Geochemical Characteristics of Selenium in Surface Soil of Central Townships in Zhaojue County, Sichuan Province
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摘要:
硒元素是人体必需的微量元素之一，食用富硒农产品是人体获取和补充硒元素的主要途径，调查区域硒地球化学特征是有效地利用富硒土地资源以及开发富硒农副产品的重要依据。本文选择四川省昭觉县域内较为重要的农耕乡镇采集表层土壤样品，采用原子荧光光谱法、X射线荧光光谱法、电感耦合等离子体质谱/发射光谱法等方法测定1328件土壤、19件玉米及20件土豆中硒等地球化学指标含量，利用相关分析与统计学等方法，结合距离加权反比插值法，探讨研究区硒含量、分布和影响因素等地球化学特征，评价土壤与作物的富硒情况及安全性。结果表明：①研究区表层土壤硒含量范围为0.04~1.50mg/kg，平均值为0.33mg/kg，划定富硒土壤面积为7.23km2，占全区土壤面积的30.31%，玄武岩发育的土壤硒含量最高，平均值为0.4mg/kg，表明区内地质背景与土壤硒含量密切相关，区内富硒土壤主要受含玄武岩夹苦橄岩、凝灰质砂泥岩的峨眉山玄武岩组地层控制；②不同的用地类型和土壤类型对硒元素的富集能力不同，人为农业活动导致土壤对硒的吸附能力下降，黄棕壤土层中黏粒或铁氧化物等易与硒结合富集；酸性土壤中硒含量与pH值成反比；土壤有机质与硒含量呈显著的正相关；土壤质地对硒含量具有一定的控制作用；③富硒土壤产出的玉米和土豆富硒率极低。研究结果认为昭觉县在开发利用富硒土壤时，旱地与水田等农耕区应及时补充有机肥并调节土壤酸碱度，并积极利用富硒资源开发其他农业产品。
Abstract:BACKGROUND Selenium (Se) is one of the essential trace elements for humans, and an important way for humans to obtain and supplement selenium is by eating natural selenium-enriched agricultural products. The geochemical characteristics of selenium in the survey area are an important basis for the effective utilization of selenium-enriched land resources and the development of selenium-enriched agricultural and sideline products.
OBJECTIVES To investigate the geochemical characteristics of selenium content, distribution and influence factors in the study area.
METHODS Soil and crop samples were collected from a central village of Zhaojue County, Sichuan Province. AFS, XRF and ICP-MS were used to determine the contents of elements including Se, Al2O3, TFe2O3, SiO2, OrgC, and pH values. Geochemical characteristics of selenium content, distribution and influencing factors in the study area were investigated using statistical and correlation analysis.
RESULTS (1) The soil selenium content in the study area ranged from 0.04 to 1.50mg/kg, with an average value of 0.33mg/kg. The delineated selenium-enriched soil area was 7.23km2, accounting for 30.31% of the total soil area. The selenium content of the soil developed in basalt was the highest, with an average of 0.4mg/kg, indicating that the geological background in the area was closely related to the soil selenium content. The Se-enriched soil in the area was mainly controlled by the Emeishan basalt Formation, which contained basalt intercalating with picrite and tuffaceous sand and mudstone. (2) The enrichment capacity of selenium varied in different land utilization and soil types. The absorption capacity of selenium in soil decreased due to human agricultural activities. Clayey particles or iron oxides in the yellow-brown loam layer were easy to combine and enrich selenium. The selenium content in acidic soil was inversely correlated to pH value. There was a significant positive correlation between soil organic matter and selenium content. Soil texture had a certain effect on selenium content. (3) Corn and potatoes from selenium-enriched soils had very low selenium content.
CONCLUSIONS During the exploitation and utilization of selenium-enriched soil, organic fertilizer should be added in time and soil pH should be adjusted in agricultural areas such as dry land and paddy field, and other agricultural products should be developed by using selenium-enriched resources.
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表 1 土壤样品分析方法、检出限及数据合格率
Table 1. Analysis method, detection limit and qualified rate of data for soil samples
分析指标 分析方法 检出限 单位 重复样合格率(%) 分析指标 分析方法 检出限 单位 重复样合格率(%) As HG-AFS 1 mg/kg 98.5 Zn ICP-MS 2 mg/kg 99.5 Cd ICP-MS 30 μg/kg 99.5 Al2O3 XRF 0.05 % 100 Cr XRF 5 mg/kg 98.5 TFe2O3 XRF 0.05 % 100 Cu ICP-MS 1 mg/kg 100 SiO2 XRF 0.1 % 100 Hg CV-AFS 0.5 μg/kg 99.5 Se AFS 0.01 mg/kg 99.5 Ni ICP-MS 2 mg/kg 99.5 Corg POT 0.1 % 99.3 Pb ICP-MS 2 mg/kg 100 pH POT 0.1 mg/kg 100 注：HG-AFS为氢化物发生原子荧光光谱法；ICP-MS为电感耦合等离子体质谱法；XRF为X射线荧光光谱法；CV-AFS为冷蒸汽原子荧光光谱法；POT为电位法。 
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表 2 作物样品分析方法、检出限及数据合格率
Table 2. Analysis method, detection limit and qualified rate of crop samples
分析指标 分析方法 检出限 数据合格率(%) CRMs 实验室重复样 As HG-AFS 0.01mg/kg 100 100 Cd ICP-MS 10μg/kg 100 100 Cr ICP-MS 0.2mg/kg 100 100 Cu ICP-MS 1mg/kg 100 100 Hg HG-AFS 0.5μg/kg 100 100 Ni ICP-MS 0.2mg/kg 100 100 Pb ICP-MS 0mg/kg 100 100 Zn ICP-MS 2mg/kg 100 100 Se ICP-MS 0.01mg/kg 100 100 注：HG-AFS为氢化物发生原子荧光光谱法；ICP-MS为电感耦合等离子体质谱法; CRMs为国家标准物质。
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表 3 表层土壤元素地球化学特征值
Table 3. Geochemical characteristics of elements in topsoil
指标 平均值 中位数 最大值 最小值 标准差 变异系数 四川表层土壤平均值 中国表层土壤平均值 K1 K2 Se(mg/kg) 0.33 0.32 1.50 0.04 0.15 0.45 0.25 0.20 1.34 1.67 Al2O3(%) 16.40 16.72 25.09 5.30 2.02 0.12 14.04 12.6 1.17 1.30 TFe2O3(%) 8.84 7.74 17.10 2.85 3.08 0.35 5.59 4.70 1.58 1.88 SiO2(%) 54.30 55.94 81.36 21.39 9.75 0.18 61.59 65.0 0.88 0.84 pH 5.53 5.35 8.11 4.34 0.57 0.10 / / / / 有机质(%) 2.34 1.95 12.80 0.36 1.35 0.57 1.46 0.35 1.60 6.69 As(mg/kg) 10.03 8.86 39.11 1.14 6.80 0.68 9.50 10.0 1.06 1.00 Cd(mg/kg) 0.26 0.23 2.84 0.04 0.16 0.63 0.34 0.09 0.76 2.88 Cr(mg/kg) 92.1 84.5 395 25.8 38.1 0.41 82.0 65.0 1.12 1.42 Cu(mg/kg) 96.9 53.3 1067 14.9 88.3 0.91 32.0 24.0 3.03 4.04 Hg(mg/kg) 0.09 0.09 0.25 0.02 0.04 0.45 0.10 0.04 0.99 2.37 Ni(mg/kg) 43.5 42.1 112 17.0 12.8 0.30 36.0 26.0 1.21 1.67 Pb(mg/kg) 30.9 31.2 88.5 9.33 8.43 0.27 38.0 23.0 0.81 1.34 Zn(mg/kg) 108 95.9 255 38.4 35.9 0.33 90.0 68.0 1.20 1.59 注：四川表层土壤平均值引自《中国土壤地球化学参数》(侯青叶、杨忠芳等，2020)；中国表层土壤平均值引自《中国土壤元素背景值》(魏复盛，1990)。K1为本区表层土壤平均值/四川表层土壤平均值; K2为本区表层土壤平均值/中国表层土壤平均值；“/”表示无此数据。
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表 4 不同用地类型和土壤类型表层土壤中硒含量特征
Table 4. Characteristics of selenium content in topsoil from different land utilization types and soil types
用地类型 样品数量(件) Se含量平均值(mg/kg) Se含量中位数(mg/kg) Se含量范围(mg/kg) 标准差(mg/kg) 变异系数 研究区Se含量背景值(mg/kg) 旱地 632 0.29 0.27 0.06~1.05 0.13 0.45 0.33 水田 13 0.24 0.21 0.09~0.32 0.06 0.27 草地 554 0.39 0.37 0.05~1.10 0.14 0.37 林地 129 0.34 0.30 0.03~1.50 0.19 0.58 土壤类型 样品数量(件) Se含量平均值(mg/kg) Se含量中位数(mg/kg) Se含量范围(mg/kg) 标准差(mg/kg) 变异系数 研究区Se含量背景值(mg/kg) 黄壤 648 0.34 0.33 0.10~1.10 0.12 0.36 0.33 红壤 63 0.23 0.16 0.04~1.50 0.21 0.94 黄棕壤 545 0.36 0.35 0.06~0.94 0.16 0.46 紫色土 50 0.17 0.16 0.05~0.36 0.08 0.46 其他 22 0.22 0.21 0.09~0.32 0.06 0.28
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表 5 不同统计单元表层土壤硒与有机质相关关系
Table 5. Correlation between topsoil selenium and organic matter in different statistical units
统计单元 样品数量(件) 相关系数 统计单元 样品数量(件) 相关系数 Pe 518 0.508** 草地 554 0.587** T1f-j 119 0.492** 林地 129 0.489** T1-2f-l 173 0.751** 黄壤 648 0.545** T2l 235 0.569** 红壤 63 0.510** T3xj 264 0.641** 黄棕壤 545 0.721** 旱地 632 0.691** 紫色土 50 0.913** 水田 13 0.451 汇总 1328 0.615** 注：“**”表示在0.01水平(双侧)上显著相关。
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表 6 研究区表层土壤环境地球化学等级划分
Table 6. Environmental geochemical grade in topsoil of the study area
重金属元素 无风险 风险可控 面积(km2) 比例(%) 面积(km2) 比例(%) As 221.22 99.74 0.58 0.26 Cd 178.00 80.25 43.80 19.75 Cr 219.82 99.11 1.98 0.89 Cu 157.04 70.80 64.77 29.20 Hg 221.81 100.00 0 0.00 Ni 214.20 96.57 7.60 3.43 Pb 221.81 100.00 0 0.00 Zn 221.81 100.00 0 0.00
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表 7 研究区不同作物重金属元素含量
Table 7. Heavy metal element contents in different crops of the study area
作物种类 含量特征 As Cd Cr Cu Hg Ni Pb Zn 玉米 最小值(mg/kg) 0.008 0.001 0.070 1.23 0.001 0.02 0.005 13.38 最大值(mg/kg) 0.030 0.015 0.108 4.89 0.003 0.27 0.086 31.53 平均值(mg/kg) 0.017 0.004 0.079 2.17 0.001 0.07 0.028 19.17 中位数(mg/kg) 0.017 0.003 0.078 1.96 0.001 0.05 0.017 18.15 标准差(mg/kg) 0.005 0.004 0.009 0.81 0.001 0.06 0.025 4.12 变异系数 0.30 0.82 0.11 0.37 0.57 0.86 0.90 0.22 限量值(mg/kg) 0.5 0.1 1.0 / 0.02 / 0.2 / 土豆 最小值(mg/kg) 0.007 0.005 0.005 0.35 0.00002 0.01 0.002 1.56 最大值(mg/kg) 0.013 0.067 0.011 1.65 0.00009 0.21 0.027 3.60 平均值(mg/kg) 0.009 0.016 0.007 0.79 0.00003 0.05 0.005 2.23 中位数(mg/kg) 0.009 0.013 0.007 0.73 0.00003 0.03 0.004 2.10 标准差(mg/kg) 0.001 0.014 0.002 0.31 0.00002 0.05 0.006 0.50 变异系数 0.13 0.84 0.21 0.39 0.49 1.00 1.05 0.22 限量值(mg/kg) 0.5 0.1 0.5 / 0.01 / 0.2 /
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