Geochemical Characteristics and Influencing Factors of Soil Selenium in Longzi County, Tibet Autonomous Region
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摘要:
硒是人体必需的微量元素之一，土壤中的硒含量与人体健康关系密切。调查土壤硒含量分布特征、圈定富硒土壤资源分布区、查明土壤硒含量影响因素，对于推动富硒土地资源开发利用、发展富硒农牧产业、预防地方疾病等均具有重要意义，也可为土壤硒背景值研究提供参比资料。土壤硒是当前热点研究领域，国内外对土壤硒研究已有很多，然而西藏地区有关土壤硒方面研究资料非常有限。本文选择西藏自治区隆子县重点耕地区为研究对象，系统采集表层土壤、垂向剖面、岩石样等样品，采用原子荧光光谱法(AFS)、容量法(VOC)、电感耦合等离子体发射光谱法(ICP-OES)等方法测定土壤中的硒、有效硒、有机质、全磷等含量指标，利用统计方法对研究区土壤硒、有效硒等地球化学含量特征及影响因素进行初步探讨。结果表明：①研究区表层土壤硒含量范围为0.14~1.51mg/kg，中位数为0.44mg/kg，是西藏土壤硒平均值(0.15mg/kg)的2.9倍和中国表层土壤Se平均值(0.26mg/kg)的1.5倍，表明研究区表层土壤中全硒含量较高；研究区表层土壤中有效硒含量范围为0.8~26.8μg/kg，中位数为9.2μg/kg，土壤有效硒占全硒含量的0.21%~5.79%；土壤硒含量高于0.4mg/kg为界限值，研究区总面积的77.25%符合富硒土壤划定标准，表明富硒土壤资源丰富；②研究区广泛分布的涅如组(T3n)和日当组(J1r)地层发育土壤中硒含量较高，中位数分别为0.44mg/kg和0.41mg/kg，土壤硒含量与地质背景密切相关；土壤理化性质包括有机质、pH、TFe2O3等对土壤全硒含量影响不显著，但土壤有效硒与有机质、pH、N、P、碱解氮、有效磷、速效钾、阳离子交换量(CEC)呈显著正相关；此外，铁氧化物(TFe2O3)对有效硒含量也有一定控制作用；③土壤垂向剖面研究发现，土壤硒含量还与表生富集作用有关。综合认为，研究区土壤Se含量较高，富硒土壤资源丰富，可以通过土壤养分管理，进一步提高土壤硒生物有效性。
Abstract:BACKGROUND Selenium (Se) is one of the essential trace elements in the human body, which has many biological functions. Insufficient or excessive intake of Se will cause a series of diseases. The trace element Se in the human or animal body cannot be synthesized by itself, but can only be supplemented from external food. Se in food, especially in plant food, mainly comes from soil. Therefore, Se in soil is closely related to human health and animal growth. China is a country lacking in soil Se content, especially in Tibet. The background value of soil Se in Tibet is significantly lower than that of surface soil in China. Therefore, local diseases such as Kashin-Beck disease are common in some areas of Tibet due to long-term insufficient intake of selenium. It is of great significance to investigate the distribution characteristic of soil Se content, delineate the distribution area of selenium-enriched soil resources and determine the influencing factors of soil Se content for promoting the development and utilization of selenium-enriched land resources, develop Se-enriched industries and prevent local diseases. This will also provide reference data for the research of soil Se background value.
OBJECTIVES In recent years, it has been a hot topic to investigate the content of Se in soil, to delineate selenium-enriched soil resources and to develop and utilize them. Tibet is the main part of the Qinghai—Tibet Plateau, which has complex and diverse soil parent materials and soil forming processes, forming unique alpine soil types. In addition, Tibet is one of the areas with the least influence of human activities and is the ideal place for environmental geochemistry research. However, due to many factors such as natural geographical location and climate, the research data of soil element geochemistry in Tibet is very limited, and research data of soil Se is rare. Thus, the characteristics, distribution and influencing factors of soil Se content in the study area were studied, to provide a basis for the exploitation and utilization of selenium-enriched land resources, the development of selenium-enriched industry and the prevention of endemic diseases in the frontier ethnic areas of the plateau.
METHODS The collection, processing and analysis of samples of surface soil, vertical profile and rock profile were carried out. The samples were collected from the key farming area of Longzi County, Shannan, Tibet Autonomous Region. The surface soil samples were collected in a grid pattern from the third national land survey map spot. The soil sampling points were mainly arranged on agricultural plots, with an average sampling density of 7.9 points/km2. A total of 1587 surface soil samples were collected, with a study area of 200km2. The sampling method for surface soil samples was determined according to the actual plot shape. When the plot was square, "X" type sampling was adopted, and when the plot was rectangular, "S" type sampling was adopted. When sampling cultivated land, 5 sub-sampling points were equally combined into 1 sample; for grassland and woodland sampling, 3-4 sub-sampling points were equally combined into one sample. The samples collected at each sub-sampling point were crushed, small stones, roots and other sundries picked out, and after fully mixing, more than 1000g samples reserved and put into sample bags by quartering method. In the study area, 10 vertical soil profiles were set up, and the sampling interval was 1 sample/20cm. The depth of all the profiles was 160cm except for the profile CM01, which was 140cm deep. In addition, a rock profile was set in the study area, and fresh rock samples were collected. The same kind of rock was collected in a multi-point mode and combined into a sample, with the sample weight of 300g. The surface soil samples, and vertical profile samples collected were naturally dried without pollution, and sieved by -10 mesh nylon sieve, then divided by quartering method, weighed and put into sample bottles and sent to laboratory for analysis. Soil samples were analyzed for Se, available Se, organic matter, pH, N, P, available N, available P, available K, etc. Rock samples were analyzed for Se. The contents of Se and available Se were determined by atomic fluorescence spectrometry (AFS), organic matter. Available nitrogen and cation exchange capacity (CEC) were determined by volumetric method (VOL), pH value was determined by ion selective electrode method (ISE), N content was determined by elemental analyzer method (EA), and available P, available K, P and TFe2O3 were determined by inductively coupled plasma-optical emission spectrometry (ICP-OES). The detection limit, accuracy, precision and reporting rate of the analytical method adopted all met the specification requirements, and the sample analysis quality was reliable.
RESULTS The results of the content of Se in soil and its influence factors, showed that: (1) The Se content in the topsoil of the study area ranged from 0.14 to 1.51mg/kg, with a median of 0.44mg/kg, which was 2.9 times as high as the average value of Tibet (0.15mg/kg) and 1.5 times as high as the average value of China (0.26mg/kg). The content of available Se in the topsoil ranged from 0.8 to 26.8μg/kg, with a median of 9.2μg/kg. The content of available Se in topsoil was 0.21%-5.79% of total Se. (2) Se-enriched (Se≥0.4mg/kg) soil resource area was 154.53km2, which accounted for 77.25% of the total area. Se-enriched soil was mainly distributed in Longzi Town and Ridang Town. There was no excess or deficiency of soil Se in the study area, which indicated that Se-enriched soil was continuous and had the potential to develop Se-enriched soil resources. (3) The geological background was closely related to the Se content in the soil. The Se rich soil was mainly controlled by the distribution of the Nieru Formation (T3n) and the Ridang Formation (J1r). The median Se content in the soil developed from the Nieru Formation (T3n) and the Ridang Formation (J1r) was 0.44mg/kg and 0.41mg/kg, respectively. Analysis of Se content in rock samples showed that Se content ranged from 0.07 to 11.00mg/kg, with an average of 1.65mg/kg. Se content was high in sericite slate and shale, which further proved that Se-enriched soil was closely related to its parent rock. (4) Soil physical and chemical properties including organic matter, pH, TFe2O3 had no significant effect on soil Se content, but soil available Se was positively correlated with organic matter, pH, N, P, alkali-hydrolyzable N, available P, available K, CEC content. There was a positive correlation between the content of organic matter and the content of available Se (R2=0.2792, P < 0.01), and between the content of organic matter and the ratio of available Se to total Se (R2=0.2597, P < 0.01). There was a positive correlation between soil available Se and pH (R2=0.103, P < 0.01). According to the soil pH grading standard, the availability of Se increased gradually from acid to alkaline soil, but in strong alkaline soil, the availability began to decrease due to the methylation reaction of Se. There was a negative correlation between available Se and TFe2O3 (R2=-0.346, P < 0.01). In the study area, the content of soil available Se had significantly positive correlation with the content of N, P, alkali-hydrolyzable N, available P and available K, which indicated that the increase of N, P and K content could significantly improve the bioavailability of soil selenium, which had a certain theoretical significance for the artificial control of soil Se content. (5) 10 vertical soil profiles were constructed in different areas of the study area, and the depth of the other profiles was 160cm except for the CM01 profile, which was 140cm. In that vertical soil profile, the content of Se and available Se decreased with the increase of soil depth. The content of Se in the soil below 100cm was less than 0.4mg/kg, and the content of available Se in the soil at 160cm was 60% less than that in the surface soil.
CONCLUSIONS The content of Se in the topsoil of the study area is high, and 77.25% of the study area is in line with the standard of Se-enriched soil. In that soil, the Se content is mainly affected by the parent materials, especially the sericite slate and shale in the Nieru Formation (T3n) and Ridang Formation (J1r). The land use type has little effect on Se content and distribution. Physical and chemical properties of the soil, such as organic matter, pH, N, P, available N, available P, available K and CEC, have little effect on total Se content, but soil available Se is significantly positively correlated with organic matter, pH, N, P, alkali-hydrolyzable N, available P, available K and CEC. Soil nutrient management can further improve bioavailability of soil selenium. Only the characteristics and influencing factors of soil Se content in Longzi County, Tibet Autonomous Region, were discussed, in order to provide a geological basis for the development and utilization of Se-enriched land resources. However, the process of Se uptake by crops is a very complex biogeochemical process, and is affected by many factors. Therefore, it is necessary to further strengthen research on the characteristics of Se content and its migration and transformation in soil-crop system.
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表 1 土壤样品分析方法及检出限
Table 1. Analytical methods and detection limit for soil samples
分析指标 分析方法 样品处理方法 检出限要求
(mg/kg)检出限
(mg/kg)方法依据 Se 原子荧光光谱法(AFS) 王水加热消解，盐酸浸提 0.01 0.01 WHCS-FF-CS/04—2019 有效硒 原子荧光光谱法(AFS) 沸水浸取 - 0.0005 WHCS-FF-CS/22—2019 有机质 容量法(VOL) 浓硫酸加热消解 0.17 0.034 NY/T 1121.6—2006 pH 离子选择性电极法(ISE) 无二氧化碳水浸取 0.1 0.1* WHCS-FF-CS/19—2019 TFe2O3 电感耦合等离子体发射光谱法(ICP-OES) 四酸加热消解，盐酸浸提 0.05 0.02 WHCS-FF-CS/02—2019 N 元素分析仪法(EA) 固体燃烧 20 15 WHCS-FF-CS/12—2019 P 电感耦合等离子体发射光谱法(ICP-OES) 粉末压片 10 4.3 WHCS-FF-CS/02—2019 碱解氮 容量法(VOL) 碱解-扩散 - 1 LY/T 1228—2015 速效磷 电感耦合等离子体发射光谱法(ICP-OES) 中碱性：碳酸氢钠浸取；
酸性：氟化铵-盐酸浸取0.25 0.2 LY/T 1232—2015 速效钾 电感耦合等离子体发射光谱法(ICP-OES) 乙酸铵浸取 1.25 1 LY/T 1234—2015 阳离子交换量
(CEC)容量法(VOL) 乙酸铵浸取 2.5 1** LY/T 1243—1999 注：“*”单位为无量纲；“**”单位为cmol/kg；“-”无检出限值。 
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表 2 表层土壤地球化学参数特征
Table 2. Characteristics of geochemical parameters for surface soil
分析指标 最小值 最大值 平均值 中位数 标准离差 变化系数 Se(mg/kg) 0.14 1.51 0.45 0.44 0.10 0.23 有效硒(μg/kg) 0.79 26.80 9.20 8.80 3.56 0.39 有机质(%) 0.37 10.50 2.53 2.45 1.03 0.41 pH 5.81 8.86 8.22 8.32 0.41 0.05 TFe2O3(%) 3.53 14.00 7.06 6.88 0.99 0.14 N(mg/kg) 489.00 4412.00 1822.81 1792.00 571.10 0.31 P(mg/kg) 289.00 1728.00 839.03 832.00 193.97 0.23 碱解氮(mg/kg) 10.00 472.00 100.99 93.80 49.61 0.49 速效磷(mg/kg) 0.66 94.30 10.96 7.51 10.00 0.91 速效钾(mg/kg) 6.00 794.00 111.15 80.00 89.00 0.80 西藏土壤硒(mg/kg) 0.04 0.37 0.15 0.14 / 0.48 中国表层土壤硒(mg/kg) 0.00 49.60 0.26 0.21 0.22 0.80 注：西藏土壤硒含量数据引自《西藏土壤元素背景值及其分布特征》(成廷鏊等，1993)；中国表层土壤硒含量数据引自《中国土壤地球化学参数》(侯青叶等，2020)。
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表 3 研究区不同地层分布区土壤中硒参数统计
Table 3. Statistics of selenium parameters in soils of different stratigraphic distribution areas in the study area
地层 样品数量 硒含量最小值
(mg/kg)硒含量最大值
(mg/kg)硒含量算术平均值
(mg/kg)硒含量中位数
(mg/kg)标准差
(mg/kg)变异系数 涅如组三段(T3n3) 110 0.22 1.03 0.43 0.42 0.11 0.25 涅如组二段(T3n2) 317 0.22 1.51 0.46 0.44 0.14 0.31 涅如组一段(T3n1) 28 0.24 0.77 0.47 0.45 0.12 0.26 日当组(J1r) 401 0.14 1.35 0.43 0.41 0.11 0.27 陆热组(J1-2l) 8 0.28 0.73 0.50 0.49 0.15 0.31 第四系(Qh) 711 0.14 0.72 0.45 0.45 0.07 0.15 辉绿岩(βμ) 9 0.14 0.46 0.37 0.44 0.11 0.30 花岗斑岩(γπ) 3 0.39 0.49 0.45 0.48 0.06 0.12 比马组(K1b)* 23 0.08 0.22 0.12 0.12 0.03 0.23 宋热岩组(T3s)* 78 0.15 0.71 0.34 0.29 0.13 0.40 典中组(E1d)* 24 0.10 0.44 0.23 0.22 0.09 0.42 注：“*”数据来源于西藏乃东区重点耕地区1:5万土地质量地球化学调查数据。
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表 4 不同土地利用方式土壤硒地球化学参数
Table 4. Geochemical parameters of selenium concentration in soils with different land use types
用地类型 样品数量 硒含量最小值
(mg/kg)硒含量最大值
(mg/kg)硒含量算术平均值
(mg/kg)硒含量中位数
(mg/kg)标准差
(mg/kg)变异系数 水浇地 860 0.26 0.98 0.45 0.44 0.07 0.17 旱地 20 0.38 0.58 0.47 0.46 0.05 0.11 天然牧草地 424 0.14 1.51 0.43 0.41 0.16 0.37 人工牧草地 81 0.26 0.74 0.44 0.43 0.08 0.18 灌木林地 115 0.25 0.65 0.45 0.46 0.07 0.15 其他林地 37 0.33 0.63 0.46 0.45 0.09 0.18 乔木林地 40 0.32 0.55 0.45 0.45 0.05 0.11 沼泽草地 6 0.33 0.7 0.53 0.52 0.14 0.27 内陆滩涂 4 0.33 0.43 0.4 0.42 0.05 0.12
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表 5 土壤有效硒和CEC与氮、磷等指标相关关系
Table 5. Correlation between soil available selenium and CEC and N, P and other indicators
指标 样品数量 氮 磷 有机质 碱解氮 有效磷 速效钾 有效硒 有效硒 1587 0.591** 0.406** 0.528** 0.538** 0.385** 0.500** 1 CEC 130 0.749** 0.649** 0.785** 0.601** 0.383** 0.431** 0.446** 注: “**”表示在置信度(双测)为0.01时，相关性是显著的。
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