Supplementary Materials forStatus of chromium accumulation of agricultural soils

across China (1989–2016)Xingyuan Lia, c, Jingru Zhangb, Jin Maa*, Taoran Shi a, Yiwei Gonga, Shuhui Yang a,

Qiyuan Liu a, c, Yaling Qu a

a State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese

Research Academy of Environmental Sciences, Beijing, 100012, China

b Guangdong Province Academic of Environmental Science, Guangzhou, 510045,

China

c School of Geography and Planning, Sun Yat-sen University, Guangzhou, 510275,

China

Number of pages: 12Table numbers: 8Figure numbers: 3

* To whom correspondence may be addressed. Email: majin@craes.org.cn (J. Ma)

List

1. Figure S1. The main areas selected for studies of Cr occurrence in agricultural soils in China.

2. Figure S2. Boxplots of the Cr concentration (mg/kg) of agriculture soils in China from different periods

3. Figure S3. The geographical distribution map of chromite deposits in China. (RESDC, http://www.resdc.cn).

4. Table S1. The background values (mg/kg) of Cr in different regions of China.

5. Table S2 Seven classes comprising the geo-accumulation index.

6. Table S3 Cr concentration (mg/kg) in agriculture soils of China from 1989 to 2016.

7. Table S4 Description of Cr concentrations (mg/kg) of agriculture soils in different periods in China.

8. Table S5 Description of Cr concentrations (mg/kg) of agriculture soils in different regions in China.

9. Table S6. Description of Cr concentrations (mg/kg) and sources of agriculture soils in the heavy polluted agricultural regions.

10. Table S7 The percent of classes of Igeo in national soils for different periods from 1989-2016.

11. Table S8 The estimated total Chromium emissions (ten thousand tons) in China, 1989-2016.

Figure S1. The main areas selected for studies of Cr occurrence in agricultural soils in China.

Figure S2. Boxplots of the Cr concentration (mg/kg) of agriculture soils in China from different periods (The dark blue and black lines represent the arithmetic and median means of Cr concentration respectively). Green line: soil environmental quality risk filter value (150 mg/kg) for contamination of agricultural land (GB15618-2018); Red line: soil environmental quality risk control value (800 mg/kg) for contamination of agricultural land (GB15618-2018); Purple line: background value (51.9 mg/kg) of agricultural soil in China; Distinct lowercase letter indicate differences among time periods (P < 0.05).

Figure S3. The geographical distribution map of chromite deposits in China. (RESDC,

http://www.resdc.cn)

Table S1. The background values (mg/kg) of Cr in different regions of China and elsewhere in the world

Region Province Cr

northeastLiaoning 61.2

Jilin 46.9Heilongjiang 59.5

north China

Beijing 66.1Tianjin 85.3Hebei 72.6Shanxi 61.5

Shandong 70

east China

Henan 65.6Shanghai 63.4Jiangsu 76.2

Zhejiang 54.5Fujian 42.9Anhui 67.5

south China

Guangdong 58.9Hainan 58.9Hunan 68.6

central China

Henan 65.6Hubei 85.7Jiangxi 45.8

southwest

Guizhou 133.3Yunnan 78

Chongqing 50.5Sichuan 50.5Guangxi 86.3

northwest

Gansu 66.4Qinghai 63Ningxia 56.3Xinjiang 50.2

Tibet 79.3Inner

Mongolia38

Shaanxi 57.9World soils 40

England 68Europe 64

Australia 48Malaysia 25.9

Thailand 25.2

Geoaccumulation index (Igeo)

Pollution level of heavy metals in soils was evaluated using the geoaccumulation

index (Igeo). The geoaccumulation index (Igeo) was calculated according to the equation

of Müller (1969).

(1)

where Cn represents the measured concentration of the element, n and Bn is the soil

background content of element n from different provinces in China. (Table S1;

CNEMC, 1990). Factor 1.5 is the background matrix correction factor due to

lithologic. The Igeo consists of seven grades or classes (Muller, 1981): Class 0

(uncontaminated) Igeo ≤0; Class 1 (from uncontaminated to moderately contaminated)

0< Igeo <1; Class 2 (moderately contaminated) 0< Igeo <2; Class 3 (from moderately to

strongly contaminated) 2< Igeo <3; Class 4 (strongly contaminated) 3< Igeo <4; Class 5

(from strongly to extremely contaminated) 4< Igeo <5; Class 6 (extremely

contaminated) 5< Igeo. Class 6 is an open class and comprises all values of the index

higher than Class 5. The elemental concentrations in Class 6 may be hundred-fold

greater than the geochemical background value (Table S2).

Table S2. Seven classes comprising the geo-accumulation index.Class Value Soil quality

0 Igeo ≤ 0 Practically uncontaminated1 0< Igeo ≤ 1 Uncontaminated to moderately contaminated2 1< Igeo ≤2 Moderately contaminated3 2< Igeo ≤3 Moderately to heavily contaminated4 3< Igeo ≤ 4 Heavily contaminated5 4< Igeo ≤ 5 Heavily to extremely contaminated6 5<Igeo Extremely contaminated

Table S3 Cr concentration (mg/kg) in agriculture soils of China from 1989 to 2016.

Sampling time

N Median

Arithmetic mean

Min Max

1989 1 47.20 47.2 47.20 47.20 1992 1 50.80 50.8 50.80 50.80 1993 3 68.06 59.05 38.10 71.00 1994 15 59.74 58.48 39.00 78.00 1995 3 58.00 60.9 38.50 86.20 1996 2 57.37 57.37 24.84 89.90 1997 6 37.94 45.63 32.28 93.90 1999 6 63.00 53.1 12.06 84.00 2000 5 58.33 61.09 47.92 96.20 2001 31 63.88 69.87 17.38 150.46 2002 14 48.97 66.32 10.43 194.00 2003 67 53.77 60.29 5.40 820.24 2004 60 61.71 66.06 24.96 149.57 2005 96 61.53 65.15 10.92 121.17 2006 106 68.80 81.23 4.08 596.70 2007 158 67.16 74.36 1.67 179.50 2008 127 67.20 82.13 13.00 594.10 2009 114 58.87 63.12 5.50 254.25 2010 149 68.89 76.32 4.30 652.18 2011 99 57.83 64.54 18.30 217.74 2012 147 64.71 74.29 1.48 416.85 2013 152 62.68 71.74 2.42 816.00 2014 115 61.45 64.35 3.20 275.58 2015 113 60.69 75.63 9.70 664.80 2016 35 69.46 65.98 29.10 123.70

Table S4 Description of Cr concentrations (mg/kg) of agriculture soils in different periods in China.

Sampling time 1989~2000 2001~2005 2006~2010 2011~2016

N1 42 268 654 661 Arithmetic mean 56.52 67.81 75.36 70.11

Median 58.51 59.89 65.92 62.45Min 12.06 5.40 1.67 1.48 Max 96.2 820.24 652.18 816

1. N: Number of data2. Soil environmental quality Risk control standard for soil contamination of agricultural land (GB15618-2018).

Table S5 Description of Cr concentrations (mg/kg) of agriculture soils in different regions in China.

Table S6. Description of Cr concentrations (mg/kg) and sources of agriculture soils in the heavy polluted agricultural regions.

Region Location Longitude LatitudeCr

(mg/kg)Emission sources

Anhui

Huainan City 116.99 32.62 174.86 Mining activities

Huainan City 116.83 32.62 211.96 Mining activities

Suzhou City 116.96 33.64 416.85 Mining activities

Suzhou City 116.97 33.61 416.85 Mining activities

BeijingDetiangou Au mining area 116.63 40.6 217.74 Mining activities

Detiangou Au mining area 116.63 40.6 187.7 Mining activities

Fujian

Fuzhou City 119.29 26.07 150.46 Industrial activities

Fuzhou City 119.31 26.04 254.25 Industrial activities

Fuzhou City 119.32 26.04 254.25 Industrial activities

Wuyishan City 118.15 27.68 154.42 N

Wuyishan City 118.03 27.75 250.9 N

Wuyishan City 118.06 27.68 275.58 N

Gansu Lanzhou City 103.9 36.06 278.14 Sewage irrigation

Guangdon

gMeizhou City 116.29 24.52 178.8

Mining activities

Guangxi

Yaoan City 108.1 23.93 176 N

Liuzhou City 109.42 24.32 178 Mining activities

Liuzhou City 109.42 24.32 152 Mining activities

Guizhou Guiyang 106.75 26.63 175.8 N

Sampling time

North East

North West

North China

East China

Central China

South China

South West

N1 133 260 251 379 146 151 305 Arithmetic

mean 65.86 75.65 64.02 72.94 65.58 67.63 81.43 Median 53.62 69.28 60.75 64.25 57.99 64.61 68.59

Min 1.48 2.42 4.077 3.2 9.7 5.5 1.67Max 652.18 313.6 217.84 820.24 91 254.25 816

1.N: Number of data2.Soil environmental quality Risk control standard for soil contamination of agricultural land

(GB15618-2018)

Guiyang 106.63 26.65 150.46 N

Hezhang City 104.88 26.73 150 N

Zunyi City 106.9 27.51 179.5 N

Zunyi City 106.86 27.59 162.7 N

Zunyi City 107.47 27.77 190.4 N

Zunyi City 107.26 27.59 166.8 Mining activities

Henan

Jiaozuo City 113.24 35.21 376.672 Mining activities

kaifeng City 114.51 34.77 150.2 Mining activities

pingdingshan City 113.27 33.72 594.1 Mining activities

Xingxiang City 113.87 35.34 152.2 Sewage irrigation

Hunan Zhuzhou City 113.13 27.83 178 Industrial activities

JiangsuXuzhou City 117.28 34.2 820.24 Mining activities

Wuxi City 120.31 31.49 664.8 Industrial activities

Liaoning

Huludao City 120.83 40.71 154.85 Mining activities

Huludao City 120.83 40.71 154.85 Mining activities

Huludao City 120.83 40.71 166.43 Mining activities

Huludao City 120.83 40.71 201.98 Mining activities

Huludao City 120.83 40.71 154.85 Mining activities

Huludao City 120.83 40.71 528.14 Mining activities

Huludao City 120.83 40.71 192.22 Mining activities

Jingzhou City 121.12 41.09 652.18 Industrial activities

Inner

MongoliaWulate City 108.65 40.73 163.3

N

Qinghai

Xining City 101.76 36.65 313.6 N

Xining City 101.8 36.59 172.3 N

Xining City 101.76 36.62 158.6 N

Xining City 101.78 36.62 158.4 N

ShandongFeicheng City 116.76 36.18 171 Fertilizers and Fungicides

Taian City 117.08 36.2 159.07 Fertilizers and Fungicides

Shannxi

Luocuan City 109.43 35.76 250 Fertilizers and Fungicides

Luocuan City 109.5 34.49 237.17 Fertilizers and Fungicides

Luocuan City 107.15 34.65 250 Fertilizers and Fungicides

Luocuan City 107.15 34.65 200 Fertilizers and Fungicides

Luocuan City 107.15 34.65 150 Fertilizers and Fungicides

Xian City 108.93 34.34 163 Fertilizers and Fungicides

Yangning City 108.08 34.27 193 Fertilizers and Fungicides

Shanghai

Shanghai 121.47 31.23 668.36 N

Shanghai 121.54 31.22 159 Sewage irrigation

Shanghai 121.47 31.23 596.7 N

Sichuan

Deyang City 104.39 31.13 157.4 N

panzhihua City 102.26 27.89 184 Mining activities

Pengshan City 103.442 30.15 240.5 Mining activities

Dayi mining area 103.5 30.57 153.42 Mining activities

Yunnan

Jianshui City 102.82 23.63 169.3933 Fertilizers and Fungicides

Yilong lake 102.54 23.65 256.24 N

Yilong lake 102.56 23.67 152.28 N

Yunjiang City 102 23.59 166.16 Mining activities

Chongqin

g

Dazu city 105.75 29.57 816 Industrial activities

Chongqing 105.66 29.46 332.41 Industrial activities

Beipei area 106.39 29.8 217.99 Industrial activities

Jianping area 106.45 29.56 300 Industrial activities

Wanzhou area 108.4 30.8 175.6 Industrial activities

Note: “N” represents the source of heavy metals is not clear.

Table S7. The percent of classes of Igeo in national soils for different periods from 1989-2016.

Period 1989-2000 2001-2005 2006-2010 2011-2016Class Percent (%)

0 Igeo ≤ 0 95.24 82.53 84.10 82.30 1 0 < Igeo ≤ 1 4.76 15.24 13.15 14.83 2 1 < Igeo ≤ 2 0.00 1.49 2.14 1.97 3 2 < Igeo ≤ 3 0.00 0.74 0.61 0.91 4 3 < Igeo ≤ 4 0.00 0.00 0.00 0.005 4 < Igeo ≤ 5 0.00 0.00 0.00 0.00

Table S8. The estimated Total Chromium emissions (ten thousand tons) in China, 1989-2016

Source

Year

Chromium salt Leatherwear Atmospheric

deposition Electroplating

1989 0.875 0.169 - -1990 0.875 - 0.337 0.180 1991 0.875 - - -1992 0.875 - - -1993 0.875 - - -1994 1.164 - - -1995 1.484 - 0.516 1996 1.628 - - 0.233 1997 1.717 - - -1998 1.913 0.367 - -1999 2.254 0.000 - 0.245 2000 2.625 0.527 0.497 -2001 3.483 - - -2002 3.567 0.553 - -2003 3.971 0.553 - 0.439 2004 3.698 0.564 - 0.514 2005 4.526 0.603 0.683 0.691 2006 4.954 0.678 0.718 0.961 2007 4.970 0.651 0.745 1.314 2008 4.002 0.709 0.776 1.468 2009 4.807 0.657 0.781 1.401 2010 6.300 0.828 0.747 1.779 2011 6.773 0.677 0.773 1.889 2012 5.950 0.783 0.783 2.029 2013 6.300 0.608 0.800 2.632 2014 5.653 0.656 0.796 2.228 2015 4.596 0.663 0.798 2.107 2016 4.600 0.812 0.795 2.224

Note: (1) Atmospheric deposition data come from Tian et al (2016) and China Statistical Yearbook on Environment 2000-2016; (2) Electroplating data came from the China Industrial Information Network (http://www.chyxx.com), Sun et al (1993) and Wang (2012); (3) Leatherwear data came from China Statistical Yearbook on Environment 2000-2016 and the China Industrial Information Network (http://www.chyxx.com); (4) Chromium salt data came from Xie et al (2014), Li (2018) and China Statistical Year book on Environment 2000-2016 ; (5) “–”represent the Total Chromium data is a lack in the year.

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