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Progress in Chemistry 2021, Vol. 33 Issue (6): 998-1009 DOI: 10.7536/PC200731 Previous Articles   Next Articles

• Review •

Removing Heavy Metals from Sludge

Guanyi Chen1,2,3, Kexuan Han1, Caixia Liu1,4,*(), Zeng Dan2, Duo Bu2   

  1. 1 School of Environmental Science and Engineering, Tianjin University,Tianjin 300350, China
    2 School of Sciences, Tibet University, Lasa 850012, China
    3 School of Mechanical Engineering, Tianjin University of Commerce, Tianjin 300134, China
    4 Tianjin Engineering Research Center for Organic Solid Waste Treatment and Energy Utilization, Tianjin University, Tianjin 300350, China
  • Received: Revised: Online: Published:
  • Contact: Caixia Liu
  • About author:
    * Corresponding author e-mail:
  • Supported by:
    National Key Research and Development Program of China(2018YFC1900105)
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The heavy metals in sludge, especially flue gas desulphurization wastewater sludge, exceed the standard seriously, which belongs to hazardous solid waste. The annual production of sewage sludge in China has exceeded 50 million tons. It is calculated that only the annual production of flue gas desulphurization wastewater sludge in coal-fired power plants reaches 90 million tons. The heavy metals in sludge, if not disposed of properly, will cause very serious secondary pollution to the ecological environment. This paper introduces the present situation of sludge treatment at home and abroad and the determination and estimation methods of heavy metals in sludge. The advantages and disadvantages of chemical process, electrokinetic treatment, bioleaching process, thermal treatment and stabilization are summarized in detail from the aspects of principle, reaction device, research progress, and hot spot. Furthermore, the authors shed light on the existing problems and development prospects of each method. In the end, the paper puts forward the prospect of economical and efficient implementation device and technical scheme with strong application.

Contents

1 Introduction

2 Determination and Estimation methods

2.1 Determination methods

2.2 Estimation methods

3 Advanced technology for disposal of heavy metal in sludge

3.1 Chemical process

3.2 Electrokinetic treatment

3.3 Bioleaching process

3.4 Thermal treatment

3.5 Stabilization

4 Conclusion and outlook

Key words: sludge, heavy metal, treatment
Table 1 Basic physical and chemical characteristics of sludge[3⇓⇓⇓~7]
The source of sludge Water content(%) Organic content(%) pH Ash(%)
Sewage Sludge 40~80 65~81 6.5~7 15~19
Flue Gas Desulfurization Wastewater Sludge 10~15 24~28 6.9~7.5 72~76
Dyeing Waste Water Sludge 80~83 31~64 7.0~7.5
Petrochemical Wastewater Sludge 40~50 8.5~9 8~13
Electroplating Sludge 70~80 7~8
Table 2 Heavy metal content of sludge[4,5,7,8]
Parameters(mg·kg-1) Cr Ni Cu Zn Cd
Sewage Sludge 10~639 13~495 55~2867 42~3568 1~40
Flue Gas Desulfurization Wastewater Sludge 440~1133 166~436 52~80 573~973 187~278
Dyeing Waste Water Sludge 132~197 0~26 150~190 2965~3745 130~152
Electroplating Sludge 6 33 128.6
Limit Value① 150 60 50 200 0.3
Table 3 Criteria of Geoaccumlation Index
Igeo level Igeo value Contamination level
0 Igeo≤0 Practically uncontaminated
1 0<Igeo≤1 Uncontaminated to moderately contaminated
2 1<Igeo≤2 Moderately contaminated
3 2<Igeo≤3 Moderately to strongly contaminated
4 3<Igeo≤4 Strongly contaminated
5 4<Igeo≤5 Strongly to extremely contaminated
6 5<Igeo Extremely contaminated
Table 4 Grouping criteria of potential ecological risk index
Grade Er Grades of ecological risk of single metal RI Grades of potential ecological risk of the environment
A Er≤40 Low risk(LR) RI<150 Low risk(LR)
B 40≤Er<80 Moderate risk(MR) 150≤RI<300 Moderate risk(MR)
C 80≤Er<160 Considerable risk(CR) 150≤RI<300 Considerable risk(CR)
D 160≤Er<320 High risk(HR) RI>320 Very high risk(VHR)
E Er≥320 Very high risk(VHR)
Table 5 Comparison of chemical process with different medicaments[15⇓⇓⇓⇓⇓⇓~22]
Agents The source of sludge Dosage Mechanism Remove rate
Citric Acid Electroplating Sludge 0.5 mol·kg-1(0.5 mol·L-1*1000 mL·kg-1) Decrease of pH values Cr 69%, Cu 57%
Nitric Acid(HNO3) Electroplating Sludge 1 mol·kg-1(1 mol·L-1*1000 mL·kg-1) Decrease of pH values Cr 76%, Cu 33%
Perhydrol(H2O2) + Nitric Acid(HNO3) Electroplating Sludge 1 mol·kg-1(1 mol·L-1*1000 mL·kg-1) Decrease of pH values and increase of oxidation-reduction potential Cr 84%, Cu 77%
Ethylene Diamine Tetraacetic Acid(EDTA) +Citric Acid Sewage Sludge CEDTA=0.125 mol·L-1, CCA=0.6 mol·L-1 Chelation and decrease of pH values Cu 39%, Zn 42%
Cd 24%, Pb 44%
Citric Acid Sewage Sludge and Soil(1∶1) 0.1 mol·kg-1
(1 mol·L-1*0.1 L·kg-1) 		Decrease of pH values Cr 49%, Cu 50%
Zn 90%, Cd 74%
Pb 87%
Ethylene Diamine Tetraacetic Acid(EDTA) Sewage Sludge and Soil(1∶1) 0.0125 mol·kg-1
(0.125 mol·L-1*0.1 L·kg-1) 		Chelation Cr 49%, Cu 39%
Cd 43%, Pb 48%
Polyepoxysuccinic Acid
(PESA) 		0.12 kg·kg-1(30 g·L-1*0.004 L·kg-1,pH=6) Chelation Hg 63%
Acrylic Acid-Maleic
Anhydride Copolymers 		0.1 kg·kg-1(30 g·L-1*0.0033 L·kg-1,pH=9) Chelation Hg 28%
Polyepoxysuccinic Acid
(PESA) 		Manganese Slag 0.1 kg·kg-1(pH=4) Chelation Cr 95%
Aspartic acid Sewage Sludge 0.09 kg·kg-1, pH=3 Chelation Cu 43%, Zn 69%
Ni 66%
N,N-bis(carboxymethyl)
glutamic acid(GLDA) 		Electroplating Sludge 0.6 kg·kg-1, pH=4 Chelation Cu 84%, Cd 89%
Ni 82%
Fig.1 The reactor of electrokinetic treatment[27,29]:(a)cuboid;(b)cylindrical
Table 6 Comparison of electrokinetic treatment with different experimental condition[26⇓~28,30]
Pretreatment The source of
sludge 		Mechanism Experimental condition Remove Rate Power Consumption
(kW·h·kg-1)
Deionized Water Sewage Sludge + Soil Electromigration,electrodialysis and electrophoresis. 2 V·cm-1, 150 h Cu 1%
Pb 2% 		0.40
Polyepoxysuccinic Acid(PESA) Application of PASP as anode working fluid can slow down corrosion of uninduced steel electrodes 2 V·cm-1, 150 h Cu 46%
Pb 33% 		0.83
Citric Acid Citric acid transformed residual fraction heavy metal into unstable fraction. 2 V·cm-1, 150 h Cu 16%
Pb 22% 		0.82
Polyepoxysuccinic Acid(PESA) + Citric Acid PASP and citric acid enhanced chelation effect. 2 V·cm-1, 150 h Cu 18%
Pb 29% 		1.35
Deionized Water Sewage Sludge Electromigration,electrodialysis and electrophoresis. 1.5 V·cm-1, pH=6, 5 d Pb 28%
Ammonia Sewage Sludge Ammonia increased the proportion of acid soluble fraction heavy metals. Vammonia:Vwater:Vsludge= 0.4∶1∶4 Cu 66%
Pb 41%
Zn 81% 		1.1
Ethylenediamine Addition of ethylenediamine does not affect sludge acidification and current density. Vammonia:Vwater:Vsludge=0.2∶1∶4 Cu 65%
Pb 53%
Zn 82% 		1.2
Magnetization Sewage Sludge The applied magnetic field produces a greater current density 2 V·cm-1, 9.5 mT,
15 g·L-1, 6 h 		Cd 97%
Pb 28%
Zn 89% 		0.07
Rhamnolipid Sewage Sludge Rhamnolipid has strong functional groups to form mobile heavy metal complexes and it can reduce the surface tension and increase heavy metals solubility 2 V·cm-1, 192 h,
2 g·L-1 		Cu 56%
Pb 52%
Zn 74%
Cr 64% 		0.06
Sodium nitrate(NaNO3) Municipal Sludge Addition of NaNO3 effect the current density and pH. 2.0 mA/cm2, 132 h Cu 83%
Ni 75% 		2.39
Table 7 Comparison of bioleaching process with different kinds of bacteria[39⇓⇓⇓⇓⇓⇓~46]
Microbial strain The Source of Sludge Substrate Dosage Removal Rate
Thiobacteria Sewage Sludge Sulfur(7.5 g/L) +FeSO4·7H2O(2.5 g/L) 10% Cd 96%
Thiobacteria Sewage sludge Sulfur(10 g/L) 5% Cu 58%, Zn 63%
Cd 48%, Cr 38%
FeSO4(10 g/L) 5% Cu 90%, Zn 60%
Cd 60%, Cr 58%
Thiobacillus Acidophilus Sewage sludge Na2S2O3(10 g/L) 10% Cu 67%, Zn 89%
Cd 82%, Ni 67%
Thermophilic Sulfur-oxidizing
Bacteria 		Sewage sludge Sulfur(2 g/L) 2% Cu 41%, Zn 61%
Ni 48%, Mn 99%
Acidithiobacillus thiooxidans
TS6 and Acidothiobacillus
ferrooxidans LX5 		Municipal sewage sludge Sulfur(2 g·L-1) + Fe(2 g·L-1) 10% Cu 85%, Cr 40%
Thiobacillus Acidophilus Sewage sludge Sulfur(8 g/L) +FeSO4 10% Cu 94%, Zn 95%
Cr 85%, Ni 86%
Pb 89%
Thiobacillus acidophilu Sewage sludge FeSO4·7H2O(20 g/L) +H2SO4(20 mL/L) 10% Cu 91%, Zn 99%
Cr 83%, Ni 87%
Pb 52%
Fig. 2 A typical thermal treatment reactor[51]
Table 8 Comparison of thermal treatment with different reaction temperature[49,50,52⇓⇓⇓ ~56]
The Source of Sludge Final temperature Time Increase of residue fraction of heavy metals
Cr Mn Ni Cu Zn Cd Pb
Sewage sludge 140 ℃ 8 h 2% - - 3% 8% 5% 1%
Dewatered Sewage sludge 190 ℃ - - - - 19% 87% 25% 0%
Acidic Sludge 160 ℃(Hydrothermal Treatment) +600 ℃(Pyrolysis) - - - 20% - 24% - -
Alkaline Sludge 13% - - 2% - -
Mixed Sludge 9% 11% 1% 34% 13% - -
Sewage sludge 220 ℃ - 18% 21% 40% 18% 9% - -
Anaerobic Digested Sludge 170 ℃ 1 h 8% - 11% 7% 4% 2% 5%
Digested Sludge 200 ℃(Hydrothermal Treatment) +950 ℃(Pyrolysis) 0.5 h+0.5 h 52% 29% 22% 43% 29% 20% 28%
Anaerobic Digested Sludge 280 ℃ 1 h 6% - 17% 7% 3% 0% 22%
Table 9 Comparison of recruitment of stable heavy metals by stabilization with different drugs[62⇓~64,67⇓ ~69]
The Source of Sludge Agent Dosage Remove rate
Cr Mn Ni Cu Zn Cd Pb
Dewatered Sewage Sludge FeSO4·7H2O 15% 2% 12% 10% 17% 7% - 6%
Residual Activated Sludge Na2S 50mg/L - 53% 41% 51% 51% 94% 35%
Dewatered Sewage Sludge (NH4)2S 2% - - 8% 5% 5% - -
Sewage Sludge Na2S·9H2O 10% - - 17% 20% 0% - -
Sewage Sludge and Soil Lime 2% - - 0% 1% 0% - 2%
Lime + Cow Dung 2% - - 2% 1% 4% - 2%
Table 10 Comparison of different heavy metal processes of sludge
Method Influencing Factor Advantage Disadvantage Scope of Application
Chemical Process Agent, Fraction of Metal Strong Adaptability Secondary Pollution Sludge with high content of heavy metals
Electrokinetic Treatment Microbial Strain, Properties of Sludge, Temperature, pH Low Cost, Low efficiency Special Reactor, Strict conditions Sludge that suitable for specific strain growth.
Bioleaching Process Temperature, Fraction of
Metal 		High removal rate,
Environment-friendly 		Strict conditions, High cost Sludge with high content of organic material
Thermal Treatment Agent, Properties and
Fraction of Metal 		Low Cost, Short Time High cost Sludge with high proportion of unstable fraction heavy metals
Stabilization Properties of Sludge, pH High efficiency,
Less influence on sludge 		Hidden danger of heavy metal re-release Sludge with high proportion of unstable fraction heavy metals
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Abstract

Removing Heavy Metals from Sludge