chernobyl accident but also from various atmospheric nuclear weapons tests mainly carried out in 1956-58 and 1961-62. Only those radionuciides which have the highest activity concentration throughout the measuring period are given in Tables 2-14. At those places where both fly ash and bottom ash have been measured, the activity concentration of all radionuciides, except K-40 is higher in the fly ash than in the bottom ash. This is probably due to that the enrichment depends on the furnance temperature. The enrichment decreases when the temperature increases. At Sandviken (Table 7) the activity concentration of Cs-134 and Cs-137 is higher in the bottom ash than in the fly ash for the 1988/89 and 1989/90 seasons. A further investigation showed that the bottom ash had a higher content of sand from the furnance, which caused an enrichment of about 4 compared with what it ought to be. The errors given in the tables are only statistical errors originating from the gamma spectrometric measurements and they are small compared with the variations of the activity concentrations both of the fuel and the ash-products. Notice that the time axes in Fig. 2 just marks the different winter seasons. It can be seen in the figure that there is a reduction in the activity concentration with time but with some exceptions. For

wood chips both Eskilstuna and Enkping (Tables 5 and 6) show large variations which cannot be explained by the single sample technique, but most probably reflect variations in the contamination of those areas where the wood chips are coming from. In this case the deposition can vary between 3 and 40 kBq/m . Also for peat there are great variations. For stersund the activity concentrations are 359,502,129 and 241 Bq/kg (Table 10 and Fig. 2). These variations are much larger than those found when a number of samples were taken during the same season. Ravila & Holm, (1994) have found standard deviations of the activity concentrations for wood chips collected from 16 different plants during the 1990/91 season of about 8-12%. For peat Hedvall & Erlandsson, (1992) found variations of 8% for summer samples and 14% for winter samples at Sandviken. Peat is coming from peat bogs within a rather small area. The variations in the activity concentration may therefore not necessarily reflect variations in the deposition but primarily variations in the activity concentration due to changes in the harvesting technique. Surface layers used one year may be followed by deeper layers the next year and then by new surface layers, etc. Variations in depth with 2050 cm may result in variations in the activity concentration of 10-20 times (Hedvall & Erlandsson, 1992)

7. Enrichment factors There is an enrichment of most radioactive nuclides in the ash products because of the loss of organic matter in the combustion process (Table 15). This factor varies with the type of fuel and year, but is on the average 40 times for wood chips and 14 times for peat with a variation of about 50%. These factors are also in agreement with the difference in the ash content which is 2-5% and 5-10% respectively. For Finnish peat, Mustonen et ai, (1989) have found an enrichment factor of 21 for the heating season 1986/87 which is in rather good agreement with 14 found in this investigation if uncertainties are taken into consideration. The statistics from the Swedish District Heating Association contain no information about fuel consumption or asn production. It only gives the produced thermal energy in GWh per year. To estimate the amount of produced ash it is therefore necessary to calculate a factor that converts GWh of thermal energy to kg ash. Ash stands here for the total amount of ash products, both flying- and bottom ash. From some of the plants we have obtained detailed information concerning the amount of used fuel, the amount of produced ash products (kg dry weight) and produced energy (GWh) for the four combustion seasons dealt with in this investigation. The calculated conversion factor is 6 kg ash per MWh for wood chips from Vstervik and 9 kg ash per MWh for wood chips both from Enkping and Boden. The calculated conversion factor is 13 kg ash per MWh and 12

kg ash per MWh for peat from Sandviken and Boden respectively (Table 16). Adopted factors for the other plants are also given in Table 16. The uncertainties for these figures are about 25% depending on the quality of the fuel and the condition of the burner. Based on these factors and the stated energy production, the measured activity concentration (mean value based on the information that the ash is composed of 75% fly ash and 25% bottom ash) the total outgoing activity and the activity per produced thermal energy unit can be calculated (Table 16). The 13 investigated power plants are burning fuel from parts of Sweden with greatly varying deposition of Cs-137 from the Chernobyl accident. It is not possible to calculate individually the activity per produced energy unit for each of all the about 75 power plants. Both peat and wood burning plants have therefore been arranged in three "activity groups". For peat, Sandviken and Hrnsand have been arranged in group I with 250, 200,150 and 150 kBq/MWh for the four heating seasons respectively, stersund and Ume in group II with 150,40,50 and 20 kBq/MWh respectively and Hudiksvall, Skellefte, Boden and Gllivare in group HI with 10,5, 8 and 5 kBq/MWh respectively. For wood chips Enkping and Eskilstuna have been arranged in group I with 50,40, 30 and 35 kBq/MWh respectively, Vstervik and Boden in group II with 15,10,10, and 5 kBq/MWh respectively and ngelholm and Boden in group III with 10, 5,4 and 3 kBq/MWh respectively. The grouping of the other about 60 power plants is based on the total deposition of Cs-137 in the neighbourhood of the plant or on the deposition on areas from where the plant is obtaining its fuel. Wood chips are mostly coming from areas within a radius of about 80 km whereas peat can be transported from bogs far away.

8. Activity concentration and generated thermal energy In Table 17 the total generated thermal energy (GWh per year), the total yearly amount of ash products (kg), the total Cs-137 activity (GBq per year) and the activity concentration (kBq/kg) are given for the different categories of more than 100 plants. For peat ash the calculated mean values for the activity concentration are 5.3,3.5,3.0 and 2.1 kBq/kg for the four sampling seasons and for wood chips the values are 2.2, 1.5, 1.2 and 1.0 kBq/kg respectively. Although these values are adopted and have great uncertainties they reflect the trend of decreasing activity concentration of Cs-137 in the ash products produced in Sweden. Very few power plants are taking their fuel from the same area year after year. For plants burning wood chips a collecting radius of 80-100 km can include areas where the deposition can vary from 1 to 100 kBq/m . For plants burning peat not only the geographical distance to the bogs may very but

also the manner in which the bogs have been harvested are causing great variations in the activity concentration of Cs-137 in the fuel. Nevertheless the mean value of the activity concentration of Cs-137 in the ash products show a reduction of about 50% both for peat and wood chips in the first 5 years after the Chernobyl accident. After that the reduction expressed as the "practical or effective" half life would approach the physical half life of 30 years. 9. Relation between deposition and activity concentration in the fuel As already mentioned the great variations in deposition within the collecting distance from the plant makes it very difficult to find a relation between the activity concentration of Cs-137 in the fuel and a deposition. The "old", pre-Chemobyl Cs137 from the atmospheric nuclear weapons tests was to about 85% deposited during the period 1961-1968. It was also more evenly deposited than the fallout from Chernobyl. The deposition reflects the precipitation and the concentration in the air, which for Cs-137 from weapons fallout as a mean only varied with a factor of two from southern (highest) to northern (lowest) Sweden (DeGeer et a!., 1978). Therefore the variations for "old" Cs-137 within a normal collection radius of 80-100 km ought to be restricted to about 25%. In Table 18 is given the deposition of "old" Cs-137. Based on an activity ratio of O.580.01 for Cs-134/Cs-137 for the Chernobyl deposition (Arntsing et al., 1991) the amount of "old" (DeGeer et al., 1978) and "new" Cs-137 in both fuel and ash products have been calculated. In Table 18 are given the activity concentration of Cs-137 in fuel from the first season 1986/87 and the calculated total deposition of Cs-137. The smaller the old deposition is compared to the new deposition the more uncertain the calculated total deposition is. As the sample values are from one sole grab sample, the uncertainties are also fairly large. Repeated sampling of wood chips gives an uncertainty of 12% (Ravila & Holm, 1994) and for peat the uncertainty is 12-15% (Hedvall & Erlandsson, 1992). Based on these figures we have attached an uncertainty of 25% to the total deposition. The activity concentration of Cs-137 in peat and wood chips as a function of the deposition of Cs137 is shown in Fig. 3. To facilitate the presentation, both axis are exponential and to guide the eye a curve has been drawn. For wood chips the relation between deposition and activity concentration is rather well represented by the curve, whereas for peat no simple relation seems to exist which may be explained by differences in location of the peat bogs but also by differences in the harvesting technique. In the table is also given the deposition from the aerial survey (SGAB, 86). These values are based on reports from the different power plants concerning the area from which the fuel has come. The agreement between the calculated deposition and the measured deposition is quite

good. Therefore it ought to be possible to get a rather good value at least for wood chips of the activity concentration of the fuel from an aerial survey and the curve in Fig. 3 for both peat and wood chips.

10. The release of radioactive substances to the surroundings The escape of radioactive products from the biofuel plant may occur in two ways, either as a deposition of the ashes in certain places or as flue-gases from the stacks. The deposits of the ashes can have varying thicknesses and even if it is several meters thick it hardly constitutes any radiation problem (Ravila & Holm, 1994). It is not possible to calculate how much Cs-137 that is released to the air from what is missing of Cs-137 in the balance between fuel and ash products based on single grab samples. Hedvall & Erlandsson, (1992) have however shown that about (122)% of the Cs-137 activity from a peat-fired heating plant escapes through the stack in the form of flue gases and is discharged into the environment. Mustonen et al, (1989) mention that the long-term average of the collection efficiency for ash products of some Finnish peat-fired power plants has been about 94%. For Sandviken we have also calculated an emission rate of 1 kg/h. We therefore suggest that for Swedish biofuel fired power plants between 1.4% (case 1) and 10% (case 2) of the activity of the ash products is leaving the stacks in the form of flue gases and is then deposited in the surroundings. In Table 19 is shown the emission rates which have been calculated for case 1 and case 2 based on the total Cs-137 activity in the ash products given in Table 17 and the number of plants in the different categories. Using a simple gaussian plume model (Slade, 1968) of the atmospheric dispersion of radio nuclides, the maximum ground level air concentration has been calculated. The calculations have been performed for a wind speed of 4 m/s, for effective stack heights of 20,60 and 100 m and for either Pasquill B- or E-weather conditions. The results are presented in Fig. 4 which can be used to translate a given emission rate into a certain air concentration. As an example an emission rate of 33 Bq/s gives a maximum ground concentration of 2600 }iBq/m . An effective dose at this distance from the stack has a'so been calculated using ICRP 56 (ICRP, 1990) and ICRP 61 (ICRP, 1991) with the assumption that the normal inhalation is 201/min for 24 h (Fig.4). If we assume that the total stack emission is 1 kg/h all year round from a 90 m tall stack, the effective dose would be a few (iSv/a (both internal and external) for a person standing 24h/day

at a spot where the ground concentration is at a maximum. The effective dose would be greater for smaller stacks. Although this is a maximum value from Swedish bio-fuel power plants the dose is very small compared to the dose from natural radiation, mainly from members of the uranium and thorium series (Hedvall & Erlandsson, 1992).

Earlier assumptions have suggested an emission rate of about 40 kg/h from smaller stacks from the Uppsala and Skellefte plants during a 7 month period (Gyllander, 1986), leading to a somewhat smaller maximum dose. Even if we use the inhalation dose factor (in Sv/Bq emitted) for a distance of 1 km from a 20 m tall stack together with our own estimates of the emission rate, Cs-137 has a negligible effect on the effective dose. The absolute maximum from bio-fuel power plants is a few \iSv per year (except for fuels with an extreme uranium and radium content (Hedvall & Erlandsson, 1992)). The dose is negligible compared to the average effective dose contribution in Sweden from natural sources including radon daughters in indoor-air which is about 4mSv per year from all sorts of sources. 11. Concluding remarks Big differences may occur from one year to another in the activity concentration of the fuel and the ash products. This is due to that both wood chips and peat in many cases are transported from places with great variations in the deposition of Cs-137, i.e. Uddevalla was this summer, 1994 importing peat from Scotland and Nykping was importing wood chips from Latvia. It is therefore very difficult to predict the future decrease in the activity concentration of both fuel and ash products or when a certain activity level will be reached. Based on the results presented in this report it would be possible to calculate the activity concentration in ash products from an aerial survey of the deposition via Fig.3 to the activity concentration in wood chips and peat. From these via an enrichment factor found in Table 15 to the activity concentration in various ash products and from there via a calculation of the emission rate and Fig. 4 to a maximum ground concentration and effective dose of Cs-137 for various stack heights and weather conditions. During the 1990/91 season the total air emission through the stacks of Cs-137 from all the heating plants was 1.6 GBq/ year for case 1 and 11.6 GBq/year for case 2 (Table

19) which gives 200 Bq/ MWh and 1550 Bq/MWh respectively. This may be compared with the emission from the stacks of the Swedish nuclear power plants which for 1992 was reported to be 0.4 Bq per produced MWh.

References Amtsing, R., Bjurman, B., De Geer, L-E., Edvardson, L., Finck, R., Jakobsson, S. & Vintersved, I. (1991). Field Gamma Ray Spectrometry and Soil Sample Measurements in Sweden Following the Chernobyl Accident. A Data Report. FOA Report D-20177-4.3 December 1991. Bjurman, B., Erlandsson, B. & Mattsson, S. (1987). Efficiency calibration of Ge spectrometers for measurements on environmental samples. Nucl. Instrum. Meth. Phys. Res., A262, 548-50. De Geer, L-E., Arntsing, R., Vintersved, I., Sisefsky, J., Jakobsson, S. & Engstrm, J. (1978). Paniculate radioactivity, mainly from nuclear explosions, in air and precipitation in Sweden mid-year 1975 to mid-year 1977. Appendix II. FOA Repon C 4OO89-T2(A1) November 1978. Edvarson, K. (1991). Fallout over Sweden from the Chernobyl accident, in The Chernobyl fallout in Sweden, ed. L. Moberg. Swedish Radiation Protection Institute, 1991. Erlandsson, B., Hedvall, R. & Mattsson, S. (1994). Radionuclide concentration in fuels and ash products from biofuel power plants. Report LUTFD2/(TFKF-3OA)/134/(1994). Department of Nuclear Physics, Univ. of Lund, Lund, Sweden. Gyllander, C. (1986). Private communication. Hedvall, R. & Erlandsson, B. (1992). Radioactivity in peat fuel and ash from a peatfired power plant. J. Environ. Radioactivity, 16, 205-28. International Commission on Radiological Protection (1990). Age-dependent doses to members of the public from intake of radionuclides. ICRP Publication 56 Annals of the ICRP. Pergumon Press, Oxford. International Commission on Radiological Protection (1991). Annual limits on intake of radionuclides by workers. ICRP Publication 61 Annals of the ICRP. Pergamon Press, Oxford. Mustonen, R., Reponen, A. & Jantunen, M. (1989). Artificial radioactivity in fuel peat and peat ash in Finland after the Chernobyl accident. Health Phys., 56,451-58. Nilsson, T & Timm, B. (1983). Environmental effects of wood and peat combustion. National Swedish Environmental Protection Board, SNV-1708. (In Swedish) Pohjola; V., Hahkala, M. & Hsnen, E. (1985). Emission inventory of coal, peat and oil-fired power plants. Technical Research Centre of Finland, Research Reports 231. (in Swedish). Ravila, A. & Holm, E. (1994). Radioactive Elements in Forest Industry. Sci. of Total Environ., 157, 339-356.

Rudling, L. & Lfroth, G. (1980). Chemicai and biological characterization of emissions from comustion of peat and wood-chips. National Swedish Environmental Protection Board, SNV-1449. (in Swedish). SGAB (1986). Map of Sweden showing the fallout Levels of Cs-137 after the Chernobyl accident, 1:200 000. Swedish Geological Company, Box 1424, S-75144 Uppsala, Sweden. Siade, D.H. (1968). Meteorology and Atomic Energy. US Atomic Energy Commission Report, TID-24190, Washington DC, USA.

Figure captions Fig. 1 Heating plants in Sweden studied in this investigation and the deposition of Cs137 after the Chernobyl accident. Fig. 2 Variations of the activity concentration of Cs-137 in the fuel and in the fly ash. Fig. 3 The measured activity concentration of Cs-137 in peat and wood chips as a function of the estimated deposition. Fig. 4 The calculated maximum ground concentration and maximum effective dose of Cs-137 as a function of the emission rate for effective stack heights of 20, 60 and 100 m for either Pasquill B- or D-weather conditions.

Table 1. Localization of the biofuel heating plants, type of fuel and sampling time.

Location ngelholm Vstervik Skvde Eskilstuna Enkping Sandviken Hudiksvall Hrnsand stersund Ume Skellefte Boden Gllivare 5615'N; 5715'N; 5824'N; 5922'N; 5939'N; 6036'N; 6144'N; 6238'N; 63H'N; 6350'N; 6445'N; 6548'N; 67O8'N; 1253'E 1653'E 1351'E 1630'E 1705'E 1645'E 1706'F 1755'E 1439'E 2015'E 2100'E 2142'E 2039'E

Fuel p.w Mar 87 Apr 87 May 87 Apr 87 Mar 87 Apr 87 Apr 87 Mar 87 Apr 87 Apr 87 Mar 87 Apr 87 Apr 87

Sampling time Dec 88 Dec88 Dec 88 Dec 88 Dec 88 Dec 88 Jan 89 Jan 89 Jan 89 Dec 88 Jan 89 Nov88 Jan 90 Jan 90 Feb90 Jan 90 Jan 90 Mar 90 Jan 90 Feb90 Feb90 Feb90 Jan 90 Jan 90 Feb91 Feb91 Jan 91 Feb91 Jan 91 Feb91 Jan 91 Feb91 Feb91 Feb91 Jan 91 Jan 91

w
w w w P P p P P P p,w p

p: peat w: wood chips

Table 2. Activity concentration of radionuclides (Bq/kg) found in peat, wood chips and various ash products from the local heating plant at ngelholm.

K-40 1986/87 wood peat fly ash bottom ash wood peat fly ash bottom ash wood peat fly ash bottom ash wood peat fly ash bottom ash n.m. 84 33926 16410 60+6 51 139+26 45020 n.m. 75 22720 45020 428 ... 2184+25 131220

Ac-228 n.m. n.m. n.m. n.m. n.d. 21 722 251 n.m. n.d. 141 181 41 ... 1013 40l

Ru-106 n.m. n.d. 7114 92 63 n.d. 256 n.d. n.m. n.d. n.d. n.d. n.d. ... 84 n.d.

Sb-125 n.m. n.d. 175 31 n.d. n.d. 72 n,d. n.m. n.d. n.d. n.d. n.d. ... n.d. n.d.

Cs-134 n.m. 21 523 10l 31 n.d. 381 81 n.m. n.d. 2+1 31 <1 221 41

Csl37 n.m. 292 73638 141+7 111 13,3+1 472+2 1121 n.m. 191 461 73+1 51 ... 6092 90l

Ce-144 n.m. n.m. n.m. n.m. n.d. n.d. n.d. n.d. n.m. n.d. n.d. n.d. n.d. n.d. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 3. Activity concentration of radionuclides (Bq/kg) found in wood chips and various ash products from the local heating plant at Vstervik.

K-40 1986/87 wood fly ash wood fly ash bottom ash wood fly ash bottom ash wood fly ash bottom ash 6610 2262+123 11810 2083123 102710 9810 1671133 2829150 3015 1777116 2489120

Ac-228 3+2 80+13 3+1 52+2 16+1 412 75+3 69+2 n.d. 42+2 48+1

Rul06 30+6 9001105 n.d. 201+8 n.d. 413 39+5 513 n.d. 1113 n.d.

Sb-125 n.d. 103+8 n.d. 27+3 n.d. n.d. 1212 n.d. n.d. 712 n.d.

Cs-134 24+2 1141159 12+1 364+5 911 411 97+2 5511 2+1 40+1 34+1

Cs-137 7814 3514+180 61+1 176015 42+1 28+1 69714 42412 2311 43+2 37012

Ce-144 n.m. n.m. 511 14613 14+1 1+1 59+2 411 n.d. 4+1 n . d

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 4. Activity concentration of radionuclides (Bq/kg) found in wood chips and various ash products from the local heating plant at Skvde.

K40 1986/87 wood fly ash bottom ash wood ash wood fly ash bottom ash wood fly ash bottom ash 59+10 1650193 1063193 88+9 147I2I 527 1751150 1799150 52+7 121617 1431123

Ac-228 42 45+8 31+5 n.d. 1311 4+1 5213 51+3 411 33+2 60+3

Ru-106 n.d. 309+39 131117 n.d. 36+6 n.d. n.d. n.d. n.d. n.d. n.d.

Sb-125 n.d. 14+1 49+11 n.d. n.d. n.d. 1813 612 n.d. n.d. n.d.

Cs-134 10+1 340118 209111 511 77+2 1.3+0.3 124+3 7612 1.6+0.3 29+1 21+1

Cs-137 24+2 1261+65 794141 2611 43313 2111 103717 65814 14+1 41514 295+3

Ce-144 n.m. n.m. n.m. n.d. 73 n.d. n.d. 1.3+0.2 n.d. n.d. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 5. Activity concentration of radionuclides (Bq/kg) in wood chips and various ash products from the local heating plant at Eskilstuna.

K-40 1986/87 wood fly ash bottom ash wood fly ash bottom ash wood fly ash bottom ash wood fly ash bottom ash 8814 I42781 97753 767 178418 1837118 878 210921 168020 2110 135820 136520

Ac-228 n.m. n.m. n.m. 2.610.3 7213 3211 <3 77+3 7012 211 4212 4211

Ru-106 23+9 684183 1314 613 151111 2.010.3 n.d. 21 n.d. n.d. 2918 n.d.

Sb-125 27+5 118+12 1416 512 6419 5+1 n.d. 64+3 2412 512 2413 211

Cs-134 58+4 1731+90 197110 6511 117715 362+1 9+1 67316 26412 2211 294+5 4311

Cs-137 164+9 4468+229 507+26 273+2 4808+10 152613 5911 4097+5 1680+20 185+3 2753+6 40012

Ce-144 n.m. n.m. n.m. 2+2 18715 1212 n.d. 97+4 5913 n.d. 1913 n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 6. Activity concentration of radion uclides found in wood and a mixture of flyand bottom ash from the local heating plant at Enkping.

K-40 1986/87 wood a s h wood a s h wood a s h wood a s h 4410 1180166 838 1471121 6616 3610+32 6413 1780+29

Ac-228

Ru-106

Sb-125

Cs-134

Cs-137

Ce-144

n.d. n.d. n.d. 813 n.d. 154+4 1 1 1 65+3

309 18471215 1915 197+11 n.d. n.d. n.d. 39114

814 205116 n.d. 10515 n.d. 21+3 212 4215

219+12 7372+381 78+2 122415 13+1 545+3 2311 687+30

555129 179101919 325+10 4978+30 73+2 3314+7 18412 5649111

n.m. n.m. n.d. 151+5 n.d. 51+4 n.d. 13+6

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 7. Activity concentration of radionuclides (Bq/kg) found in peat and various ash products from the local heating plant at Sandviken.

K-40 1986/87 peat fly ash bottom ash peat fly ash bottom ash peat fly ash bottom ash peat fly ash bottom ash 1314 35059 7061101 92 42610 123615 315 566110 1202120 <40 566+10 778120

Ac-228 916 117+42 116+3 411 123+3 6613 3+1 6312 56+2 6111 6312 7212

Ru-106 80120 13101340 70140 12+5 196+8 2119 n.d. 92110 n.d. n.d. 92110 n.d.

Sb-125 30+10 4001100 2516 1012 19014 n.d. 1113 104+4 n.d. 7+2 10414 3112

Cs-134 530170 785011650 2830+720 15011 2998125 6418110 12413 1425+40 2610130 5811 1425140 645110

Cs-137 1150+160 16790+3560 6030+1690 64613 12843113 277201100 74815 8912125 16098116 47413 10777125 537315

Ce-144 21110 250170 1517 1512 n.d. n.d. 312 7+4 n.d. n.d. n.d. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 8. Activity concentration of radionuclides (Bq/kg) found in peat and various ash products from the local heating plant at Hudiksvall.

K-40 1986/87 peat fly ash bottom ash peat fly ash bottom ash peat fly ash bottom ash peat fly ash bottom ash 26+9 29423 23216 30+2 440110 351+10 44 25411 163110 3212 12616 12616

Ac-228 I03 77+12 81+12 n.d. 4511 4612 411 11314 10113 1311 13614 13814

Ru-106 n.d. 43+13 20+6 n.d. 9+3 10+3 813 n.d. n.d. n.d. 1016 n.d.

Sb-125 3+2 4+1 n.d. n.d. 4+1 311 n.d. 19+3 n.d. n.d. n.d. n.d.

Cs-134 1612 14218 10516 411 44+1 36+1 811 7712 38+1 211 2111 2411

Cs-137 49+3 551+30 348118 2611 290+2 231+2 55+1 620+4 28012 28+1 28213 298+3

Ce-144 n.m. n.m. n.m. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not delected

Table 9. Activity concentrations of radionuclides (Bq/kg) found in peat and in various ash products from the local heating plant at Hrnsand.

K-40 1986/87 peat fly ash bottom ash n.m. 33636 3824

Ac-228 n.m. n.m. n.m.

RulO6 14028 18311237 175144

Sb-125 531O 857+68 100+18

Cs-134 1183+62 13950+722 2019+105

Cs-137 29211150 34480+1769 50051258

Cc-144 n.m. n.m. n.m.

nun.:

not measured

Table 10. Activity concentration of radionuclides (Bq/kg) found in peat and various ash products from the local heating plant at stersund.

K-40 1986/87 peat fly ash bottom ash peat fly ash bortoir ash peat 1) peat 2) fly ash bottom ash peat 3) fly ash bottom ash 39+15 n.d. 91795 4414 45210 121010 345 233 43920 121450 66 52911 1207ll

Ac-228 S+4
.i..

Ru-106 n.d. 6511 n.d. n.d. 428 104 105 n.d. 217 n.d.

Sb-125 n.d. 194 n.d. 42 383 21 n.d. n.d. 163 n.d. 41 173 n.d.

Cs-134 12316

Cs-137 3595

Ce-144 n.d.

n.m.
23310 11012 553110 27915 2011 8+1 28315 8611 2911 207+5 7111

n.m.
690+29 50215 2468+5 1323+10 129+2 65+1 1854110 56616 24112 1766+5 61012

n.m.
n.d. n.d. 2.3+0.3 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.

193 n.d. 312 231 91 51 552 2610 21 332 251

1988/89

1989/90

1990/91

53
146 n.d.

n.m.: not measured n.d.: not detected

Table 11. Activity concentration of radionuclides (Bq/kg) found in peat and wood chips and a mixture of these with 70% peat and 30% wood and ash from the local heating plant at Ume.

K-40 1986/87 peat wood ash pcat+wood ash pcat+wood ash pcal+wood ash 6510 107 39230 586 74515 283 1129140 n.m. 41010

Ac-228 n.d. n.d. n.d. 51 983 n.d. 424 n.m. 464

Ru-106 n.d. n.d. 294+51 n.d. 2310 n.d. 2822 n.m. n.d.

Sb-125 62 93 19626 n.d. 424 1+1 232 n.m. 16830

Cs-134 975 226119 4779+247 291 83910 191 1164110 n.m. 253+4

Cs-137 271+30 573114 122601629 13112 3788+8 13212 7375122 n.m. 2185+7

Ce-144 n.d. n.d. n.d. n.d. 3+1 n.d. 2+1 n.m. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not delected

Table 12. Activity concentration of radionuclides (Bq/kg) found in peat and various ash products from the local heating plant at Skellefte.

K-40 1986/87 peat fly ash bottom ash pcai fly ash bottom ash peat fly ash bottom ash peat fly ash bottom ash 99 2592 82248 212 39719 1087111 364 64012 n.m. 302 3177 105320

Ac-228 n.d. n.d. n.d. 11 2ll 191 61 181 n.m. 41 221 161

Ru-106 n.d. 104123 188 n.d. n.d. n.d. n.d. n.d. n.m. n.d. n.d. n.d.

Sb-125 n.d. 419 n.d. n.d. 102 n.d. n.d. 92 n.m. n.d. 82 n.d.

Cs-134 71+4 920148 533128 2211 18112 65+1 811 14212 n.m. 811 8611 611

Cs-137 187110 2374+22 1366170 11412 94613 34011 5811 1016+10 n.m. 6912 83713 6312

Ce-144 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.m. n.d. n.d. n.d.

1988/89

1989/90

1990/91

n.m.: not measured n.d.: not detected

Table 13. Activity concentration of radionuclides (Bq/kg) found in peat, wood chips and various ash products from the local heating plant at Boden.

K-40 1986/87 peat fly ash bottom ash wood fly ash bottom ash 1988/89 peat fly ash bottom ash wood fly ash bottom ash 1989/90 peat fly ash bottom ash wood fly ash bottom ash 1990/91 peat fly ash bottom ash wood fly ash bottom ash 1219 481129 19213 2411 1942107 1351+81 475 54910 93717 7610 1801127 1019110 4014 600125 953+10 42+10 1841150 1615120 1813 714110 960110 4013 2230+4 1720122

Ac-228 6+3 3516 8+2 3+3 78+12 93116 n.d. 2511 1611 n.d. 4813 1214 211 2112 2111 111 5012 53+2 n.d. 2711 18+1 211 58+3 48+2

Ru-106 n.d. 190+25 92121 n.d. 109+16 12+4 n.d. 1313 n.d. n.d. 50+8 20+8 n.d. 1015 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.

Sb-125 n.d. 16+3 n.d. n.d. 21+4 n.d. n.d. 711 n.d. n.d. 15+2 211 n.d. 612 n.d. n.d. 812 n.d. n.d. n.d. n.d. n.d. n.d. n.d.

Cs-134 711 199+11 38+2 16+1 345+18 113+7 311 73+1 32+1 3+1 18413 15+1 5+1 60+1 3511 2+1 90+2 2811 1+1 17+1 5+1 111 88+2 4011

Cs-137 3712 887+46 141+7 46+3 1268+ 65 389121 2211 47812 200+22 1911 1100+6 10811 5111 58613 33813 1311 82213 257+3 711 293+2 79+2 811 1106+6 49513

Ce-144 n.m. n.m. n.m. n.m. n.m. n.m. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.

n.m.: n.d.:

not measured not detected

Table 14. Activity concentration of radionuclides (Bq/kg) found in peat and various ash products from the local heating plant at Gallivaie.

K-40 1986/87 peat fly ash peat fly ash peat fly ash peat fly ash 2211 288119 164 65610 30l 38410 n.d. 5591S

Ac-228 n.d. n.d. n.d. 20l n.d. 211 21 30l

Ru-106 n.d. 72111 n.d. 613 n.d. n.d. n.d. n.d.

Sb-125 n.d. 1012 n.d. 3+1 n.d. n.d. n.d. n.d.

Cs-134 1111 95+5 31 26+1 2+1 8+1 1+1 1+1

Cs-137 53+3 469+20 2511 28312 2411 26811 411 70+1

Ce-144 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.

188/89

1989/90

1990/91

n.d.:

not detected

Table 15. Enrichment factors of fuel to fly- and bottom ash. Figures within brackets are not reliable.

86/87 flyash Vstervik wood wood wood wood wood wood wood wood K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs K-40 Cs 34 47 28 43 16 29 bot. ash ....

88/89 flyash 18 31 bot ash 9 1 17t 16t 24 6 18t 16t 155 43 12 9 nm nm 28 3 nm nm nm nm 13t 29t 52 3 20 10 13 6

S9/90 flyash 17
DOL

90/91 flyash (59) 20 23 25 65 14 bot ash (83) 17 28 18 65 2 28t 31t nm 11 4 12 nm nm (201) 3 nm

mean

ash 2: 15 36 85 19 (29) 55t 44t nm nm 41 5 nm nm 45 8 nm nm nm nm 40t 58l nm nm 24 7 38 17 nm nm

25 35 72
24 (72)

31+12

Skvde

18 27 11 3 27t 33t 54 5 9 7 2 2 24 2 6t 47t 39t 21t nm nm 91 8 16 5 56 8

...

4724

Eskilstuna

23 18

2O8

Enkping

...

...

...

...
47 20 15 11

Sandviken

peat peat peat peat

peat peat peat peat peat

27 15 11 10 12 12

nm nm 64 11 nm nm 13 14 nm nm nm nm

nm 23 4 11 nm nm (88) 7 nm nm nm nm nm nm 11 12 40 29 56 113 nm 18

194

Hudiksvall

Ill

Hrnsand

nm nm
10 5

stersund

nm nm

95

Ume

peat wood wood

pejit+wood peal+wood Skellefte peat peat peat peat wood wood Gllivare peat peat

nm nm nm nm

nm nm
29 13 40 26 81 25 13 9

nm nm nm nm nm
35 1 134

19 8 12 23 24 60 41 10

18 18 15 12 44 53 13 8

Boden

53 8 43 51 nm nm

237

6337

nm nm

nm nm

115

nm: not measured

t: total fly- and bottom ash

Table 16. Conversion factor for total produced ash (kg/MWh) which is either calculated or adopted, total activity per year (MBq) and activity per produced energy unit (kBq/MWh) of Cs-137.

Con. fac.
(kg/MWh) 86/87 Wood chips ngelholm Vstervik Skvde Eskilstuna Enkping Boden Peat Sandviken Hudiksvall Hrnsand stersund Skellefte Boden Gllivare Mixed Ume 12 (a) 26 13 (c) 12 (a) 12 (a) 12 (a) 12 (a) 10 (c) 12 (a) 24.7 0.82 10.1 2.45 0.85 0.51 7 (a) 7 (c) 7 (a) 9 (a) 9 (c) 9 (a) 0.08 3.57 6.42 11.0 0.90

Total activity
(GBq) 88/89 0.22 1.39 7.61 2.02 0.65 89/90 0.02 0.64 8.11 0.69 0.86 90/91 0.38 0.46 5.65 2.49 1.33

Activity per energy unit

(kBq/MWh) 86/87 3.9 25 8.0 31 161 0.4 88/89 2.7 10 3.0 36 45 7.7 89/90 0.4 4.4 6.6 31 30 6.1 90/91 3.4 2.9 2.7 19 51 8.6

22.5 0.42 3.89 0.70 0.50 0.30

11.9 0.78 2.57 0.73 0.39 0.31

16.5 0.43 1.86 0.66 0.16 0.09

197 6.6 325 25 7.0 4.7

196 3.6 29 9.5 4.1 2.8

130 7.1 18 10 5.2 2.7

130 3.8 18 8.1 2.4 0.7

7.0

12

2.6

147

45

89

26

(a) adopted (c) calculated information missing

Table 17. Total generated thermal energy, total amount of ash products produced per year, total Cs-137 activity per year and activity concentration from 13 Swedish power plants. Peat Category I: Sandviken and Hrnsand, II: stersund and Ume, III: Hudiksvall, Skellefte, Boden and Gllivare. Wood chips Catgory I: Enkping and Eskilstuna, II: Vstervik and Boden, III: ngelholm and Skvde.

Category

86/87 88/89 89/90 90/91 86/87 88/89 89/90 90/91 (GWh) (GWh) (GWh) (GWh) (GBq) (GBq) (GBq) (GBq) (lO^g) (lO^g) U0kg) (iokg) (kBq/kg) (kBq/kg) (kBq/kg) (kBq/kg) 199 2.39 265 3.18 1121 13.5 1585 19.0 436 3.49 1239 9.91 1658 13.3 3333 26.7 252 3.02 645 7.74 1052 12.6 1949 23.4 400 3.20 1184 9.47 1501 12.0 3085 24.7 232 2.78 944 11.3 1466 17.6 2642 31.7 430 3.44 1226 9.81 1809 14.5 3465 27.7 286 3.43 1257 15.1 1478 17.7 3021 36.3 579 4.63 1579 12.6 2261 18.1 4419 35.4 50 20.9 40 12.6 11 0.8 101 5.3 22 6.3 19 1.0 17 1.2 58 2.2 50 16.5 26 3.4 5 0.4 81 3.5 16 5.0 12 1.3 8 0.7 36 1.5 35 12.6 47 4.2 12 0.7 94 3.0 13 3.8 12 1.2 7 0.5 32 1.2 43 12.5 25 1.7 7 0.4 75 2.1 20 4.3 9 0.7 7 0.4 36 1.0

peat I

I I

I I I
total

wood chips I

II

III
total

Table 18. Activity concentration of Cs-137 in the fuel, pre-Chemobyl (old) activity of Cs-137, calculated old deposition, calculated total deposition and estimated deposition of Cs-137 from the aerial survey (SGAB, 1986).

Act. cone. (Bq/kg) Wood chips ngelholm Vstervik Skvde Eskilstuna Enkping Boden Peat Sandviken Hudiksvall Hrnsand stersund Skellefte Boden Gllivare Mixed Ume 277 1089 50 2921 367 191 39 54 12 80 25 168 567 47

Old

Old deposition (kBq/m2)

Deposition aerial survey (kBq/m2)

(%)

758 196 347 75 42 327

1.4 0.9 1.15 1.15 1.1 0.65

0-2 2-5 0-2 3-10 5-30 0-2

21 328 4 106

81
438 6215

1.05 0.85 0.8 0.8 0.7 0.65 0.8

20-60 2-5 30-40 2-10 2-10 0-2 0-2

74

0.9

10-20

Cs-137(kBq/m2)
>100 60-100 30-60 3-30

- / Enkping Eskilstuna

Fig. 1 Heating plants in Sweden studied in this investigation and the deposition of Cs137 after the Chernobyl accident.

KT-

ngelholm Vstervik o Skvde

o Enkping Eskilstuna

o Sandviken Hudiksvall

o Hrnsand stersund

Skellefte Umefi

Boden,peat Boden,wood 0 Gllivare

V
10 peat wood fly ash -\ 1 1 h-TH 1 1 1 1

1 90/91 I 86/87

86/87

88/89

90/91 I 86/87

88/89

90/91 I 86/87

88/89

1 1 h 88/89 90/91 I 88/89 86/67

iI\90/91 i 86/87 88/89 90/91

Fig. 2 Variations of the activity concentration of Cs-137 in the fuel and in the fly ash.

1 o Hr / /

Cs-137
o peat x wood chips mix
/ "o" pa
'

o San

_ 1000 -

/
x Enk

Ume/

e
u
C o

I 100

/ x Vs o Gl o Bod /

<

o Hud x Bod / o st 'x Sk

o Ske
/ x ng

10
:

i 1

10 Deposition
Fig. 3 The measured activity concentration of Cs-137 in peat and wood chips as a function of the estimated deposition.

100

10000

1000

1000 -

o
CQ C
4-

w
re

a. o
vi

et

c o
T3 C 3 O
ro

0.01

1 Emission rate

10 (Bq/s)

100

Fig. 4 The calculated maximum ground concentration and maximum effective dose of Cs-137 as a function of the emission rate for effective stack heights of 20, 60 and 100 m for either Pasquill B- or D-weather conditions.