Chemosphere xxx (xxxx) xxx

Contents lists available at ScienceDirect

Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

Leaching characteristic of potentially toxic metals of artificial soil

made from municipal sludge compost
Feili Li*, Luze Shao, Yihao Chen, Gaoxiang Zhang, Qingting Nie, Zanfang Jin**
College of Environment, Zhejiang University of Technology, Hangzhou, 310032, China

h i g h l i g h t s g r a p h i c a l a b s t r a c t

The leaching behavior of heavy

metals (HMs) in sludge compost col-
umn was studied.

Cu, Pb, Zn, Cd, Ni were decreased by
13%, 8.4%, 12%, 5.9%, and 11%,
respectively.

Treating EDTA increased metal con-
centrations in leachates and delayed
peak times.

The migration of HMs was related to
N and P in the column rather than
EDTA treating.

a r t i c l e i n f o a b s t r a c t

Article history: Landscaping of municipal sludge is a good choice to solve the sludge disposal problem, and EDTA
Received 19 August 2020 treatment can effectively promote the uptake of heavy metals (HMs) by plants, but the heavy metal
Received in revised form leaching process and its main control factors are still poorly understood during the sludge landscaping
8 October 2020
disposal. In this study, the migration behavior of HMs in artificial soil made from municipal sludge
Accepted 11 October 2020
Available online xxx
compost (MSC) were investigated using soil column experiments. After six leaching events for a total of
one year’s rainfall, the average reduction percentage of total phosphorus, total nitrogen, organic matter in
Handling Editor: Willie Peijnenburg the MSC artificial soil were 13.4%, 10.1%, and 7.8%, respectively, while those of copper, lead, zinc, cad-
mium, nickel were 12.9%, 8.37%, 11.5%, 5.94%, and 10.7%, respectively. Treating ethylenediaminetetra-
Keywords: acetic acid (EDTA) to the MSC artificial soil further enhanced the leach index of HMs to different degrees.
Heavy metal HM concentration in leachate were increased with peak times postponed. Though EDTA treatment
Soil column experiment increased HM concentrations in subsoil, it did not change their water washing efficiency. The retention of
Leaching index HMs in subsoil was related to properties of local soil and its interaction with leachate. The potential
Water washing efficiency
ecological risk was of quite strong risk category in the MSC artificial soil and rapidly decreased from
Municipal sludge waste
moderate to slight risk in subsoil. Cadmium was the main contribution accounting for 46%e93% of
ecological risk. For landscaping applications, the composition of MSC artificial soil and local soil, as well
as the capacity of the surrounding water, needs to be considered.
© 2020 Elsevier Ltd. All rights reserved.

1. Introduction

With the rapid development of Word’s economy, huge amounts

of sludge are produced. It was reported that 1.5 Mt of sewage sludge
* Corresponding author. ;
** Corresponding author. was produced in the United Kingdom each year (Nuamah et al.,
E-mail addresses: [email protected] (F. Li), [email protected] (Z. Jin). 2012), while 6.25 Mt of dry solids in sludge were produced in

https://doi.org/10.1016/j.chemosphere.2020.128632
0045-6535/© 2020 Elsevier Ltd. All rights reserved.

Please cite this article as: F. Li, L. Shao, Y. Chen et al., Leaching characteristic of potentially toxic metals of artificial soil made from municipal
sludge compost, Chemosphere, https://doi.org/10.1016/j.chemosphere.2020.128632
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

China in 2013 (Zhang et al., 2018a). It is urgent to have a safe, other factors. If EDTA is applied to activate heavy metals in soil, its
economic, and efficient treatment and/or disposal of municipal concentration is also an important factor. SOM and EDTA often have
sludge. Compared with the high cost of incineration and the limited the opposite effect. SOM has a positive effect in the contribution of
resources occupying of landfill, (Liu et al., 2014; Feng et al., 2015; the accumulation of heavy metals in soil (Aissaoui and Barkat,
Yang et al., 2015; Zhang et al., 2017), landscaping of sludge is more 2020). Pb and Cd were reported to be bound to the sludge five
economic and environmental friendly, and make the most of the and eight times more strongly as compared to soil, respectively, due
nutrients in sludge for plant growing (Fytili and Zabaniotou, 2008; to the high amount of SOM (Souza et al., 2019). However, EDTA
Han et al., 2019; Yuan et al., 2019). The use of stable sewage sludge application enhances the mobility of heavy metals, for example, it
as a fertilizer can also regulate the physical, chemical and biological increased the concentrations of Cd and Pb by 109% and 101% in
properties of the soil (Pathak et al., 2009) and provide better plant leachates (Gul et al., 2019). These factors make the leaching
growth (Tsakou et al., 2001; Singh and Agrawal, 2007) and behavior of heavy metals more complicated and difficult to predict.
ecosystem services (Tang et al., 2019). In this paper, a column leaching study, coupled with local
Pollutants in sludge, especially heavy metals, have become a key deposition simulation, was conducted to investigate the leaching
factor limiting sludge land use (Fang et al., 2016; Liu, 2016). How- behaviors of heavy metals from artificial soil made from municipal
ever, if sewage sludge was applied in landscaping, heavy metals in sludge compost (MSC). Untreated sludge was from industrial and
the sludge could be effectively blocked from the food chain, residential area but there was no hazardous sludge. After the
avoiding direct threats to human and animal health (Grispen et al., applying different dose of EDTA. Artificial soil was different from
2006). Landscaping plant usually have high biomass yields, but ordinary soil, as characterized as high organic matter content, high
generally have very low bioconcentration factor values (Shang CEC, high pH value and other characteristics after composted and
et al., 2020). Applying chelating reagents, such as ethyl- mixed. The attenuation and migration characteristics of heavy
enediaminetetraacetic acid (EDTA), hedta-EDTA, and other organic metals in soil, as well as growth and decline of heavy metals in
acids can remarkably increase the mobility of metals and thus leachate were systematically studied, and the potential environ-
enhance plants extractive ability (Turgut et al., 2004). The addition mental risks were evaluated.
of EDTA enhanced the bio-concentration factor of Cu, Zn, Ni, Cd, and
Pb of Italian ryegrass, which were 1.9, 1.6, 4.1, 2.7 and 4.8 times that 2. Materials and method
of the control group (Li et al., 2020), while applying of
11 mmol kg1 oxalic acid had increased the biomass of Sedum and 2.1. Materials
improved its remediation efficiency of Cd from soils of low-level Cd
contamination (Hou et al., 2019). However, excessive EDTA could The experimental artificial soil was taken from Ningbo High-
inhibit plant growth (Li et al., 2020), due to its toxicity to plants and tech Zone Pure Energy Saving Technology Co., Ltd., which was
soil microorganisms, as well as its degradation (Evangelou et al., mixed with rice husk (2e4%), straw (2e4%), and lime (5e10%) after
2007). municipal sludge was aerobic composted, and can be used as soil
The combination of sludge landscaping and chelating reagent directly. The local soil was obtained from the campus of Zhejiang
assisting provides a promising sludge disposal method at present. University of technology, which is belong to fluvo-aquic soil with a
However, the prerequisite is accurate understanding heavy metal pH of 6.65, SOM of 9.32 g kg1, total phosphorus (TP) 1.07 g kg1,
leaching behavior, which is complex and metal-specific (Firdaus e and total nitrogen (TN) 1.38 g kg1 (Table 1). The physicochemical
et al., 2017). It was reported, applying sludge significantly properties of artificial soil include pH 7.98, 234 g kg1 SOM,
increased the concentration of heavy metals in the soil, and 14.9 g kg1 TP, and 11.7 g kg1 TN (Table 1). The contents of heavy
resulting in high Ni concentration of 180 mg L1 in the leachate, metals in the two soils were also listed in Table 1, together with the
which greatly exceeded the Spanish drinking water index of standard values to be followed (GB/T23486-2009 of Disposal of
20 mg L1 (Toribio and Romanya, 2006). Heavy metal leaching was sludge from municipal wastewater treatment plantdQuality of
rapid, the peak loads were general occurred in first three leaching sludge used in gardens or parks).
events (Liu et al., 2018). However different heavy metals had quite
various migration capacities in the sludge (Fang et al., 2016). For
example, Pb was much easier leaching from slags than Cu (Potysz 2.2. Design of leaching experiment
et al., 2019).
In addition, the leaching rates of heavy metals are also affected Soil column. The leaching experimental equipment is shown in
by soil organic matter (SOM), soil pH, cation exchange capacity, and Fig. 1. The main part is composed of soil column, peristaltic pump,
liquid supply tank and filtrate collection barrel. The soil column was

Table 1
Physical and chemical properties of local soil and artificial soil made from municipal sludge compost.

Index Local soil Artificial soil Sludge landscaping standard Pollutants limits for the land
(GB/T23486 e 2009) application of sewage sludge
(EPA/831-B-93-002b)

pH (1: 2.5) 6.65 7.98 6.5e8.5

Organic matter (g kg1) 9.32 234 25
Bulk weight (g cm3) 1.36 1.19 /
Moisture content (%) 19.22 26.2 40
Total phosphorus (g kg1) 1.07 14.9 Total nutrient＞3%
Total nitrogen (g kg1) 1.38 11.7
Cu (mg kg1) 27.18 48.8 1500 4300
Pb (mg kg1) 13.49 225 1000 840
Zn (mg kg1) 62.13 1397 2000 7500
Cd (mg kg1) 0.42 8.75 20 85
Ni (mg kg1) 24.31 148 200 420

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F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

2.3. Analysis test method

2.3.1. Pretreatment of soil samples

The artificial soil samples were evenly laid in a plastic tray and
placed in a dry and ventilated place; during air drying, the large
clods in the sample were manually crushed, and the leaves, stones,
small sands, and other debris in the soil were sorted out. The air-
dried sample was ground into a mortar and sieved (100 mesh) in
a mortar. After the sample was thoroughly mixed, it was placed in a
polyethylene bottle or a sample bag and stored in a dry state.

2.3.2. Soil analysis

Soil pH was determined with a glass electrode (phS-3C, Leici,
Shanghai, China) in suspensions of 1:2.5 (soil: water, w/v) (Wu
et al., 2007); The content of soil organic matter (SOM) was
measured by the K2Cr2O7 oxidation spectrophotometry method
provided by the Ministry of Environmental Protection of the Peo-
ple’s Republic of China, HJ615-2011. The total N in the amendments
was determined by the Kjeldahl method (McGill and Figueiredo,
1993). Total P was determined by phosphomolybdic blue spectro-
Fig. 1. Image of soil column for leaching experiment. photometry using UVevisible spectrophotometer (Pradhan and
Pokhrel, 2013).
In this experiment, the soil and leachate were pretreated by
closed microwave digestion (CEM MARS6, USA), contents of Cu, Pb,
made of plexiglass, with a height of 100 cm, an inner diameter of Zn, Cd and Ni were determined by flame atomic absorption spec-
20 cm and a thickness of 15 mm. The bottom was first lined with a trometry (PerkinElmer AA-800, USA). The detection limits were
thick nylon mesh, then placed from bottom to top: cleaned 0.0020, 0.020, 0.0020, 0.0010 and 0.0040 mg mL1 for Cu, Pb, Zn, Cd
ceramsite 5 cm thick (for filtration, easy for leachate discharge); a and Ni by flame-AAS, and were 0.0010, 0.0050, 0.00010, 0.00030
layer of fine nylon mesh, local soil 60 cm thick, artificial soil 20 cm and 0.0010 ng mL1 by graphite furnace-AAS, respectively.
thick (not compacted to achieve the purpose of simulating the
tillage layer), a layer of coarse nylon mesh, ceramsite 3 cm thick for 2.4. Leaching index, water washing coefficient and ecological risk
liquid buffer. The 60 cm thick local soil has a control density of assessment
1.1e1.3 g cm3 and could be compacted with a wooden stick to
prevent wall effect when leaching. Before leaching experiments, The leaching index (LI, %) is used to evaluate the leaching loss of
the artificial soil (8 kg) in the control column, and Column A, Col- heavy metals in artificial soil column, the calculation equation is as
umn B and, Column C were treated EDTA with 0, 1, 3, and follows：
5 mmol kg1 (soil), respectively, that is 0, 8, 24, and 40 mmol EDTA,
then stabilized for 7 days, leaching started. C  Ci
LIð%Þ ¼  100 (1)
Simulated rainwater and precipitation. The chemical compo- C
sition of simulated natural rainwater was Ca2þ 1.50, Naþ 6.80, NHþ 4
2.62, Mg2þ 2.00, Kþ 1.78, SO2 2
4 10.0, CO3 2.61, Cl
1
1.17, mg$L1, and where, C, and Ci (mg.kg1) are the initial and the final concentration
at last adjusted pH to 5.0, according to local precipitation, used to in artificial soil layer before and after six-leaching events,
accurately simulate the leaching and migration behavior of heavy respectively.
metals in local soil under acid rain conditions after the application The purpose of water washing coefficient (WWC) is to reflect the
of compost sludge to local soil. The amount of leaching water was migration ability of heavy metals in local soil, it is calculated using
about 1200 mm referring to the annual rainfall of 1100e1400 mm the following equation：
in Hangzhou, and a maximum rainfall is about 200 mm. The
P
n1
simulated rainfall volume is calculated as V ¼ C  S  102 , where, ðCiþ1  CÞ
V is the annual rainfall volume (L); C is annual rainfall (mm); and S WWCð%Þ ¼ i
 100 (2)
is rain collecting area (cm2). The calculated rainfall volume is P
n
ðCi  CÞ
approximate 36 L, and it was divided into six leaching events, so i
that the simulated rainfall at each leaching event is 6 L. After each
rainfall, the next leaching was carried out after 2 days of stabili- where, C is the metal concentration in local soil as a background
zation until all 6 times were completed. value; Ci and Ciþ1 are concentrations of heavy metal in layer i and
Contents of heavy metals in leachates and left in soil column. layer i þ 1 soil, respectively.
The volume of leachate was recorded by leaching every time, the The Hakanson potential ecological risk index was used in heavy
pH was measured, and the total concentration of heavy metals (Cu, metal pollution assessment (Hakanson, 1980). The calculation for-
Pb, Zn, Cd, Ni) were determined. After the leaching experiment, mula is as follows：
samples were taken 5, 10, 15, 20, 25, 30, 40, 50, 60, 70, 80 cm depth
using a ring knife sampler. The sample was air-dried, a half was Ci
Eri ¼ Tir  (3)
ground to pass 2 mm sieve, then placed in a glass bottle for Cri
determination of organic matter. The left half were ground to pass a
100-mesh sieve for total amount of heavy metals (Cu, Pb, Zn, Cd, X
n
and Ni) determination after digestion. RI ¼ Eri (4)
i¼1

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F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

RI is the comprehensive potential ecological hazard index; Eri is 3.2. Heavy metals in soil profiles
the potential ecological index of a single heavy metal i; C i is the
measured concentration of heavy metal i, Tri is the toxicity response The contents of five heavy metals in soil profile of each column
coefficient of heavy metal i, which were defined for Cu]Pb ¼ 5, were presented in Fig. 2 d e h. In control column, after six leaching
Zn ¼ 1, Cd ¼ 30, and Ni ¼ 6 (Suresha et al., 2012); n is the number of events for a total of one year’s rainfall, the average contents of Cu,
heavy metal elements; Cri is the reference ratio of heavy metal i, this Pb, Zn, Cd, and Ni in the artificial soil layers of control column were
paper adopts the second level standard of Environmental quality 42.4, 206, 1220, 8.20, and 132 mg kg1, which were decreased by
standard for soils GB 15618－1995 (Huang et al., 2018). The clas- 12.9%, 8.37%,11.5%, 5.94%, and 10.7%, respectively, compared with
sification was defined as slight, moderate, strong, quite strong, and the initial values of artificial soil in Table 1 and the grey line in Fig. 2.
extremely strong, when Eri was <30, 30e60, 60e120, 120e240, and In soil column profiles, heavy metal contents decreased from top to
>240, and RI was <60, 60e120, 120e240, 240e480, and >480. bottom. Compared with the top layer, the decrease percentages of
heavy metal contents in each soil layer ranged in 2.5%e36.5%,1.3%e
91.6%, 0.70%e94.7%, 0.48%e99.0%, and 4.2%e81.3% for Cu, Pb, Zn,
2.5. Quality control Cd, and Ni, respectively. There were obvious differences in migra-
tion rates between heavy metals (Zhang et al., 2018b).
Milli-Q water was used for all solution preparation in the Compared with the control column, the concentration of the
experiment, and all reagents were of analytical grade. All glassware above five heavy metals at artificial soil layer in EDTA treated col-
and plastic containers were washed and soaked in 10% (v/v) HNO3 umn decreased by 3.8%e14%, 3.3%e19.4%, 2.2%e33.5%, 2.4%e20.8%,
for at least 24 h prior to use, thoroughly washed with tap water, and 5.2%e25.9%, respectively. As a result, the concentration of heavy
then rinsed three times with Milli-Q water. In terms of quality metals in the lower layer of local soil increased by e 0.5%e
control, the blank experiment and parallel experiment were con- 21.1%, 9.9%e81.7%, 10.2%e136.1%, 26.3%e126.6%, and 4.3%e
ducted. The blank values were low and acceptable, and all parallel 86.4%, respectively, relative to the control group. The promotion
experiments were performed in triplicate, and the results were effect of EDTA on heavy metals leaching was obviously. In general,
expressed as their respective average values. EDTA could increase the solubility of heavy metals in soil (Gul et al.,
Certified soil reference of GBW07403 and plant reference of 2019), made heavy metals migrate down with acid rain, and the
GBW07605 obtained from the China National Center for Standard higher the EDTA concentration, the more amount of leached
Reference Materials were used as the accuracy quality control, and metals.
the relative standard deviations of the five metals were less than However, the leaching behaviors of heavy metals were quite
10%. different among elements. Leaching index (LI) of heavy metals,
calculated with Eq. (1), were listed in Table 2. The loss rates of heavy
3. Results and discussion metals expressed as LI ranged in 5.9%e12.9% and followed the order
of Cu > Zn > Ni > Pb > Cd in control column, but ranged in 10.4%e
3.1. Nitrogen, phosphorus, and organic matter in soil profiles 33.6% and followed the order of Zn > Ni > Cu > Pb > Cd in EDTA
treated columns. It was partially consistent with the order of
The contents of total nitrogen (TN), total phosphorus (TP), and Cd > Zn > Ni in a calcareous soil (Jalali and Latifi, 2018), and the
SOM were showed in Fig. 2a e c. In control column, after six order of Cd > Cu > Zn > Pb in polluted soil after applying EDTA
leaching events for a total of one year’s rainfall, the average con- 5.0 mmol kg1 (Chen et al., 2004), except Cd. Another research
tents of TN, TP, and SOM in artificial soil were 10.5, 12.9, indicated Pb was the most mobile element leaching from slags of a
215 mg kg1, decreased by 10.1%, 13.4%, and 7.8% comparing with historical copper smelting, which was exposed to Acidithiobacillus
the initial values in Table 1 (expressed as the grey dotted lines in thiooxidans mimicked the extremely acidic conditions (Potysz et al.,
Fig. 2), respectively, indicating a retention capacity order of 2019). The high pH value of 7.98 in artificial soil was a major reason
TP < TN < SOM. It was reported that compost could efficiently for the lowest leaching capacity of Cd. It had been reported that Cd
enhance soil cation exchange capacity and water holding capacity, release rates were very low at pH > 5 (Strobel et al., 2001). However,
reduced the potential leaching of nutrients (Cao et al., 2018). when EDTA dosage increased from 0 to 5 mmol kg1, LI value of Cd
Compared artificial soil treated with 1, 3, 5 mmol kg1 EDTA was growing fastest with an increase of 3.5 times, followed by Ni
with the control column, the mean loss percentage of TN increased and Zn with increases of 3.1 and 2.9 times, and the least ones were
by 9.2%, 18.7%, and 27.4%, that of TP increased by 6.0%, 18.6%, and Pb and Cu with increases 2.8 and 1.9 times, respectively. These
28.4%, and that of SOM increased by 2.3%, 7.6%, and 16.1%, respec- phenomena indicated that the promoting effect of EDTA on the
tively, increasing as treated EDTA dosage increased. It had been leaching rate of heavy metals depends on the properties of soil and
reported that EDTA leaching promoted the loss of soil total P, the nature of heavy metals.
however it increased the content of SOM and total Kjeldahl N of In order to study the rule of leaching and migration of heavy
agricultural soil (Hu et al., 2014). Differences should be due to metal elements in soil column, the water washing coefficient
different soil properties and leaching methods. In each column (WWC) of heavy metals, calculated with Eq. (2) were listed in
profile, all data points of each item formed decay lines from the top Table 3. A high WWC value corresponded to strong leaching and
down. The steep drops at 20-cm depth were attributed to the migration ability of heavy metal elements between soil layers. The
boundaries between artificial soil and local soil. The leaching loss in average WWC values were 63.3% for Cu, 55.7% for Pb, 54.1% for Zn,
the upper artificial soil caused increases in concentrations of TN, TP 53.5% for Ni, and 52.5% for Cd. A conclusion could be drawn by from
and SOM. Compare with the initial values of local soil, TN increased the data bars in Table 3 that with the increase of soil depth, the
by 3.6%e43.5% (Fig. 2a), TP increased by 23.4%e407.5% (Fig. 2b), and leaching mobility of each heavy metals at the lower layer of local
SOM increased by 5.4%e74.3% (Fig. 2c) in subsoil of the columns. soil in columns decreased gradually, which was due to the decrease
For EDTA treated columns, TN increased by 4.6%e166.0%, TP of heavy metal contents in layers of soil columns from top to bot-
increased by 44.5%e88.8%, and SOM increased by 4.5%e268%, tom. The subsoil had a certain retention effect on heavy metal
compared with the control column. At the bottom of columns, the leaching, mainly including the adsorption of soil colloid and a series
contents of TN, TP, and SOM decreased to close to the initial values of reactions (neutralization, sedimentation, complexation, etc.)
before leaching. (Johnson et al., 1996; Ong et al., 2018). However, the WWC values of
4
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

Fig. 2. Total nitrogen (a), total phosphorus (b), contents of soil organic matter (c) and heavy metals (deh) in soil column after annual rain leaching.

Table 2
Classification standard in E and Ri grading standards.

Ecological risk level Slight Moderate Strong Quite strong Extremely strong

Ei Hakanson <40 40e80 80e160 160e320 320

This study <30 30e60 60e120 120e240 240
RIi Hakanson <150 150e300 300e600 600 e
This study <60 60e120 120e240 240e480 480

different soil columns with the same metal at the same soil depth layer for each element, which mostly appeared at depth of 50 cm,
had no obvious change rule, which indicated that EDTA had little and was 30 cm for Cd and Ni. SPSS 16.0 software was performed to
effect on the retention behavior of heavy metals in the subsoil. analyze partial correlations under soil depth control, and it was
Fig. 2 d e g showed that there was a second peak in the local soil found that most heavy metals were significantly correlated with

5
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

Table 3
Leaching index and water washing coefficient of heavy metals of artificial soil columns.

Element Column EDTA dosage, mmol kg1 LI WWC

25 cm 30 cm 40 cm 50 cm 60 cm 70 cm

Cu CK 0 12.9% 82.5% 89.0% 76.1% 58.5% 53.3% 42.6%

A 1 17.0% 85.6% 75.5% 66.8% 53.9% 49.9% 52.3%
B 3 18.9% 75.6% 80.7% 71.2% 58.2% 50.4% 25.6%
C 5 24.8% 82.0% 80.2% 72.2% 60.4% 52.6% 23.6%
Pb CK 0 8.4% 86.7% 83.2% 65.8% 47.0% 41.6% 20.8%
A 1 12.7% 84.8% 78.7% 65.7% 48.4% 40.8% 13.4%
B 3 16.0% 84.4% 79.3% 64.4% 47.7% 28.4% 14.1%
C 5 23.1% 81.7% 78.6% 65.5% 45.8% 42.8% 26.1%
Zn CK 0 11.5% 74.1% 83.1% 68.4% 41.3% 21.3% 25.7%
A 1 20.1% 77.6% 75.9% 73.9% 52.9% 31.4% 14.6%
B 3 26.2% 76.3% 73.6% 68.6% 43.0% 37.4% 23.0%
C 5 33.0% 72.6% 76.5% 67.2% 45.1% 47.1% 27.7%
Cd CK 0 5.9% 75.5% 69.5% 63.3% 55.7% 42.9% 23.8%
A 1 10.4% 78.7% 68.5% 62.6% 47.9% 50.0% 35.7%
B 3 11.7% 76.3% 61.4% 49.5% 48.4% 42.2% 31.6%
C 5 20.7% 71.2% 58.7% 50.0% 41.6% 33.3% 21.4%
Ni CK 0 10.7% 87.6% 67.0% 42.4% 52.7% 56.1% 32.2%
A 1 17.2% 88.3% 63.3% 33.4% 41.6% 43.8% 38.3%
B 3 26.7% 81.3% 65.7% 44.2% 42.1% 40.1% 36.6%
C 5 33.6% 81.0% 67.6% 57.5% 47.1% 35.3% 38.5%

*LI means leaching index, and WWC means water washing coefficient of heavy metals. CK, A, B, and C represent artificial soil is treated with 0, 1, 3, and 5 mmol kg1 EDTA,
respectively.

TN, TP and SOM (Table 4). In the leaching process of artificial soil each leaching event were shown in Fig. 3, as well as pH of the
column, P was easily released during the decomposition of SOM, leachates. In the control column, pH decreased from 7.23 in the first
and then migrated down and adsorbed by soil sorption sites in the leaching to 7.08 in the sixth leaching, with an average of 7.16, and
lower layer (Moortel et al., 2012). This was very consistent with our the variation in pH was relative stable. When EDTA was added into
results in Fig. 3. Compared with SOM and N, P contents in the lower the artificial soil, pH decreased to 6.56, 6.32, and 5.74 in the first
local soil was more similar to those in the upper artificial soil (Fig. 3 leaching as EDTA doses was 1, 3, and 5 mmol kg1, respectively.
a, b, and c), and the maximum concentration occurred at the soil After that pH increased gradually as leaching times increased. By
column depth of 50 cm. Some heavy metal elements migrate and the 6th leaching, and the final values were relatively close, an
precipitate or accumulate together with P, because Phosphatic clay varied between 6.89e6.64.
has high affinity for Pb in the presence of humus soil, followed by In the control column, their concentrations in the leachate
Cu, Zn and Mn (Chaturvedi et al., 2007). Our research indicated that ranged in 0.012e0.033 mg L1 for Cu, 0.090e0.242 mg L1 for Pb,
Cu, Pb and Zn transported down in the column, with the maximum 0.018e0.460 mg L1 for Zn, 0.002e0.005 mg L1 for Cd, and
concentrations appeared near 50 cm depth, which was highly 0.004e0.089 mg L1 for Ni. According to standard of the fifth type
consistent with the former research. On the other hand, SOM and N of water, which is mainly applicable to agricultural water areas and
contents in subsoil decrease rapidly with the increase of depth, general landscape waters of the Surface Water quality Standard of
which was consistent with the changes of Cd and Ni contents, China, the standard values are 1, 0.1, 2, and 0.01 mg L1 for Cu, Pb,
which reached their maximum values at a depth of 30 cm. Zn, and Cd, respectively. The value of Ni was 0.610 mg L1 recom-
mended by the National water quality standard e Human health
standard table which was formulated with reference to the U.S.
3.3. Concentration of heavy metals in leachate
environmental protection agency. The maximum heavy metals
concentrations in the leachate were 0.03, 2.42, 0.23, 0.50, and 0.15
We measured the concentration of heavy metals in the leach-
times the above standard values, respectively. However, most
ates, which simply and directly reflected the migration ability of
heavy metal concentrations usually peaked at the second or third
heavy metals in the soil column, therefore we did not carry out
morphological analysis of heavy metals in the artificial soil. The leaching event, and then decreased, which was similar to the re-
ported (Liu et al., 2018).
concentration of heavy metals in the leachate from soil columns at
EDTA can be used as an auxiliary reagent to increase the content
Table 4 of water-soluble heavy metals in soil to improve the phytor-
Partial correlation analysis between heavy metals and soil composition in leaching emediation efficiency (Turgut et al., 2004), however it remarkably
soil columns. increased the concentrations of heavy metals in leachates. With the
Cu Zn Pb Cd Ni TN TP SOM increase of EDTA concentration, the promoting effect was more
obvious. The ratios of maximum to the standards of heavy metals in
Cu 1
Zn 0.769** 1 column A, B and C increased by 0.07e6.5, 0.15e7.7, and 0.26e9.0
Pb 0.667** 0.691** 1 times, respectively. The heavy metal concentration peaks in
Cd 0.529** 0.534** 0.368 1 leachate appeared at the fourth or fifth leaching events. This change
Ni 0.619** 0.408* 0.598** 0.774** 1 was not consistent with the change in pH. When EDTA is used to
TN 0.760** 0.738** 0.557** 0.876** 0.807** 1
TP 0.708** 0.779** 0.837** 0.442* 0.596** 0.662** 1
treat artificial soil, the selected concentration should be considered
SOM 0.705** 0.600** 0.278 0.849** 0.694** 0.896** 0.416* 1 according to the dilution capacity of the surrounding water envi-
ronment, and ecological risk assessment based on local conditions
**,*mean significant correlations at p < 0.01 and p < 0.05, respectively, with soil
depth as control variable. is needed.

6
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

Fig. 3. Heavy metal concentrations in leaching solution of soil columns.

7
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

3.4. Potential ecological risk

298.9
291.3
275.5
258.4
106.7
108.6
82.13
53.73
28.81
15.45
8.71
RI
The potential ecological risk (Eri ) of Cu, Zn, Pb and Ni, calculated
using Eq. (3), ranged from 0.27 to 13.3 (Table 5), falling into the

5.16
4.92
4.82
4.78
3.37
4.13
3.82
3.12
2.37
1.69
1.56
Ni
category of slight risk according to the recommend values (Table 2).
However, those of Cd ranged from 4.0 to 313, in which, values in

277.1
270.4
255.4
238.5
94.67
96.67
69.33
41.33
20.67
9.33
4.00
Cd 0e20 cm artificial soil were all greater than 120, reaching the quite
strong risk category. When the soil depth reached 40e50 cm, the
risk of Cd decreased to the slight risk. Though Cd is the high water
3.44
3.30
3.10
2.49
2.05
1.37
1.45
1.59
0.83
0.63
0.39
Zn
5 mmol kg1 EDTA

solubility and fluidity (Hassan and Aarts, 2011), the LI value was the
lowest among the five heavy metals both in EDTA treated or un-
11.28
10.84
10.35
10.83
4.95
4.78
5.82
5.97
3.32
2.22
1.33
treated artificial soil, due to the high contents of N and SOM (Jalali
Pb

and Latifi, 2018) and high soil pH (Strobel et al., 2001), which
allowed its risk to decrease rapidly in the subsoil of the columns.
1.91
1.86
1.81
1.76
1.71
1.67
1.71
1.72
1.62
1.58
1.43

*Values in red, purple, and yellow shades indicate quite strong, strong, and moderate risk, and the left without shades indicate slight risk, which have been defined in Table 2.
Cu
Eri

The potential ecological risk (RI) of each level in soil columns,

calculated using Eq. (4), ranged from 8.7 to 340, with Cd as the
325.0
319.4
313.6
292.0
75.32
91.39
77.39
44.79
27.28
16.07
10.21
predominated contributor accounting for 46% ~ 93%. Similar to Eri of
RI

Cd, the potential ecological risks were much higher in the upper
layer of artificial soil than the lowers. Cd was also classified under
5.66
5.32
5.12
5.62
2.79
3.50
3.64
2.40
1.81
1.55
1.46
Ni

high risk to a very high-risk category in sediment in Lake Hussain

Sagar, India (Ayyanar and Thatikonda, 2020). Therefore, in order to
301.1
296.6
291.4
270.4
65.33
80.67
65.33
34.00
19.33
10.67
6.00

reduce the ecological risk caused by Cd in artificial soils in land-

Cd

scaping, plants with good Cd remediation ability should be

prioritized.
3.75
3.44
3.29
3.08
1.47
1.29
1.16
1.38
0.78
0.49
0.32
Zn
3 mmol kg1 EDTA

The effect of heavy metals in leachate on water body will

diminish due to dilution and sorption by sediment and localized to
12.40
12.02
11.85
11.04
3.95
4.32
5.60
5.33
3.78
1.84
1.01

areas close to the landscaping site (McDowell, 2010). In fact, when

Pb

artificial soil is applying in landscaping, plant uptake can reduce the

content of available heavy metals in soil (Turgut et al., 2004; Li et al.,
2.06
2.03
1.96
1.86
1.78
1.61
1.66
1.67
1.58
1.52
1.42
Cu
Eri

2020), and the canopy interception effect can reduce runoff (Tao
et al., 2020), which will further reduce potential ecological risk.
331.0
325.3
318.8
297.9
59.87
69.45
59.77
52.48
27.94
19.66
12.87

However, this is not the focus of this work and will not be discussed
RI

further.
6.33
6.07
6.17
5.97
2.01
3.19
3.46
1.97
1.60
1.47
1.42
Ni

4. Conclusion
305.6
300.8
294.8
275.3
51.33
59.33
48.67
42.67
20.67
14.00
8.67
Cd

The leaching risks of heavy metals in artificial soil made from

municipal sludge were studied in order to better understand its risk
4.19
3.77
3.49
3.25
1.38
1.19
1.03
1.29
1.05
0.56
0.30

in land use. After six leaching events for a total of one year’s rainfall,
Zn
1 mmol kg1 EDTA

the average percentage reduction of Cu, Pb, Zn, Cd, Ni were in 12.9%,
8.37%, 11.5%, 5.94%, and 10.7%, respectively. The maximum heavy
12.70
12.58
12.41
11.48
3.64
4.16
5.04
4.99
3.14
2.22
1.06
Pb

metal concentrations in the leachate were below the standard

values, except Pb. Treating EDTA to artificial soil further enhanced
2.11
2.08
2.01
1.91
1.51
1.57
1.58
1.56
1.48
1.42
1.42

the LI of heavy metals, especially those of Zn and Cu, and increased

Cu
Eri

the heavy metal concentrations both in subsoil and in leachate.

However, it performed less effect on migration ability of heavy
339.9
337.8
334.1
325.6
52.27
49.99
45.18
36.61
26.99
17.83
9.57

metals according to values of water washing efficiency (WWE). The

RI

retention of heavy metals in subsoil was related to properties of

6.91
6.62
6.51
6.45
1.81
2.42
2.60
1.79
1.56
1.54
1.44

local soil and its retention to N and P. The potential ecological risk of
Ni
Potential ecological risk index form for heavy metals.

subsoil of local soil was moderate and mostly slight catalogue.

Selecting the appropriate EDTA concentration according to the
313.1
311.6
308.6
301.1
45.33
42.67
36.00
28.00
20.67
12.67
5.33
Cd

composition of artificial soil and local soil, with aids of phytor-

emediation, the risk of landscaping of artificial soil can be further
4.28
4.25
4.00
3.74
0.94
0.58
0.77
0.91
0.61
0.32
0.27

reduced and limited.

Zn
0 mmol kg1 EDTA

13.33
13.16
12.84
12.27

CRediT author statement

2.72
2.91
4.35
4.41
2.69
1.89
1.12
Pb

Feili Li: Conceptualization, Funding acquisition. Luze Shao:

2.22
2.16
2.11
2.01
1.47
1.42
1.47
1.51
1.46
1.42
1.41
Cu

Writing- Original draft. Yihao Chen: Methodology, Formal analysis,

Eri

Data curation. Gaoxiang Zhang: Investigation, Writing - Review

Depth (cm)

and Editing. Qingting Nie: Software. Zanfang Jin: Supervision,

Project administration.
Table 5

* Each soil column was composed of the upper layer of 20-cm

10
15
20
25
30
40
50
60
70
80
5

artificial soil made from municipal sludge compost and the lower
8
F. Li, L. Shao, Y. Chen et al. Chemosphere xxx (xxxx) xxx

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