Transfer of ²³⁸U and ²³²Th from soils to tea leaves on Luong My farm, Hoa Binh province, Viet Nam

VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4 (2019) 106-115 106 Original Article  Transfer of 238U and 232Th from Soils to Tea Leaves on Luong My Farm, Hoa Binh Province, Vietnam Hoang Huu Duc1,2, Nguyen Duc Minh2, Phan Viet Cuong3, Le Toan Anh3, Somsavath Leuangtakoun4, Bui Van Loat4,* 1Centre for Environment Treatment Technology, High Command of Chemistry, 282, Lac Long Quan, Tay Ho, Hanoi, Vietnam 2Graduate University of Science and Technology, VAST, 18 Hoang Quoc Viet, Hanoi, Vietnam 3Research and Development Centre for Radiation Technology, Vietnam Atomic Energy Institute, 202A, Street 11, Thu Duc, Ho Chi Minh City, Vietnam 4Department of Nuclear Physics, Faculty of Physics, VNU University of Science, 334 Nguyen Trai, Hanoi, Vietnam Received 30 September 2019 Revised 22 October 2019; Accepted 29 October 2019 Abstract: This paper studies the soil-to-plant transfer factors of natural occurring radioisotopes (238U and 232Th) on Luong My Tea farm, Tan Thanh district, Luong Son commune, Hoa Binh province. The activity concentrations in leaves, trunk and roots of the tea tree at no harvest period (winter break) were determined. The measurements were carried out using gamma spectroscopy with high puritygermanium detector HP(Ge). The research results show that the activity of 238U and 232Th is higher in the tea tree’s leaves than in its trunk and roots. The soil-leave transfer factors (TF) for 238U and 232Th were determined as follows: TFU-238 = 0.52 – 0.87; TFTh-232 = 0.25 – 0.43. Keywords: Luong My Tea farm, transfer factors, soil-leave, trunk. 1. Introduction Transfer of artificial radionuclides along terrestrial food chainshas been studied extensively since thesecond part of the last century,with understandable emphasis on 137Cs since 1986. ________ Corresponding author. Email address: loat.bv58@gmail.com https//doi.org/ 10.25073/2588-1124/vnumap.4398 H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 107 Naturallyoccurring radionuclides have not been studied to the same extent.In the course ofthe last years, however, the interest intheassessment other impacts of these radioactive elements on arable soils, soil microbiota, edible plants and humans has been increasing constantly. Many investigations have been carried out in differentcountries, especially in those where concentrations of naturallyoccurring radionuclides in soils are particularly high [1-3]. The most common terrestrial radioisotopes are 238U, 232Th, and 40K. In this paper, we will discuss the transfer soil to tea tree of two of them: uranium and thorium. Uranium and thorium are major energy sources, which drive the evolution of Earth and Planets. Both these radionuclides are components of the biosphere, and thus occur naturally in all soils and plants, though their concentrations in plants may be rather low. There are numerous reports in literature on biogeochemistry of U and Th. Unfortunately, a large part of available publications refers to the studies performed either in highly contaminated areas or in nutrient solutions that have been artificially ‘spiked’ with radionuclides. Meanwhile, it would be more important to assessthe effects of background levels of natural radioactivity in soil, plants and humans [4-10]. The study of U and Th transfer from soil to edible vegetation through root uptake is very important, especially considering theaccumulation of these radionuclides in the food chains. An understanding of the mobility of U and Th in soils and their transfer to different plants requires a detailed knowledge of U and Th interactions with soil composed of abiotic and biotic components. Despite numerous studies on U and Th contents in vegetation, there is little information yet related to the rate of their uptake and storage by different plant species. Previous experimental results demonstrated that distribution of U and Th in soil is highly variable. For example, activity concentrations of 238U in soil can vary by around three orders of magnitude depending on various factors [10]. Therefore, an assessment of the radionuclide distributions in the soil–plant system may be rather complicated.Many studies haveshown that soil-plant transfer factor for 232Th is smaller than that of 238U [10,11]. In addition, the correlation of concentration of these two radionuclides in soil and plants was assessed by using the Spearman's rank correlation coefficient. This quantity has a value between -1 and 1. A correlation coefficient of 0 (or near 0) means that the two variables have no relation to each other; conversely, if a coefficient of - 1 or 1 means the two variables have an absolute relationship. If the value of the correlation coefficient is negative (<0), that means that when one variable increases, the other decreases (and vice versa); If the correlation coefficient value is positive (> 0), it means that when this variable increases, the other variable increases, and when it decreases, the other variable decreases. The purpose of this work is to determine the TF coefficients of 238U and 232Th, the distribution of concentration activities on the parts of tea plants in Luong My farm. 2. Research object and method 2.1. Sampling area Luong My tea farm was selected for our study. This is a low semi-mountainous area having attitude above sea level of 50-80 m, with slope is about 2-3 %. It has low mountain band which was formed by macma stone, limestone and terrigenous sediment. Climate of this area is typically monsoon tropical. Winter usually is since November to March and summer is from April to October and average rain level is about 1.760 mm. The sampling area is quite flat, height difference between sampling position in comparison to sea level is ignorable. (see Fig.1). H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 108 Fig.1. Mapping of the sampling location, Luong Son, Hoa Binh, Viet Nam. 2.2. Tea tree of Luong My farm As mentioned, theobject of our research is tree tea, its leaf is popularly used to make a drink in Vietnam. Tea tree is usually found in tropical and near tropical climate. It is a neutral one in the young stage while an adult tea tree adapts very well with sunshine. Under shadow, tea leaveshave dark green color and less shoot due to weak photosynthesis. The scattered light in high mountain area has a good influence to tea quality that direct light. In the foggy, wet and cool weather together with temperature difference between day and night are good condition for having high quality tea leaf. Usually, most suitable rainfall for growing up of tea tree is about 1500-2000 mm, air humidity is about 80-85 % is good for tee root growth. For tea trees planted by seed, it normally has tap-root, lateral and absorbed. Tap-root usually has alength of 1 m, depending on the soil character and processing method, manured manner, tea tree age and its species. Tap-root does not exist in tea tree which is planted by using tea branch. The lateral and absorbed root are distributed mainly in the depth from 5 to 50 cm and their horizontal distribution is about two times of tree shadow area. For the tea tree, which is planted by using branches, lateral root is well developed. In the natural growth condition, tea trunk is a single and straight, its branches are arised continuously to form a branch and shot system. In our work, tea trees selected for study are over 20 years (see Fig.2)old which were planted in the period from 1981 to 1995. In this farm, tea tree branches are cutted and tree are fertilized twice per years, one in early season about on February and other on November, at the last of season. Fig.2. Mature tea tree. H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 109 2.3. Sampling method and position In this work, 14 tea trees and corresponding 14 surrounded soil samples were collected from 14 different positions. Distance between sampling positions is about 700-1500m. Soil wassampledat4 points within area of 1 m2 around the tea tree and in 5 depth layers of 10 cm, 20 cm, 30 cm, 40 cm and 50 cm by using special sampling tool (see Figure 3) then removed stone, tree root and putted into plastic boxes. Tea tree samples with full three parts as root, trunk and leaf were washed and then putted in the plastic bag. In 14 sampling positions, 42 samples of the tea tree parts and 70 soil samples in 5 different depth layers were collected. The information about samples and their labels are shown in Table 1. Table 1. Information of the collected samples Position Sample label Tree Soil Leaf Trunk Root Whole tree 10cm 20cm 30cm 40cm 50cm Average of 5 soil layers 1 L1 T1 R1 C1 D1-10 D1-20 D1-30 D1-40 D1-50 D1 2 L2 T2 R2 C2 D2-10 D2-20 D2-30 D2-40 D2-50 D2 3 L3 T3 R3 C3 D3-10 D3-20 D3-30 D3-40 D3-50 D3 4 L4 T4 R4 C4 D4-10 D4-20 D4-30 D4-40 D4-50 D4 5 L5 T5 R5 C5 D5-10 D5-20 D5-30 D5-40 D5-50 D5 6 L6 T6 R6 C6 D6-10 D6-20 D6-30 D6-40 D6-50 D6 7 L7 T7 R7 C7 D7-10 D7-20 D7-30 D7-40 D7-50 D7 8 L8 T8 R8 C8 D8-10 D8-20 D8-30 D8-40 D8-50 D8 9 L9 T9 R9 C9 D9-10 D9-20 D9-30 D9-40 D9-50 D9 10 L10 T10 R10 C10 D10-10 D10-20 D10-30 D10-40 D10-50 D10 11 L11 T11 R11 C11 D11-10 D11-20 D11-30 D11-40 D11-50 D11 12 L12 T12 R12 C12 D12-10 D12-20 D12-30 D12-40 D12-50 D12 13 L13 T13 R13 C13 D13-10 D13-20 D13-30 D13-40 D13-50 D13 14 L14 T14 R14 C14 D14-10 D14-20 D14-30 D14-40 D14-50 D14 Fig. 3. Soil sampling scheme. H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 110 2.4. Sample preparation The collected soil samples were exposed under sunshine for naturally drying. After that, these samples were dried at 1100C in the oven until weight changing less than 1%. The dried soil samples were removed remaining stone by using a sieve with a hole diameter of 1 mm and then ground to achieve the particle dimension of 0.25 mm. Full part tea tree samples were washed carefully to remove the soil and dust by clean water and distilled which then were dried at 1100C and also finely ground to obtain particle dimension of 0.5 mm. The processed samples were mixed carefully to ensure homogeneity and packed in a cylinder box with diameter of 74 mm and height of 30 mm. Weight of soil samples are 180 g and that of tea tree ones are 100 g. All these samples were sealed for 4 week to establish secular equilibrium before measurement. 2.5. Sample measurement and data analysis Samples were measured by the CANBERRA lead shielded-low background gamma spectrometer with high purity germanium detector HPGehaving resolution of 1.86 keV at 1332.49 keV photo-peak of 60Coand relative efficiency is 15 %. In order to accumulate enough statistics and reduce statistical error, measurement time for soil samples was 100.000 second while that for plant were 150.000 seconds. In addition to that, background measurement time was 100.000 seconds. The Geniee 2000 softwarewas used for data acquisition and spectrum analysis. The activities of 238U and 232Th contained in the samples were deduced by mean of our own developed method using only one absolute value of the efficiency at energy of 1460.82 keVcorresponding to characteristics gamma ray of 40K and relative efficiency curve [12]. For each sample, the relative efficiency curve F(E) is constructed based on 295.57 keV and 351.9 keV gamma peaks of 214Pb and 609.31 keV, 1120 keV , 1764.49 keV peaks of 214Bi . The activity of 232Th was extracted by 911.1 keV gamma rays of 228Ac and 583.19 keV gamma ray of 208Tl, respectively. The typical measured gamma spectra of the soiland tea tree samples are shown in Figure 4 and 5. Fig.4. Gamma spectrum of soil sample at position 1 (layer 0-10cm) Fig.5. Gamma spectrum of tea leaf sample at position 1. H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 111 Soil-plant transfer of radionuclides is evaluated using transfer factor (TF) which is defined as theratio betweenthe activity of radionuclides in plant CP(in Bq.kg -1dry plant) and activity of radionuclide in soil CS (in Bq.kg -1dry soil) [13,14]and is calculated as: 𝑇𝐹 = 𝐶𝑃 𝐶𝑆 In addition to that, we have analyzed, including investigation the distribution of U and Th in soil layers, the distribution of U and Th in the tea tree parts (see next session). To evaluate the relationship between U and Th activity in soil and tea, Spearman's rank correlation coefficient was calculated. Uncertainties of all measurements were calculated taking into account random and systematic components of uncertainty, i.e. uncertainties due to sample preparation, efficiency calibration, measurement of sample and nuclear data [15]. The total uncertainty was calculated by uncertainty propagation equation.The uncertainties were presented at the 95% confidence level. 3. Results and discussion Many experimental studies shown that the soil-plant transfer of radionuclide depends very much on the physical and chemical properties of the soil. Therefore, we have first analyzed soil to evaluate the soil character by the laboratory of the University of Science, Vietnam National University, Hanoi and the obtained results are shown in Table 2. Table 2. The physical and chemical properties of the soil at tea farm Luong My Physical and chemical characteristics of research land Sample notation Sand (%) Limon (%) Clay (%) Humus (%) Ca2+ (𝑚𝑒 100𝑔 𝑠𝑜𝑖𝑙⁄ ) Mg2+ (𝑚𝑒 100𝑔 𝑠𝑜𝑖𝑙⁄ ) Fe3+ (mg/kg ) pH D1 22.7 36.5 46.2 3.48 4.04 2.87 84.1 5.86 D2 23.7 38.2 48.1 3.57 4.05 2.98 85 6.21 D3 28.6 46.1 45.3 2.0 6.79 4.23 62 5.96 D4 26.1 46.7 45.1 2.1 6.68 4.13 63.1 6.05 D5 25.6 34.0 40.4 2.11 4.72 3.28 70 6.12 D6 23.3 32.1 41.1 2.0 4.67 3.36 69.2 5.97 D7 18.9 36.5 43.1 2.36 4.34 3.02 79 5.85 D8 19.7 37.1 43.2 2.35 4.2 3.05 78 6.08 D9 26.4 35.2 43.3 3.10 4.02 2.99 80.2 5.89 D10 22.1 34.9 39.1 3.22 4.1 2.89 78.9 6.14 D11 19.8 4.01 40.2 3.41 4.13 2.78 80.2 6.23 D12 20.1 46.2 38.9 3.0 3.98 3.02 75.1 5.75 D13 25.6 39.8 44.5 3.55 4.51 3.1 76.8 5.92 D14 18.8 37.5 46.1 3.05 4.46 3.14 77.8 6.03 With these results, we could conclude that tea tree collected from 14 different positions were grown in the same condition. The activity range in the soil layers of 238U is 20.81 - 48.34 Bq/kg dry. This value of 232This higher, with the activity range: 32.14 - 58.74 Bq/kgdry. U and Th are two radioactive isotopes that have naturally existed in the earth since the formation of the earth. The measured activities of 238U together with 232Th in soil are shown in Fig.6 and as can be seen, these two isotope’s concentration are H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 112 scattered, it means that there isn’t any dependence between them in the soil.This is especially evident when the spearman coefficient is close to zero ( = 0.23). The concentration depth profile analyzing shown that 238U and 232Th aredistributed quite uniformly in different soil layers (see Fig. 7 and Fig. 8). Fig. 6. Scatterplot of 238U versus 232Th concentration in soil (Bq/kg dry). Fig. 7. Concentration of 238U in soil layers. Fig. 8. Concentration of 232Th in soil layers. The concentration of plant radioactive isotopes is usually not linearly related to their concentration in the soil [7, 16, 17]. When analyzing and determining the activity of U and Th in tea leaves, this is clearly seen. While the activity of U in soil is lower than Th, but in tea leaves U is higher (Table 3). 20 30 40 50 60 70 15 25 35 45 55 C o n ce n tr at io n 2 3 2 T h in so il (B q /k g d ry ) Concentration 238U in soil (Bq/kg dry) 0 20 40 60 0 10 20 30 40 50 60 C o n ce n tr at io n 2 3 8 U in so il (B q /k g d ry ) Depth of soil surveyed (cm) 0 20 40 60 80 0 10 20 30 40 50 60C o n ce n tr at io n 2 3 2 T h in so il (B q /k g d ry ) Depth of soil surveyed (cm) H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 113 Table 3.238U and 232Th activity in tea trea (Bq/kg dry) 238U Root Trunk Leaf C1 3.02±0.30 3.68±0.50 20.86±1.2 C2 4.25±0.40 4.64±0.41 22.1±1.6 C3 4.46±0.48 5.51±0.61 26.8±1.2 C4 2.36±0.20 5.63±0.30 19.7±2.1 C5 4.4±0.3 4.91±0.44 20.3±2.3 C6 6.17±0.8 5.23±0.60 19.01±1.4 C7 3.94±0.71 4.31±0.21 25.8 ± 1.2 C8 5.17±0.22 4.44±0.26 24.0± 1.1 C9 5.15±0.40 3.39±0.25 20.1±1.1 C10 3.18±0.26 3.95±0.29 18.8±1.4 C11 4.12±0.42 3.39±0.25 26. 9±1.7 C12 3.21±0.34 4.49±0.36 27.6±2.1 C13 3.01±0.31 3.03±0.25 19.8±2.1 C14 5.69±0.42 7.02±0.51 27.2±2.3 232Th Root Trunk Leaf C1 2.84±0.22 5.11±0.31 14.76±0.91 C2 1.85±0.14 4.34±0.34 12.88±0.87 C3 1.55±0.18 5.82±0.32 16.5±1.2 C4 1.49±0.19 6.51±0.50 15.01±0.89 C5 1.81±0.36 3.42±0.27 16.75±0.77 C6 3.02±0.35 1.54±0.25 17.02±0.79 C7 3.49±0.45 5.21±0.28 13.40±0.59 C8 4.22±0.42 6.10 ±0.29 12.7±1.0 C9 4.11±0.56 9.67±0.24 17.1±1.0 C10 2.26±0.25 3.38±0.21 17.3±1.1 C11 1.98±0.18 4.56±0.22 18.3±1.1 C12 2.13±0.16 8.10±0.25 16.9±1.1 C13 3.11±0.47 4.20±0.19 14.40±0.98 C14 2.56±0.26 8.17±0.14 12.70±0.76 Results showed that the 232Th combination in leaves varied from 12.70 to 18.30 Bq/kg dry, while 238U changed from 18.77 to 27.64 Bq/kg dry. The average activity of 238U in leaves is about 3-5 times higher than that of trucks and roots. Similar to 238U, 232Th is also concentrated mainly in leaves, in trucks and lower in roots. The average activity of 232Th in leaves is about 4 times higher than that in trucks and 6 times higher than that in roots.Thus, the ability to accumulate radioactive isotopes 238U and 232Th on different parts of plants is very different.The research results obtained are consistent with the study results presented in [18, 19], 238U tends to move towards the outer extremities of the tree and accumulates the most in new leaves and sprouts.It however, in order to evaluate the soil-plant transfer of 238U in comparison to 232Th in these tea leaves, we calculated transfer factor (TF), the results are shown in Table 4. The same tree, same growing conditions, but it is clear that the soil to tea leaves transfer of U and Th varies over a wide range. The TF(238U) is 0.52 - 0.87 and TF(232Th) is 0.25 – 0.43.Considering the H.H. Duc et al. / VNU Journal of Science: Mathematics – Physics, Vol. 35, No. 4(2019) 106-115 114 whole survey area, TF(238U) is 2 times higher than TF(232Th).These research results are consistent with many other research ones [6]. Table 4. Transfer factor of 238U and 232Th fromsoilto tea leaves Position TF(238U) TF(232Th) Position TF(238U) TF(232Th) 1 0.61 ± 0.07 0.31± 0.04 8 0.77± 0.08 0.30± 0.04 2 0.69± 0,07 0.26± 0.02 9 0.58± 0.06 0.41± 0.03 3 0.82± 0,08 0.43± 0.07 10 0.51± 0.05 0.38± 0.04 4 0.62± 0,09 0.37± 0.03 11 0.77± 0.06 0.43± 0.04 5 0.67± 0,08 0.40± 0.03 12 0.87± 0.09 0.40± 0.04 6 0.52± 0,05 0.38± 0.03 13 0.67± 0.09 0.30± 0.03 7 0.71± 0,08 0,25± 0.03 14 0.74± 0.09 0.27± 0.03 Average 0.68 0.35 3. Conclusions In our study, concentration of 238U and 232Th in soil and different parts of tea tree at 14 different positions of Luong My tea tree farm and these isotope’s soil-leaves transfer factor were first time determined. We can conclude that there is no correlation between 238U and 232Th in the soil, both U and Th are uniformly distributed in different soil layers. As many other researches, soil-tea leaves transfer of U and Th varies in a wide range and that of U is greater than that of Th twice. References [1] S.B. Chen,Y.G. Zhu, Q.H. Hu, Soil to plant transfer of 238U, 226Ra and 232Th on a uranium mining-impacted soil from southeastern China. J. Environ. Radioact. 82 (2005) 223–236. [2] A. TermiziRamli, A.Wahab, M.A. Hussein, A.Khalik Wood, Environmental 238U and 232Th concentration measurements in an area of high level natural background radiation at Palong, Johor, Malaysia.J. Environ. Radioact. 80 (2005) 287–304. [3] F. Vera Tome, P.B. Rodrigues, J.C. 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