Comparison of the Forms of Heavy Metals and the Absorption and Transport by Rice between Industrial and Agricultural Contaminated Paddy Soils
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摘要:目的 稻田土壤重金属污染是当前农产品安全生产关注的重要问题。本文比较分析工业和农业污染源稻田土壤重金属的赋存形态及水稻吸收运移，以期为稻田土壤重金属污染控制提供参考。方法 在长江中下游地区调查选取工业源和农业源重金属污染稻田各27块，在水稻成熟期使用抖根法采集根际土壤及水稻根系和籽粒样品，采用Tessier七步提取法分析土壤中重金属赋存形态，及土壤－水稻系统重金属迁移富集。结果 所分析的Cd、Pb、Cu和Zn土壤全量，工业源稻田均显著高于农业源稻田30%以上，特别是土壤Cd全量达到农用地土壤污染风险管控值的280%以上。土壤中重金属均以残渣态为主（占总量46.84% ~ 64.99%）。Zn、Cd和Cu的交换态占比，工业源土壤高于农业源；相反，腐殖酸结合态占比农业源土壤高于工业源；工业源土壤中Cd、Zn表现出较高的土壤-作物迁移性。工业源水稻籽粒Cd、Cu、Pb含量分别高出农业源76%、172%和298%。冗余分析表明，重金属土壤有效态含量是影响水稻根系重金属累积的主要因子，同时，工业源中水稻根系重金属的累积对土壤pH值响应较强烈，而农业源对土壤有机质的响应更加强烈。结论 土壤重金属的赋存形态及水稻的吸收因污染途径的不同存在一定的差异，工业污染稻田中土壤重金属有效性较高，植物迁移与食物污染风险较大。Abstract:objective Heavy metal pollution of paddy soil is an important issue for the quality and safety of agricultural products. The differences in the forms of heavy metals and their absorption and transport by rice in industrial and agricultural contaminated sources were investigated in order to provide a reference for heavy metal contamination control in paddy soils.Method In the middle and lower reaches of the Yangtze River, 27 rice fields contaminated by heavy metals from industrial sources and agricultural sources were selected. The root shaking method was used to collect rhizosphere soil, rice roots and rice seeds during the rice maturity period.Result The contents of Cd, Pb, Cu and Zn in the soil contaminated by industrial source were more than 30% higher than by the agricultural source rice field. Meanwhile, the total content of soil Cd was more than 280% of soil pollution risk control value of agricultural land. The residual form was the main form of heavy metal, accounting for 46.84% to 64.99%. The exchangeable form of Zn, Cd and Cu from industrial source were higher than those from agricultural source. The proportion of humic acid binding heavy metals in the agricultural soil was higher than that in the industrial soil. Cd and Zn in the industrial source soils showed a high soil-crop mobility. The contents of Cd, Cu, Pb in rice seeds from industrial source was 76%, 172% and 298% higher than those from agricultural source. RDA showed that the main factor for the accumulation of heavy metals in rice roots was its bioavailable form in soil. The accumulation of heavy metals in rice roots from industrial source responded more strongly to pH, while that from agricultural source responded more strongly to soil organic matter.Conclusion Therefore, the forms of heavy metals in soil and the absorption of heavy metals by rice were different due to different pollution routes. In rice fields contaminated by industry, the availability of heavy metals and the risks of plant migration and food contamination were higher.
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Keywords:
- Pollution source /
- Paddy soil /
- Heavy metal form /
- Bioavailability /
- Redundant analysis
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图 1 两种典型污染源水稻土采样点分布图
Figure 1. Sampling sites of paddy soil from two typical contamination sources
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图 2 两种污染源稻田土壤中不同形态Cd、Pb、Cu、Zn含量占比
Figure 2. Proportions of different forms of heavy metals in paddy soil from two pollution sources
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图 3 水稻根系重金属含量与土壤重金属形态及理化性质的冗余分析
Figure 3. Redundancy analysis for heavy metal contents in rice root，and soil heavy metal forms and soil physical and chemical properties
表 1 改进的Tessier顺序提取法[19]
Table 1 Improved Tessier sequential extraction method
形态
Form编号
Number提取剂
Extractant操作步骤
Step水溶态 F1 25 ml超纯水 200次/分振荡2 h 离子交换态 F2 25 ml 1.0 M的MgCl2（pH = 7.0） 200次/分振荡2 h 碳酸盐结合态 F3 25 ml 1.0 M的CH3COONa（pH = 5.0） 200次/分振荡5 h 腐殖酸结合态 F4 50 ml 0.1 M的Na4PO7（pH = 10.0） 200次/分振荡3 h，加HNO3消煮 铁锰结合态 F5 50 ml 0.25 M的HONH3CL-HCl混合液 200次/分振荡6 h 强有机结合态 F6 3 ml HNO3，8 ml H2O2，2.5 ml 3.2 M的CH3COONH4-HNO3混合溶液 83 ℃ ± 3 ℃恒温水浴2.5 h，静置10 h离心，取上清液加HNO3和HCLO4消煮 残渣态 F7 5 ml混酸（HCL+HNO3 = 4+1） 消煮 
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表 2 土壤基本理化性质
Table 2 Physical and chemical properties of tested soils
性质
Property含量范围
Content range平均值
Mean中位数
Median标准差
Standard deviation工业源
Industrial
source农业源
Agricultural
source工业源
Industrial
source农业源
Agricultural
source工业源
Industrial
source农业源
Agricultural
source工业源
Industrial
source农业源
Agricultural
sourceSOM（g kg−1） 22.50 ~ 32.84 22.52 ~ 54.53 26.88 36.37 26.71 33.61 2.98 9.69 全氮（g kg−1） 1.09 ~ 1.63 1.47 ~ 1.76 1.35 1.60 1.35 1.59 0.21 0.11 速效磷（mg kg−1） 124.79 ~ 150.39 131.79 ~ 165.36 137.24 148.98 135.36 144.79 7.79 11.99 速效钾（mg kg−1） 81.26 ~ 98.77 86.54 ~ 101.31 90.37 93.80 91.57 94.17 6.45 6.12 pH 5.44 ~ 6.04 5.70 ~ 7.30 5.85 6.35 5.97 6.40 0.20 0.49 CEC（cmol kg−1） 5.74 ~ 10.89 5.26 ~ 9.69 7.57 7.41 7.20 7.20 1.29 1.12 砂粒（%） 25.0 ~ 43.0 21.0 ~ 41.0 32.0 30.0 30.0 31.0 7.0 6.6 粉粒（%） 51.0 ~ 66.0 52.0 ~ 66.0 59.8 59.3 61.0 59.5 5.5 4.2 黏粒（%） 6.0 ~ 13.0 3.0 ~ 21.0 8.2 10.7 7.0 7.5 2.8 6.8
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表 3 工业和农业源污染稻田土壤重金属全量
Table 3 Heavy metal contents in paddy soils contaminated by industrial and agricultural sources
污染源
Contamination source均值 ± 标准差（mg kg−1）
Mean ± SD最小值（mg kg−1）
Min最大值（mg kg−1）
MaxPB* PS** Cd 工业源 1.0811 ± 0.3626 a 0.6683 2.0256 11.91 ± 2.91 2.80 ± 1.22 农业源 0.6092 ± 0.2382 b 0.1234 1.0690 5.09 ± 2.30 1.33 ± 0.53 Pb 工业源 90.80 ± 37.41 a 42.30 166.91 3.36 ± 1.46 0.94 ± 0.43 农业源 50.17 ± 16.10 b 22.60 72.46 1.82 ± 0.60 0.45 ± 0.17 Cu 工业源 40.52 ± 14.01 a 24.43 75.15 2.00 ± 0.67 0.81 ± 0.28 农业源 29.92 ± 7.63 b 22.38 52.11 1.37 ± 0.40 0.50 ± 0.19 Zn 工业源 119.15 ± 21.89 a 65.07 169.86 1.77 ± 0.32 0.60 ± 0.10 农业源 91.68 ± 33.51 b 58.35 192.6 1.46 ± 0.52 0.44 ± 0.19 注：PB*为以土壤背景值为参考的污染指数；PS**为以农用地土壤污染风险管控标准为参考的污染指数
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表 4 水稻根系和籽粒中重金属含量
Table 4 Heavy metal contents in rice roots and seeds
污染源
Pollution source根（mg kg−1）
Root籽粒（mg kg−1）
SeedPi范围
Range of soil pollution indexCd 工业源 1.4833 ± 0.3084 a 0.1819 ± 0.0484 a 0.53 ~ 1.25 农业源 0.5056 ± 0.1263 b 0.1031 ± 0.0218 b 0.29 ~ 0.69 Pb 工业源 26.19 ± 5.22 a 0.4566 ± 0.1121 a 1.32 ~ 3.34 农业源 10.10 ± 5.41 b 0.1148 ± 0.0361 b 0.28 ~ 0.89 Cu 工业源 15.23 ± 2.59 a 0.6330 ± 0.1723 a 0.037 ~ 0.100 农业源 6.239 ± 1.13 b 0.2323 ± 0.0848 b 0.012 ~ 0.041 Zn 工业源 13.800 ± 3.693 a 1.8457 ± 0.4915 a 0.026 ~ 0.059 农业源 10.593 ± 3.358 a 1.6882 ± 0.5347 a 0.020 ~ 0.059 注：P为水稻籽粒中的重金属含量与国家食品卫生标准值之比
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