Scientia Agricultura Sinica ›› 2019, Vol. 52 ›› Issue (2): 293-311.doi: 10.3864/j.issn.0578-1752.2019.02.009

• SOIL & FERTILIZER·WATER-SAVING IRRIGATION·AGROECOLOGY & ENVIRONMENT • Previous Articles     Next Articles

Environmental Risks for Application of Phosphogysum in Agricultural Soils in China

WANG XiaoBin,YAN Xiang(),LI XiuYing,JI HongJie   

  1. Institute of Agricultural Resources and Regional Planning, Chinese Academy of Agricultural Sciences, Beijing 100081
  • Received:2018-05-24 Accepted:2018-08-22 Online:2019-01-16 Published:2019-01-21
  • Contact: Xiang YAN E-mail:yanxiang@caas.cn

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Abstract:

Phosphogypsum (PG) is an industrial by-product gypsum obtained from wet process production of phosphoric acid, and it is one of the largest solid waste emissions in the chemical industry. With the development of phosphate and compound fertilizer industry at the late 1950s, the PG waste residue discharged from the production process had continuously increased in China. To solve the environmental problems caused by massive PG stockpiling, at present, PG was mainly used as for building materials, such as cement retarder, and gypsum-building materials, as well as for filling mine pits and road construction. Some researches have also tried to use PG instead of natural gypsum for saline-alkali land amendment in agriculture since 1990s. However, several harmful elements in phosphate rock were preserved or enriched in PG in the process of wet process phosphoric acid production, resulting in high concentration of hazardous pollutants, including heavy metals, fluoride (F), and radioactive element radium ( 226Ra) in PG, and to some extent, even far beyond the limits of national standards for soil environmental quality and for groundwater quality. For example, the concentrations of heavy metals Cr, As, Cd and Hg in PG exceed the limits (about 20%-67%) of Soil Environmental Quality Risk Control Standard for Soil Contamination of Agricultural Land (GB 15618-2018); and the leachable concentrations of Hg, Cd, Pb, Ni, Cr and Be in PG exceeded the limits (IV-V) of Standards for Groundwater Quality (GB/T 14848-2017). The concentrations of total F and water-soluble F in PG exceeded the critical values of total and soluble F (about 89% and 100%, respectively) in soils of endemic fluorosis-affected areas in China, and the leachable concentration of F in PG exceeded the limit (V) of Standards for Groundwater Quality, and some exceeded the limit of Identification Standards for Hazardous Wastes Identification for Extraction Toxicity (GB 5085.3-2007). According to the concentration of pollutants in PG, as compared with the limits of Soil Environmental Quality Risk Control Standard (GB 15618-2018), the long-term impacts of PG application (if PG input was at rate of 22.5 t·hm -2·a -1, and with no leaching) on the accumulations of pollutants in the soil could be estimated. For instance, the accumulation of Cd, Hg, F and 226Ra from un-contaminated to contaminated soils would need 1, 5, 4 and 25 years, respectively. Some field experiments have shown that PG could lead to the risk of excessive pollutants (such as F, As, Cd, Hg, Pb and Zn) enriched in some agricultural products. In 2017, the Identification Standards for Solid Wastes General Rules (GB 34330-2017) was issued in China, which stipulated clearly that those by-products produced in the production process, including PG produced in the inorganic chemical production process, were solid wastes; and those directly used for soil amendment, land reconstruction, land restoration and other land use methods by solid waste disposal were still managed as solid wastes. In order to ensure soil health, food safety, and environmental quality, it was suggested that those industrial waste like PG without any harmless treatment of pollutants, and with harmful elements far beyond the limit standard should not be allowed to directly use as for soil remediation or conditioning in the farmlands by solid waste disposal methods, to prevent hazardous pollutants from entering food chain and harming to human health.

Key words: industrial waste, environmental safety risk, soil pollution, phosphogysum, heavy metals

Table 1

Concentration of elements in phosphate ores in China"

pH Hg Cd As Pb Cr Ni Cu Zn F 226Ra 232Th 40K 238U
(mg·kg-1) (Bq·kg-1)
参考文献References [40,47-48] [49] [47,50-51] [49,50] [49,50,51] [49,50,51] [49] [48,51] [48,51] [50,52-61] [62,63,64,65,66,67,68,69] [62,63,64,65] [63,65-66] [62,63,64]
样本数Num. 4 1 15 5 15 15 1 12 12 35 40 17 13 13
最小值Min. 4.68 0.69 0.13 0.58 5.5 7.5 48.8 1.3 0.6 5100 47.0 0.4 12.5 117.6
最大值Max. 9.28 0.69 2.29 20.40 283.0 123.8 48.8 12.5 10.7 37500 1566.0 14.7 231.0 1640.0
平均Ave. 7.39 0.69 0.42 9.46 35.4 25.3 48.8 9.8 8.7 22191 316.9 6.7 139.1 394.3
标准差SD. 2.10 0.53 8.29 71.1 27.6 3.1 2.6 9917 319.0 5.7 66.1 402.9
变异系数CV (%) 28.4 125.6 87.58 201.0 109.3 31.6 30.4 44.7 100.7 85.6 47.5 102.2
土壤环境背景值
Soil background [44,45]		 0.065 0.097 11.2 26.0 61.0 26.9 22.6 74.2 478 44.7 16.5 588.3 32.4
土壤环境风险系数
Environment risk coeff.		 10.62 4.31 0.84 1.36 0.41 1.81 0.43 0.12 46.4 7.1 0.4 0.2 12.2

Table 2

Concentration of radionuclides in phosphogysum and national environmental quality standard-limits"

226Ra 232Th 40K 238U 内照射指数IRa 外照射指数Ir
参考文献References [62,71-77] [62,71-77] [18,72-73,76-78] [62,64] [62,71-77] [62,71-77]
样本数Num. 31 29 27 4 31 30
最小值Min. 82.1 0.33 1.0 40 0.41 0.23
最大值Max. 788.0 137.00 1669.0 147 3.93 2.83
平均Ave. 305.0 21.94 277.2 87.8 1.59 1.05
标准差SD. 210.7 36.65 404.8 46.6 1.12 0.73
变异系数CV (%) 69.1 167.0 146.0 53.1 70.6 69.7
磷矿石中含量Phosphate ores (Table 1) 316.9 6.7 139.1 394.3
富集系数Enrichment coeff. 0.96 3.27 1.99 0.22
土壤环境背景值Soil background [45] 44.7 16.5 588.3 32.4
土壤环境风险系数Enrichment coeff. 6.8 1.3 0.5 2.7
超出标准率Over limits (%) 52 52 43
GB 6566—2010 [70] <200 <1.0 <1.0

Table 3

Concentration of elements in phosphogysum and enrichment coefficients of elements, national environmental quality standard-limits"

pH Hg Cd As Pb Cr Ni Cu Zn F总 F水溶
参考文献
References		 [20,81-84,
106-107]		 [9,71,81,
85-87] 		[9-10,20,
71,78,81,
85-89]		 [9-10,20,
71,78,81,
85-86,89]		 [9,71,78,
81,85-89]		 [9-10, 78,
81,85,87,89]		 [78,81,85,
87-89]		 [9, 71,
81,85-89]		 [9, 71,78,
81,85-89]		 [1, 9-10,16, 22,
34,43,52, 72-73,
78,81-84,88,90-107]		 [9-10,43,
73,83,101,105-108]
样本数Number 37 12 35 30 33 25 23 27 33 126 15
最小值Min. 1.8 0.06 0 0.297 1.3 0 0.28 1.87 0 40 11.84
最大值Max. 6.5 10.78 37 66.5 240.5 1200 335 160 210 20400 7500
平均Ave. 3.41 1.61 1.96 18.3 38.6 106.8 31.9 29.0 67.3 3662 2143
标准差SD. 1.22 2.95 6.18 14.6 42.7 236.4 67.4 29.7 62.4 3657 2530
变异系数CV (%) 35.9 183.6 314.5 80.1 110.5 221.4 211.4 102.6 92.7 99.9 118.1
磷矿石中含量Phosphate ores (Table1) 7.39 0.69 0.42 9.46 35.39 25.27 48.80 9.77 8.66 22191
富集系数Enrichment coeff. 2.33 4.68 1.93 1.09 4.23 0.65 2.97 7.77 0.17
土壤环境背景值Soil background [44] 0.065 0.097 11.2 26 61 26.9 22.6 74.2 478
土壤环境风险系数Environment risk coeff. 24.7 20.2 1.6 1.5 1.8 1.2 1.3 0.9 7.7
超标数Over limits’ Num. 8 22 12 2 5 1 3 1 112 15
超出土壤标准率Over limits (%) 66.7 62.9 40.0 6.1 20.0 4.3 11.1 3.0 88.9 100.0
GB 15618—2018 limits [79] <0.5 <0.3 <20 <70 <150 <60 <50 <200
参考限量Referred limits[80] ≤800 ≤2.5

Table 4

Comparison between leachable contents of the elements in phosphogypsum and national environmental quality standard- limits for hazardous pollutants"

元素
Elements		 浸出浓度 Leachable contents (Over-limit level) (mg·L-1) GB 5085.3—2007[117]
Limited value
(mg·L-1)		 GB 8978—1996[115]
Limited value
(mg·L-1)		 GB/T 14848—2017 [116]
Limited value (mg·L-1)
No. 1 [118] No. 2[103] No. 3[33]
湿法Wet 干法Dry III IV V
pH 4.22*-4.99*
(V)		 2.23*-5.73*
(V-IV)		 2.96*-3.09*
(V)		 3.05*-5.37*
(V)		 ≤2.0 & ≥12.5a） 6-9b） 6.5-8.5 5.5-6.5,8.5-9 <5.5,>9
F 10.1*-98.0*
(V)		 2.75*-45.9*
(V)		 98.6*-224*
(V)		 10.9*-20.2*
(V)		 100 10-20 ≤1.0 ≤2.0 >2.0
Hg 0.000015-0.00159* (I-IV) 0.0002-0.014*
(I-V)		 0.007-0.009*
(V)		 0.000015
(I)		 0.1 0.05 ≤0.001 ≤0.002 >0.002
Cd 0.015*-0.05*
(V)		 0.005-0.023*
(III-V)		 0.018*-0.027*
(V)		 0.016*-0.065*
(V)		 1 0.1 ≤0.005 ≤0.01 >0.01
As 0.0033-0.03
(II-III)		 0.0007-0.117*
(I-V)		 0.0096-0.047 (II-III) 0.009-0.016 (II-III) 5 0.5 ≤0.01 ≤0.05 >0.05
Pb 0.72*-2.00*
(V)		 <0.1*
(IV)		 0.18*-0.26*
(V)		 0.19*-1.07*
(V)		 5 1.0 ≤0.01 ≤0.1 >0.1
Cr 0.04-0.17*
(III-V)		 <0.05
(III)		 0.03-0.06*
(III-IV)		 0.02-0.08*
(III-IV)		 15 1.5 ≤0.05 ≤0.1 >0.1
Ni 0.15*-0.28*
(V)		 0.04*-0.07*
(IV)		 0.19*-0.33*
(V)		 0.16*-0.32*
(V)		 5 1.0 ≤0.02 ≤0.1 >0.1
Cu 0.04-0.11
(II-III)		 0.02-0.06
(II-III)		 0.024-0.15
(II-III)		 0.034-0.13 (II-III) 100 0.5-2.0 ≤1.0 ≤1.5 >1.5
Zn 0.097-0.415
(I-II )		 0.005-0.272
(I-II )		 1.51*-5.10*
(IV-V)		 0.036-0.771*
(I-III)		 100 2.0-5.0 ≤1.0 ≤5.0 >5.0
Ba 0.05-0.064
(II)		 3*-4.7*
(IV-V)		 0.119-0.128
(III)		 0.059-0.136 (II-III) 100 ≤0.70 ≤4.0 >4.0
Be 0.005*-0.009*
(IV)		 <0.005*
(IV)		 0.008*-0.012*
(V)		 0.004*-0.010*
(V)		 0.02 0.005 ≤0.002 ≤0.06 >0.06

Table 5

The effect of phosphogypsum (PG) on contents of pollutants in agricultural products"

试验地点/土壤
Sites /Soils tested		 作物
Crop		 磷石膏用量
PG rates
(kg·hm-2)		 作物中In plant (mg·kg-1)
F As Cd Hg Pb Zn
沈阳康平县盐碱土[10]
Saline soil in Shenyang		 玉米Maize
/水稻Rice		 3750 0.62-1.18
/0.41-1.28
甘肃天水秦安县黄绵土[11]
Dryland in Gansu		 大豆籽粒Soybean seed
/秸秆Stalks		 1500-12000
/0.10-0.14
/0.11-0.24		 1.10-4.86
/1.10-4.86
天津滨海盐碱地[16]
Coastal saline soil in Tianjin		 水稻Rice
/玉米Maize		 1500-5250 4.69-5.28
/3.33-3.90
山东陵县盐碱土[122]
Saline soil in Shandong		 小麦Wheat 15000-60000 2.09-3.54
贵州模拟磷石膏渣场[123,124]
Modified PG matrix in Guizhou		 蔬菜Vegetables 磷石膏改良基质
Modified PG matrix		 79-266 0.66-1.56 46-362
云南玉溪江川县低硫缺磷土壤[20]
Tobacco-planting soil in Yunnan		 烤烟Tobacco 90000 0.87-0.89
GB/T 18406.1—2001[121] ≤1.0 ≤0.5 ≤0.05 ≤0.01 ≤0.2
GB 13106—91[125] ≤20

Table 6

Assumed cumulative loading of elements that could result from phosphogypsum application to soil and estimated over- limit years (hypothetical assumption)"

Hg Cd As F 226Ra
(Bq·kg-1)
(mg·kg-1)
磷石膏中元素浓度Max. content in PG (mg·kg-1)
10.8 37.0 66.5 20400 788
磷石膏年用量Annual rate of PG (t·hm-2) 土壤中元素年累积量Accumulation in soil (kg·hm-2)
4.5 0.049 0.167 0.299 92 3.5
22.5 0.243 0.833 1.496 459 17.7
40.5 0.437 1.499 2.693 826 31.9
58.5 0.631 2.165 3.890 1193 46.1
超标年限Over-limit (years)
4.5 23.1 4.1 150 19.6 127
22.5 4.6 0.8 30 3.9 25
40.5 2.6 0.5 17 2.2 14
58.5 1.8 0.3 12 1.5 10
GB 15618—2018 limits [79]
参考限量Referred limits[80]		 <0.50 <0.30 <20 ≤800
GB 6566—2010 limits [70] (Bq·kg-1) ≤200
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