1. Introduction
The natural radiation exposure on the earth’s surface is a key index of the radiation environmental impact assessment. The natural radiation has two principal sources: high-energy cosmic rays coming from the sun and outer space and natural radionuclides, including terrestrial and cosmogenic radionuclides[1,2]. According to UNSCEAR, irradiation of the human body from external sources is mainly by gamma radiation from radionuclides in the 238U and 232Th series and from 40K[1,2]. The contributions of these radionuclides to the annual effective dose are listed in Table 1.
Natural radiation sources | External exposure dose (mSv) | Percentage (%) | Internal exposure dose (mSv) | Percentage (%) | Total exposure dose (mSv) | Percentage (%) | |
---|---|---|---|---|---|---|---|
Cosmic rays | 0.410 | 17 | — | — | 0.410 | 17 | |
Cosmogenic radionuclides | — | — | 0.015 | 1 | 0.015 | 1 | |
Primordial Radionuclides | |||||||
40K | 0.150 | 6 | 0.180 | 7 | 0.330 | 13 | |
238U series | 0.100 | 4 | 1.239 | 51 | 1.339 | 55 | |
232Th series | 0.160 | 7 | 0.176 | 7 | 0.336 | 14 | |
Total | 0.820 | 34 | 1.616 | 66 | 2.436 | 100 |
The terrestrial radiation level depends mainly on the activity concentration of natural radionuclides in the soils and rocks[4,5]. When it approximates Clarke values (crustal abundance), about 42% of gamma-ray fluence in air originates from 40K, 25% from the 238U series in equilibrium, and 32% from the 232Th series in equilibrium, respectively[6]. Great interest expressed worldwide for the study of naturally occurring radiation and environmental radioactivity has led to surveys in many countries [7-11].There are two traditional methods that have been used to evaluate external exposures of gamma radiation. One is based on dose rate monitoring and the other entails calculating the gamma absorbed dose rate in air using in-situ gamma-ray spectrometry[12-14]. However, a different method, based on geochemical prospecting data, can be utilized to evaluate the terrestrial radiation level in the Chengdu Plain.
2. Theory
2.1 Relationship between gamma absorbed dose rate in air and the activity concentration of radionuclides in soil and rock
If the radionuclides are homogeneously distributed in infinite soil or rock, and gamma-ray attenuation can be ignored for 1 m of air (if the gamma ray energy is 1.0MeV, only 0.88% gamma ray is attenuated through 1 m air), the air kerma rate of a monoenergetic gamma ray 1 m above the ground surface is[15]
where ρ (g·cm-3) is the density of the soil or rock; ci (Bq·g-1) is the activity concentration of the ith radionuclide; μi is the linear attenuation coefficient of soil or rock for a gamma ray emitted from the ith radionuclide; and
Radionuclide in soil or rock | Conversion coefficients of activity concentration | Conversion coefficients of exposure rate and gamma absorbed dose rate | |||
---|---|---|---|---|---|
Radioactive element | Concentration (g·g-1) | Radionuclide | activity concentration (Bq·kg-1) | Gamma-ray exposure rate (μR·h-1)* | Absorbed dose rate (nGy·h-1) |
U | 1×10-6 | 238U(226Ra) | 12.35 | 0.653 | 5.765 |
Th | 1×10-6 | 232Th | 4.06 | 0.287 | 2.494 |
K | 1×10-2 | 40K | 313 | 1.505 | 13.078 |
*1R=2.58×10-4C/kg
2.2. Uranium–radium equilibrium
The data in Table 2 were based on the assumption that the 238U and 232Th series reach secular decay equilibrium. However, it may not be the case for the 238U series. Some decay products of the 238U series may dissociate from the source material, which facilitates their subsequent environmental transfer. For example, 234U may be somewhat deficient relative to 238U in soils and enhanced in rivers or the sea. 226Ra may also have slightly different activity concentration from 238U because of its greater mobility.
The 238U decay chain can be divided into two groups according to the geochemical behavior and the contributions to the gamma radiation level of the radionuclides: the uranium group and the radium group. The uranium group consists of 238U, 234Th, 234Pa, 234U and 230Th. The gamma-ray energy fluence of this group is about 2% of the total in the equilibrium 238U decay series. The radium group is composed of 226Ra and its progeny. At secular equilibrium, the radium group emits about 98% of gamma-ray energy fluence and the main gamma emitter is 214Bi[6]. Ignoring the emanation in soils or rocks, we find that it takes about one month for 226Ra to reach secular equilibrium with 214Bi. Consequently, we can evaluate the gamma absorbed dose in air of the 238U decay series by measuring the total gamma count rate or gamma spectra.
Before using the concentration of uranium to evaluate the gamma absorbed dose rate of the 238U decay series, we need first to convert the concentration of uranium (CU) to the concentration of radioactive equivalent uranium (CeU)[3], which is based on the Ra–U equilibrium constant (ξ). The calibration formula is as follows:
where CeU is the concentration of radioactive equivalent uranium. ξ is the Ra–U equilibrium constant, which can be calculated by using
where CRa is the concentration of radium, which can be easily obtained by using in-situ gamma spectrometry. When the emanation of radon is considered, the concentration of radioactive equivalent uranium (CeU) is given by
where η is the emanation coefficient of radon, defined as the ratio between the concentration of radon into the atmosphere (CRn) and that produced by 226Ra (CRn0). β is defined as the radioactive equivalent uranium ratio:
The 232Th series is a little different from the 238U series. The 232Th series only needs 60 years to reach secular equilibrium. The half-life of 220Rn is 54.5s; so it may not escape from the soil easily. Therefore, in this paper, a secular equilibrium is assumed for the 232Th series for discussion.
3. Geochemical Data and Experiments
3.1 Geological condition of the Chengdu Plain
The Chengdu Plain lies in the west of the Sichuan Basin and to the east of the Tibetan Plateau. It is a compound alluvial fan that was washed by natural rivers originated mostly from the Tibetan Plateau (e.g., the Minjiang River, the Tuojiang River, and the Qingbai River). The western portion abuts the edge of the overthrust of the front Longmenshan Mountain, and the eastern portion borders on Longquanshan Mountain[16,17].
There are three major tectonic units in the Chengdu Plain: the Longquanshan fault zone, the Chengdu Basin, and the Longmenshan fold. These tectonic units are bounded by two NE–SE-trending faults, i.e., the Dayi–Penguan fault and the Pujiang–Xinjing–Deyang hidden fault[18]. The main geological tectonic units of the Chengdu Plain are shown in Fig. 1.
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F001.jpg)
3.2. Geochemical data
The geochemical prospecting data were provided by the Sichuan Geological Survey. The Chengdu Plain was divided into many small quadrate regions of 4 × 4 km and soil or rock was sampled in each quadrate region.
3.3. Determination ofβ
To obtain the concentration of radioactive equivalent uranium (CeU), we must determine the radioactive equivalent uranium ratio β in advance. Dozens of soil samples were collected from the Chengdu Plain, the concentration of uranium was determined by laser-induced fluorometry and that of radium was determined by gamma spectrometry.
Figure 2 shows that there is a linear relationship between the radioactive equivalent uranium ratio and the concentration of uranium in soil or rock, and the adjusted R Square(R2) is 0.64. When the concentration of uranium falls in the range of (0-5) ×10-6g/g (representing 99% of the collected samples), this linear relationship can be written as follows:
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F002.jpg)
Where β is the radioactive equivalent uranium ratio and CU is the concentration of uranium in soil or rock. The concentration of uranium can be converted to the concentration of equivalent uranium (Ceq) as follows:
4. Results
In order to evaluate the gamma absorbed dose rate in air based on geochemical prospecting data, in-situ gamma-ray spectrometry was used to measure the gamma absorbed dose rate in air in an area of section in the Chengdu Plain. The conversion coefficients of the gamma absorbed dose rate in Table 2 were used to calculate the gamma absorbed dose rate 1 m above the surface from geochemical prospecting data. The radioactive equivalent uranium (Ceq) value was calculated using Eq. (7) and was used as the 238U concentration in Table 2. The results are shown in Fig. 3. The average gamma absorbed dose rate in air using in-situ gamma-ray spectrometry is 73.91 nGy/h. The average gamma absorbed dose rate in air using geochemical prospecting data is 80.67 nGy/h. The gamma dose rates obtained by these two methods agree well, indicating that the geochemical prospecting data can be used to evaluate the terrestrial radiation in the Chengdu Plain.
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F003.jpg)
Table 3 lists the activity concentration of 40K, 232Th, and 238U and terrestrial radiation levels in the Chengdu Plain. For comparison, data for China and the earth are also given. As shown in Table 3, the activity concentration of 40K is about one order of magnitude higher than that of 238U or 232Th. For 40K, 232Th, and 238U, the ranges of activity concentration are 179.21–1173.19, 11.78–225.74, and 16.26–224.77 Bq·kg-1, respectively. The gamma absorbed dose rate in air using geochemical prospecting data and the conversion coefficients in Table 2 is in the range of 25.53–177.99 nGy·h-1, with an average of 74.26 nGy·h-1 and a standard deviation of 13.36 nGy·h-1.
Nation or region | Activity concentration of 238U, 232Th, and 40K in soil (Bq·kg-1) | Gamma absorbed dose rate (nGy·h-1) | ||||||
---|---|---|---|---|---|---|---|---|
238U | 232Th | 40K | ||||||
Average value | Range | Average value | Range | Average value | Range | Average value | Range | |
Chengdu Plain | 55.6 | 16.26–224.77 | 57.6 | 11.78–225.74 | 559.1 | 179.21–1173.19 | 74.26 | 25.53–177.99 |
China* | 38.5 | 7.3–449 | 54.6 | 10.3–1844 | 584 | ND–1548 | 81.5 | 11.6–523 |
Earth** | 40 | — | 40 | — | 480 | — | 80 | — |
The terrestrial radiation level in the Chengdu Plain varies greatly, mainly as a result of the differing geological conditions. To analyze the regional variations, isograms of the terrestrial radiation in the Chengdu Plain are shown in Figs. 4, 5, and 6. The main tectonic units of the Chengdu Plain are also marked on these figures.
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F004.jpg)
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F005.jpg)
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F006.jpg)
5. Discussion
The geological condition of the Chengdu Plain has a great impact on the terrestrial radiation level and distribution. As shown in Fig.4, in certain areas of the Chengdu Plain, such as the thrust belts and alluvial fan area, the activity concentrations of 40K are higher than elsewhere. There are two reasons for this difference. First, the thrust belts and Longmenshan fold are covered by forest, where the soil is abundant with humus and the concentration of K is enriched. Second, the alluvial fans are mainly conventional paddy fields, agricultural fertilizers may be a contributor to the elevated 40K concentrations[21]. The distribution of 232Th is shown in Fig.5 and is more homogeneous. However, because of the enrichment process in the clay, 232Th activity concentration in the alluvial fans is slightly higher than elsewhere. Fig.6 shows the distribution of 238U. The activity concentration of 238U is greatly influenced by the major tectonic units; in regions of the Longquanshan thrust belt, the Penguan fault, and the Pujiang–Xinjing–Deyang hidden fault, it is >50 Bq·kg-1.
Because of the high activity concentrations of 238U and 40K, the gamma absorbed dose rates in air in some regions (e.g., the Longquan thrust belt, the Longmenshan fold, and the Pingluoba hidden fault) are higher than elsewhere. The tectonic units with high terrestrial radiation levels are shown in Fig. 7. Moreover, owing to the high activity concentration of 232Th and 40K, the radiation level in the alluvial fans is also higher.
-201710/1001-8042-28-10-013/alternativeImage/1001-8042-28-10-013-F007.jpg)
6. Conclusion
Compared with the measured data by in-situ gamma-ray spectrometry, using geochemical prospecting data to calculate the terrestrial gamma absorbed dose rate in air is efficient and reliable. However, it is necessary to first derive the radioactive equivalent uranium data from the prospecting data. Our results indicate that the average terrestrial radiation level in the Chengdu Plain is slightly lower than the average value of China and the earth, and varies greatly with the complex geological conditions. The gamma absorbed dose rates in air over the fold belts and fault zones are higher than the average, and the activity concentrations of 40K and 232Th in the alluvial sediments of clay are also higher than the averages.
Sources
.(Assessment of health risk levels associated with terrestrial gamma radiation dose rates in Nigeria
. Environ. Int. 27, 21-26 (2001). DOI: 10.1016/S0160-4120(01)00039-3Radiological monitoring: terrestrial natural radionuclides in Kinta District, Perak, Malaysia
. J. Environ. Radioactiv. 100, 368-374 (2009). DOI: 10.1016/j.jenvrad.2009.01.001Determination of terrestrial gamma, 238U, 232Th and 40K in soil along fracture zones
. Radiat. Meas. 44, 116-121 (2009). DOI: 10.1016/j.radmeas.2008.10.001Natural soil gamma radioactivity levels and resultant population dose in the cities of Zacatecas and Guadalupe, Zacatecas, Mexico
. Health Phys. 84, 368-372 (2003). DOI: 10.1097/00004032-200303000-00010Natural radioactivity in Spanish soils
. Health Phys. 66, 194-200 (1994). DOI: 10.1097/00004032-199402000-00010Measurement of gamma radiation levels in soil samples from Thanjavur using γ-ray spectrometry and estimation of population exposure
. J. Med. Phys. 35,48-53 (2010). DOI: 10.4103/0971-6203.55966A comparative study of terrestrial gamma dose rate in air measured by thermoluminescent dosimeter, portable survey meter and HPGe gamma spectrometer
. J. Environ. Radioactiv. 164,13-18 (2016). DOI: 10.1016/j.jenvrad.2016.06.020A general account of the regional geology of Sichuan province
. Regional geology of China. 1, (1990). pp. 8-12. (in Chinese)Natural radiation environment in China
. Int. Congr. Ser.. 1225, 39-46 (2002). DOI: 10.1016/S0531-5131(01)00548-9Radiation exposure due to agricultural uses of phosphate fertilizers
. Radiat. Meas. 43, 1402-1407 (2008). DOI: 10.1016/j.radmeas.2008.04.084.