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Econ. Environ. Geol. 2021; 54(1): 21-33
Published online February 28, 2021
https://doi.org/10.9719/EEG.2021.54.1.21
© THE KOREAN SOCIETY OF ECONOMIC AND ENVIRONMENTAL GEOLOGY
Evaluation of Stabilization Capacity for Typical Amendments based on the Scenario of Heavy Metal Contaminated Sites in Korea
Correspondence to : heelee@pknu.ac.kr
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided original work is properly cited.
Abstract
The purpose of this study is to determine the order of priority for the use of amendments, matching the optimal amendment to the specific site in Korea. This decision-making process must prioritize the stabilization and economic efficiency of amendment for heavy metals and metalloid based on domestic site contamination scenarios. For this study, total 5 domestic heavy metal contaminated sites were selected based on different pollution scenarios and 13 amendments, which were previously studied as the soil stabilizer. Batch extraction experiments were performed to quantify the stabilization efficiency for 8 heavy metals (including As and Hg) for 5 soil samples, representing 5 different pollution scenarios. For each amendment, the analyses using XRD and XRF to identify their properties, the toxicity characteristics leaching procedure (TCLP) test, and the synthetic precipitation leaching procedure (SPLP) test were also conducted to evaluate the leaching safety in applied site.
From results of batch experiments, the amendments showing > 20% extraction lowering efficiency for each heavy metal (metalloid) was selected and the top 5 ranked amendments were determined at different amount of amendment and on different extraction time conditions. For each amendment, the total number of times ranked in the top 5 was counted, prioritizing the feasible amendment for specific domestic contaminated sites in Korea. Mine drainage treatment sludge, iron oxide, calcium oxide, calcium hydroxide, calcite, iron sulfide, biochar showed high extraction decreasing efficiency for heavy metals in descending order. When the economic efficiency for these amendments was analyzed, mine drainage treatment sludge, limestone, steel making slag, calcium oxide, calcium hydroxide were determined as the priority amendment for the Korean field application in descending order.
Keywords stabilization, soil contamination, soil remediation, amendment, mine drainage treatment sludge, steel making slag
국내 중금속 부지오염시나리오를 고려한 안정화제의 중금속 안정화 효율 규명
양지혜 · 김단우 · 오유나 · 전소영 · 이민희*
부경대학교 지구환경과학과
요 약
국내 오염시나리오별 안정화 효율과 경제성이 뛰어난 안정화제를 선택하여 적용할 수 있도록, 국내외에서 연구된 대표적인 안정화제를 대상으로 국내 중금속 오염 현장 부지 특성별 중금속 안정화 효율이 높은 안정화제 순위를 결정하였다. 총 5종류의 오염시나리오를 가정하여 각각 해당되는 국내 오염부지 토양을 확보하였다. 국내외 활용도와 안정화 효율 연구 결과, 오염특성별 부지 시나리오에 적용 가능성 등을 고려하여 기존에 연구되었던 안정화제 13가지를 선정하였다. 선정한 오염 토양과 안정화제의 오염 가능성과 현장 적용 가능성을 평가하기 위하여 XRD/XRF 분석, 독성용출시험과 인공강우용출시험 등을 실시하였다. 부지 오염시나리오를 대표하는 5종류 오염 토양에 대하여 선정된 13종의 안정화제에 의한 비소, 수은, 납, 6가 크롬, 아연, 니켈, 구리 등 총 8종의 중금속(반금속인 비소 포함) 용출 저감 효과를 규명하는 용출 배치실험을 수행하였다.
총 5개 오염 토양에 대하여 13개 안정화제 주입 비율 3%, 5%, 7% 적용 시, 각 중금속(비소 포함)에 대한 중금속 용출 저감 효율이 안정화제를 주입하지 않은 토양 대비 20% 이상을 나타내는 안정화제 중에서 저감 효율이 높은 순위부터 5개 안정화제(Top 5)를 선택하였다. 각 안정화제에 대하여 안정화제 주입비율, 중금속 종류, 부지별 조건에 따라 수행된 배치실험 결과에 대하여 Top 5에 해당하는 총 횟수를 합산하여, 다양한 국내 부지 오염시나리오에 적용할 수 있는 안정화제의 순위를 결정하였다. 5개 오염토양에 대하여 8개 중금속 항목별 용출 저감 효율이 20% 이상인 경우, 가장 안정화 효율이 높은 순위는 광산배수처리 슬러지(mine drainage treatment sludge), 산화철, 생석회, 소석회-석회석, 황화철, 바이오차 순으로 나타났다. 위 안정화제들에 대하여 안정화제의 효율대비 단가를 산정한 결과, 광산배수처리 슬러지, 석회석, 제강슬래그(비소의 경우), 생석회, 소석회 순으로 경제성이 높게 나타나 현장 적용성이 뛰어난 것으로 밝혀졌다.
주요어 토양 안정화, 토양 오염, 토양 정화, 안정화제, 광산배수 슬러지, 제강슬래그
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Research Paper
Econ. Environ. Geol. 2021; 54(1): 21-33
Published online February 28, 2021 https://doi.org/10.9719/EEG.2021.54.1.21
Copyright © THE KOREAN SOCIETY OF ECONOMIC AND ENVIRONMENTAL GEOLOGY.
Evaluation of Stabilization Capacity for Typical Amendments based on the Scenario of Heavy Metal Contaminated Sites in Korea
Jihye Yang, Danu Kim, Yuna Oh, Soyoung Jeon, Minhee Lee*
Department of Earth Environmental Sciences, Pukyong National University
Correspondence to:heelee@pknu.ac.kr
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided original work is properly cited.
Abstract
The purpose of this study is to determine the order of priority for the use of amendments, matching the optimal amendment to the specific site in Korea. This decision-making process must prioritize the stabilization and economic efficiency of amendment for heavy metals and metalloid based on domestic site contamination scenarios. For this study, total 5 domestic heavy metal contaminated sites were selected based on different pollution scenarios and 13 amendments, which were previously studied as the soil stabilizer. Batch extraction experiments were performed to quantify the stabilization efficiency for 8 heavy metals (including As and Hg) for 5 soil samples, representing 5 different pollution scenarios. For each amendment, the analyses using XRD and XRF to identify their properties, the toxicity characteristics leaching procedure (TCLP) test, and the synthetic precipitation leaching procedure (SPLP) test were also conducted to evaluate the leaching safety in applied site.
From results of batch experiments, the amendments showing > 20% extraction lowering efficiency for each heavy metal (metalloid) was selected and the top 5 ranked amendments were determined at different amount of amendment and on different extraction time conditions. For each amendment, the total number of times ranked in the top 5 was counted, prioritizing the feasible amendment for specific domestic contaminated sites in Korea. Mine drainage treatment sludge, iron oxide, calcium oxide, calcium hydroxide, calcite, iron sulfide, biochar showed high extraction decreasing efficiency for heavy metals in descending order. When the economic efficiency for these amendments was analyzed, mine drainage treatment sludge, limestone, steel making slag, calcium oxide, calcium hydroxide were determined as the priority amendment for the Korean field application in descending order.
Keywords stabilization, soil contamination, soil remediation, amendment, mine drainage treatment sludge, steel making slag
국내 중금속 부지오염시나리오를 고려한 안정화제의 중금속 안정화 효율 규명
양지혜 · 김단우 · 오유나 · 전소영 · 이민희*
부경대학교 지구환경과학과
요 약
국내 오염시나리오별 안정화 효율과 경제성이 뛰어난 안정화제를 선택하여 적용할 수 있도록, 국내외에서 연구된 대표적인 안정화제를 대상으로 국내 중금속 오염 현장 부지 특성별 중금속 안정화 효율이 높은 안정화제 순위를 결정하였다. 총 5종류의 오염시나리오를 가정하여 각각 해당되는 국내 오염부지 토양을 확보하였다. 국내외 활용도와 안정화 효율 연구 결과, 오염특성별 부지 시나리오에 적용 가능성 등을 고려하여 기존에 연구되었던 안정화제 13가지를 선정하였다. 선정한 오염 토양과 안정화제의 오염 가능성과 현장 적용 가능성을 평가하기 위하여 XRD/XRF 분석, 독성용출시험과 인공강우용출시험 등을 실시하였다. 부지 오염시나리오를 대표하는 5종류 오염 토양에 대하여 선정된 13종의 안정화제에 의한 비소, 수은, 납, 6가 크롬, 아연, 니켈, 구리 등 총 8종의 중금속(반금속인 비소 포함) 용출 저감 효과를 규명하는 용출 배치실험을 수행하였다.
총 5개 오염 토양에 대하여 13개 안정화제 주입 비율 3%, 5%, 7% 적용 시, 각 중금속(비소 포함)에 대한 중금속 용출 저감 효율이 안정화제를 주입하지 않은 토양 대비 20% 이상을 나타내는 안정화제 중에서 저감 효율이 높은 순위부터 5개 안정화제(Top 5)를 선택하였다. 각 안정화제에 대하여 안정화제 주입비율, 중금속 종류, 부지별 조건에 따라 수행된 배치실험 결과에 대하여 Top 5에 해당하는 총 횟수를 합산하여, 다양한 국내 부지 오염시나리오에 적용할 수 있는 안정화제의 순위를 결정하였다. 5개 오염토양에 대하여 8개 중금속 항목별 용출 저감 효율이 20% 이상인 경우, 가장 안정화 효율이 높은 순위는 광산배수처리 슬러지(mine drainage treatment sludge), 산화철, 생석회, 소석회-석회석, 황화철, 바이오차 순으로 나타났다. 위 안정화제들에 대하여 안정화제의 효율대비 단가를 산정한 결과, 광산배수처리 슬러지, 석회석, 제강슬래그(비소의 경우), 생석회, 소석회 순으로 경제성이 높게 나타나 현장 적용성이 뛰어난 것으로 밝혀졌다.
주요어 토양 안정화, 토양 오염, 토양 정화, 안정화제, 광산배수 슬러지, 제강슬래그
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Table 1 . Soil samples based on 5 different pollution scenarios.
Type of pollution scenario Pollution Source Main target Soil name Abandoned mine site Oxidation of sulfide mineral (including AMD) As and Hg Farm land soil (S1) As and Hg Mine tailing storage site soil (S2) Residential area (required In-situ cleanup process) Heavy metal waste Heavy metals such as Pb, Zn and Ni Illegal metal and construction waste storage site soil (S3) Steep slope site (required In-situ cleanup process) Artillery shell fragments Heavy metals such as Cu and Zn Military bomb test site soil (S4) Multi-contaminated site Heavy metal and oil waste TPH + heavy metals (Pb, Zn, Cu and Cr+6) Waste storage site soil (S5)
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Table 2 . The evaluation criteria used in the ranking for amendments.
Evaluation grade Evaluation criteria Color index Excellent ● Three or more cases, showing the extraction lowering efficiency ≥ 50% Green Good ●One or two cases, showing the extraction lowering efficiency ≥ 50% + More than one case, showing the extraction lowering efficiency 20 – 50% Blue ● Three or more cases, showing the extraction lowering efficiency 20 – 50% Intermediate ●One case, showing the extraction lowering efficiency ≥ 50% + More than one case, showing the extraction lowering efficiency 0 - 20% Yellow ●More than one case, showing the extraction lowering efficiency 20 – 50% + More than one case, showing the extraction lowering efficiency 0 – 20% ● Three or more cases, showing the extraction lowering efficiency 0 - 20% Weak ●Other cases (showing no distinct extraction lowering efficiency) Oringe Exclusion for evaluation ●When the concentration of extracted water for the initial soil (without amendment) was less than 0.005 mg/L White
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Table 3 . The pH and extraction results for 5 soil samples.
Soil type pH Type of extraction Concentration of extracted solution (Unit: mg/L or mg/kg) Cd Cu Pb Ni Zn As Hg Cr+6 S1 8.01 TCLP 0.000 0.000 0.000 0.000 0.875 0.318 0.076 0.000 SPLP 0.000 0.004 0.000 0.000 0.000 0.147 0.014 0.000 Aqua regia extraction(1) 57.86 16.73 337.75 12.57 245.84 136.28 4.7 2.520 S2 8.06 TCLP 0.033 0.018 0.000 0.038 1.973 1.550 0.144 0.000 SPLP 0.024 0.006 0.087 0.003 0.117 1.251 0.063 0.000 Aqua regia extraction(1) 3.50 32.97 39.63 11.00 133.20 2225.28 27.3 2.084 S3 7.26 TCLP 0.245 3.973 0.865 0.180 73.320 0.025 - 0.000 SPLP 0.000 0.112 0.153 0.827 0.524 0.009 - 0.000 Aqua regia extraction(1) 36.63 1560.11 1606.06 119.47 4796.87 75.01 - 4.476 S4 7.91 TCLP 0.028 1.617 2.145 0.008 7.146 0.000 - 0.000 SPLP 0.000 0.078 0.009 0.000 1.083 0.000 - 0.000 Aqua regia extraction(1) 3.410 451.300 76.920 6.580 702.960 6.330 - 1.088 S5 6.15 TCLP 0.825 3.345 28.943 0.195 26.110 0.030 - 0.000 SPLP 0.000 0.008 0.009 0.000 0.028 0.000 - 0.000 Aqua regia extraction(1) 45.12 366.05 1573.26 57.44 2428.74 5.24 - 8.364 Tolerance limit of waste extraction process (TLWEP) 0.300 3.000 3.000 - - 1.500 0.005 1.500 * Unit of (1): mg/kg; Red color: ≥ TLWEP.
* Red: ≥ soil pollution warning limit of 3 area; yellow: ≥ soil pollution warning limit of 2 area; green: ≥ soil pollution warning limit of 1 area.
* -: no data.
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Table 4 . Chemical compositions of amendments from XRF analysis.
Compound Weight % Biochar1 Biochar2 Steel making slag1 Steel making slag2 CMDS MMDS CaO Ca(OH)2 Calcite SiO2 88.2 26.92 13.06 29.74 8.67 7.99 5.26 1.79 1.88 Al2O3 10.32 2.01 12.13 10.03 9.74 2.99 0.82 Fe2O3 4.66 26.59 24.27 38.79 30.84 0.85 0.61 CaO 1.56 22.56 44.65 19.31 34.57 27.28 84.33 84.77 96.65 MgO 0.91 5.58 5.84 4.28 5.1 7.91 5.6 11.08 MnO 0.13 0.27 3.08 6.68 0.97 1.12 CuO 2.34 ZnO 2.12 Na2O 4.37 K2O 4.95 7.22 0.17 0.23 0.17 P2O5 1.35 3.98 2.42 0.07 TiO2 0.51 0.59 0.91 V2O5 0.56 Cr2O5 0.35 1.87 SO3 2.77 13.59 0.85 0.64 1.86 10.65 0.67 0.74 1.47 Cl Total 99.87 99.98 100 100 99.99 99.99 100 99.98 100
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Table 5 . Major minerals of amendment resulted from XRD analysis.
Amendment Major minerals Formula Properties Iron sulfate Rozenite FeSO4•4(H2O) The secondary mineral originated from melanterite (FeSO4•7(H2O)) Biochar1 Cristobalite SiO2 Amorphous organic material with small dose of cristobalite and calcite Calcite CaCO3 Organic material - Biochar2 Dolomite CaMg(CO3)2 Amorphous organic material with dolomite, calcite and small dose of quartz Calcite CaCO3 Quartz SiO2 Organic material - Steel making slag1 Wuestite FeO Amorphous silicate minerals with wuestite and brownmillerite Brawonmillerite Ca2(Al,Fe)2O5 Steel making slag2 Dolomite CaMg(CO3)2 Amorphous silicate minerals with dolomite and pyroxene Pyroxene CaFeSi2O6 Coal mine drainage sludge (CMDS) Aragonite CaCO3 Aragonite, calcite and quartz with amorphous iron bearing silicate minerals Calcite CaCO3 Quartz SiO2 Metal mine drainage sludge (MMDS) Calcite CaCO3 Calcite and gypsum with amorphous iron bearing silicate minerals Gypusum CaSO4•2(H2O) Calcium oxide Lime CaO Lime with small dose of portlandite and quartz Portlandite Ca(OH)2 Quartz SiO2 Calcium hydroxide Portlandite Ca(OH)2 Portlandite with calcite Calcite CaCO3 limestone Calcite CaCO3 Calcite with small dose of quartz Quartz SiO2
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Table 6 . Extraction results for amendments.
Amendment pH Type of extraction Concentration of extracted solution (Unit: mg/L) Cd Cu Pb Ni Zn As Hg Cr+6 Iron sulfide 3.33 TCLP 0.000 0.000 0.037 0.000 0.019 0.000 0.000 0.000 SPLP 0.000 0.000 0.623 0.000 0.124 0.000 0.000 0.000 Biochar1 9.85 TCLP 0.000 0.000 0.000 0.000 0.569 0.000 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Biochar2 7.34 TCLP 0.047 0.052 0.073 0.020 1.859 0.018 0.000 0.000 SPLP 0.005 0.033 0.034 0.009 0.187 0.014 0.000 0.118 Steel making slag1 9.28 TCLP 0.000 0.000 0.000 0.000 0.000 0.008 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Steel making slag2 8.31 TCLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.087 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Coal mine drainage sludge (CMDS) 8.65 TCLP 0.000 0.000 0.000 0.070 0.012 0.000 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Metal mine drainage sludge (MMDS) 9.39 TCLP 0.000 0.000 0.000 0.000 0.071 0.000 0.000 0.000 SPLP 0.000 0.014 0.000 0.000 0.000 0.000 0.000 0.000 Calcium oxide 12.63 TCLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Calciumhydroxide 12.46 TCLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.010 0.000 0.000 Limestone 8.81 TCLP 0.000 0.000 0.000 0.000 0.019 0.000 0.000 0.000 SPLP 0.000 0.000 0.000 0.000 0.000 0.000 0.000 0.000 Tolerance limit of waste extraction process (TLWEP) 0.300 3.000 3.000 - - 1.500 0.005 1.500
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Table 7 . The pH change of soil after the addition of amendment (0 – 7%).
Amendment % pH Amendment % pH S3 soil S2 soil S1 soil S4 soil S3 soil S2 soil S1 soil S4 soil Iron oxide 0 8.0 6.9 7.8 7.1 Steel making slag1 0 8.0 7.1 7.9 6.6 1 8.1 7.0 7.9 7.3 1 8.3 8.6 9.0 8.3 3 8.1 7.1 7.8 7.1 3 9.8 10.4 10.3 9.3 5 8.1 7.1 8.0 6.5 5 9.9 10.7 11.0 10.6 7 8.0 7.2 7.7 6.8 7 10.2 11.3 11.0 10.6 Manganese oxide 0 8.1 6.9 7.8 7.2 CMDS 0 8.3 7.3 7.6 6.4 1 8.2 7.5 7.9 7.5 1 8.2 8.2 7.9 8.0 3 8.1 7.3 7.9 7.3 3 8.2 8.3 8.1 8.2 5 8.1 7.6 7.9 7.5 5 8.2 8.4 8.2 8.3 7 8.2 7.5 7.7 7.2 7 8.4 8.3 8.2 8.4 Iron sulfide 0 8.1 7.0 8.0 7.3 Calcium oxide 0 8.2 7.1 7.8 6.4 1 8.1 6.9 7.8 7.3 1 11.0 12.0 12.0 12.2 3 8.1 6.3 7.6 7.0 3 12.4 12.7 12.6 12.7 5 8.0 6.6 7.4 5.2 5 12.7 12.7 11.8 12.8 7 7.9 5.2 7.3 5.6 7 12.7 12.7 11.7 12.8 Iron sulfate 0 8.0 6.9 7.9 7.3 Calcium hydroxide 0 8.2 7.4 7.5 6.4 1 7.4 4.2 5.0 4.1 1 11.0 11.5 11.4 12.1 3 5.9 3.8 4.1 3.7 3 12.4 11.9 12.1 12.7 5 4.4 3.7 3.9 3.4 5 12.6 12.0 12.3 12.8 7 4.5 3.6 3.8 3.3 7 12.7 12.5 12.1 12.8 Zero iron 0 8.1 7.1 7.8 6.7 Limestone 0 8.3 7.7 7.9 6.4 1 8.0 7.2 7.9 6.7 1 8.3 8.4 7.9 7.7 3 8.1 7.3 7.8 6.9 3 8.3 8.2 8.4 7.9 5 8.0 7.6 7.9 7.6 5 8.3 8.3 7.9 7.8 7 8.1 7.7 7.8 7.4 7 8.3 8.3 7.9 7.9 Biochar1 0 8.3 7.3 7.8 6.4 MMDS 0 8.2 7.5 7.9 6.2 1 8.1 7.5 7.9 6.3 1 8.2 8.2 8.1 7.9 3 8.1 7.8 8.1 7.3 3 8.1 7.7 8.3 7.6 5 8.1 8.0 8.2 7.5 5 8.3 7.7 8.7 7.8 7 8.1 8.0 8.2 7.7 7 8.5 7.6 9.1 7.9 Steel making slag2 0 8.1 7.1 7.9 6.9 1 8.1 7.7 8.1 7.2 3 8.1 7.6 8.2 7.5 5 8.1 8.0 8.2 7.7 7 8.1 8.1 8.2 7.7
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Table 8 . Ranking of amendments for heavy metals (metalloid) based on the stabilization efficiency.
3% addition 5% addition 7% addition Total case number Rank Amendment Cases ranked in the top 5 Amendment Cases ranked in the top 5 Amendment Cases ranked in the top 5 Iron oxide 6 Iron oxide 10 Iron oxide 13 29 3 Manganese oxide 3 Manganese oxide 1 Manganese oxide 1 5 Iron sulfide 5 Iron sulfide 6 Iron sulfide 9 20 Iron sulfate 4 Iron sulfate 4 Iron sulfate 3 11 Zero iron 1 Zero iron 1 Zero iron 1 3 Biochar 8 Biochar 5 Biochar 5 18 Steel making slag1 0 Steel making slag1 5 Steel making slag1 3 8 Steel making slag2 0 Steel making slag2 2 Steel making slag2 4 6 CMDS 25 CMDS 20 CMDS 14 59 1 Calcium oxide 9 Calcium oxide 9 Calcium oxide 6 24 4 Calcium hydroxide 9 Calcium hydroxide 8 Calcium hydroxide 6 23 5 Limestone 9 Limestone 9 Limestone 5 23 5 MMDS 19 MMDS 7 MMDS 6 32 2
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Table 9 . The analysis for the economic efficiency of amendments.
Amendment S3 soil S2 soil A. Manufacturing (or purchasing cost)/kg (won) B. The average of stabilization efficiency for Zn and Pb The ratio A/B (won) A. Manufacturing (or purchasing cost)/kg (won) B. The average of stabilization efficiency for As The ratio A/B (won) Iron oxide 8,500 87% 9,970 8,500 93% 9,140 CMDS 101 84% 120 101 99% 102 MMDS 101 88% 115 101 99% 102 Limestone 14 78% 18 14 61% 23 Zero iron 92,100 22% 418,636 92,100 28% 328,929 Iron sulfate 3,240 - - 3,240 100% 3,240 Steel making slag1 78 - - 78 33% 236 Biochar1 2,143 77% 2783 2,143 - - Calcium oxide 130 37% 351 130 97% 134 Calcium hydroxide 270 57% 474 270 97% 278
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