Evaluation of Characteristics of Sludge generated from Active Treatment System of Mine Drainage

Jung-Eun Kim; Won Hyun Ji

doi:10.9719/EEG.2023.56.4.409

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Econ. Environ. Geol. 2023; 56(4): 409-419

Published online August 30, 2023

https://doi.org/10.9719/EEG.2023.56.4.409

Evaluation of Characteristics of Sludge generated from Active Treatment System of Mine Drainage

Jung-Eun Kim^1,2, Won Hyun Ji^2,*

Author Info. +

¹National Environment Lab. (NeLab), Seoul, 02841, Korea
²Department of Energy & Climate Environment Fusion Technology, Graduate shool Hoseo University, Asan, 31499, Korea

Correspondence to : ^*greenidea@hoseo.edu

Received: March 13, 2023; Revised: July 13, 2023; Accepted: August 4, 2023

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

Acid mine drainage(AMD) treatment is classified as both passive and active treatment. During the treatment, about 5,000 tons of neutralization sludge is generated as a by-product per year in Korea. This study was conducted to evaluate the characteristics of sludge generated from physico·chemical treatment processes as an active treatment from 5 different sources (D, H, S, T, Y) and the possibility of the sludges being recycled. The sludges have a pH range of 5.86 ~ pH 7.89, and a water content range of 51% ~ 82%. Most of particle sizes were less than 25 μm. In analysis of inorganic elements, the concentration of Al, Fe, and Mn were between 1,189 mg/kg ~ 129,344 mg/kg, 106,132 mg/kg ~ 338,011 mg/kg, and 3,472 mg/kg ~ 11,743 mg/kg, respectively. The concentration of As and Zn in sludge-T, Cd in sludge-D, Ni in sludge-H, Zn in sludge-S, and Cd in sludge-Y exceeded the soil contamination standards of Korea. The results from 2 separate kinds of leaching test, the Korea Standard Leaching Test(KSLT) and Toxicity Characteristic Leaching Procedure(TCLP), showed that all the sludges met the Korea groundwater standards. From the XRD and SEM-EDS analysis, the peaks of calcite and quartz were found in the sludges. The sludge also had a high proportion of Fe and O, and the majority of the composition was amorphous iron hydroxide.

Keywords acid mine drainage(AMD), coal mine drainage sludge, arsenic, adsorption, leaching test

광산배수의 적극적 처리시설에서 발생하는 슬러지 특성 평가

김정은^1,2 · 지원현^2,*

¹환경기술정책연구원 (NeLab)
²호서대학교 일반대학원 에너지기후환경융합기술학과

요 약

산성광산배수 처리방법은 적극적 처리방식과 소극적 처리방식이 일반적으로 사용되고 있으며, 이때 발생되는 부산물인 슬러지는 국내에서 약 5천 톤/년으로 발생하고 있다. 본 연구는 적극적 처리방식 중 물리·화학적 처리방식으로 정화 후 발생되는 슬러지의 특성을 조사하여 재활용 가능여부를 검토하기 위함이다. 5개소(D, H, S, T, Y) 수질정화시설의 슬러지의 특성을 물리·화학적 분석을 통해 검토하였다. 그 결과 pH는 pH 5.86 ~ pH 7.89로 측정되었고, 수분함량은 51 % ~ 82 %로 분석되었으며, 입자 크기는 대부분 25 ㎛보다 작은 미립자로 구성되었음을 확인할 수 있었다. ICP-OES를 이용한 슬러지 내 무기물질 분석결과, Al, Fe, Mn의 농도범위는 각각 1,189 mg/kg ~ 129,344 mg/kg, 106,132 mg/kg ~ 338,011 mg/kg, 3,472 mg/kg ~ 11,743 mg/kg로 조사되어 고농도로 존재함을 확인 할 수 있었다. 그 외 무기물질 중 중금속류에 대해서는 T-슬러지는 As와 Zn, D-슬러지는 Cd, H-슬러지는 Ni, S-슬러지는 Zn, Y-슬러지는 Cd의 농도가 토양오염우려기준을 초과하였다.
또한 슬러지의 용출 특성을 알기위해 폐기물 용출시험(KSLT) 및 TCLP 시험을 진행하였다. 슬러지 재활용시 용출되어 지하수에 미치는 영향 확인을 위해 지하수 수질기준(생활용수) 20개 항목에 대하여 수행하였다. 용출시험결과 특정유해물질 16개 항목에서 모두 불검출로 확인되었으며, 일반항목 4개 항목에 대해서는 모두 생활용수 기준치 이내로 만족하였다. XRD, SEM-EDS의 분석결과, 슬러지는 주로 방해석, 석영의 패턴을 보였으며, 높은 Fe, O의 구성비율로 철수산화물이 높은 비중을 차지하는 것으로 보였다. 이를 통해서 비매체접촉형 방식의 재활용의 가능성이 있을 것으로 판단된다.

주요어 산성광산배수, 석탄광산배수슬러지, 비소, 흡착, 용출시험

Article

Research Paper

Econ. Environ. Geol. 2023; 56(4): 409-419

Published online August 30, 2023 https://doi.org/10.9719/EEG.2023.56.4.409

Evaluation of Characteristics of Sludge generated from Active Treatment System of Mine Drainage

Jung-Eun Kim^1,2, Won Hyun Ji^2,*

¹National Environment Lab. (NeLab), Seoul, 02841, Korea
²Department of Energy & Climate Environment Fusion Technology, Graduate shool Hoseo University, Asan, 31499, Korea

Correspondence to:^*greenidea@hoseo.edu

Received: March 13, 2023; Revised: July 13, 2023; Accepted: August 4, 2023

Abstract

Keywords acid mine drainage(AMD), coal mine drainage sludge, arsenic, adsorption, leaching test

광산배수의 적극적 처리시설에서 발생하는 슬러지 특성 평가

김정은^1,2 · 지원현^2,*

¹환경기술정책연구원 (NeLab)
²호서대학교 일반대학원 에너지기후환경융합기술학과

Received: March 13, 2023; Revised: July 13, 2023; Accepted: August 4, 2023

요 약

주요어 산성광산배수, 석탄광산배수슬러지, 비소, 흡착, 용출시험

Fig 1.

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Figure 1.Mine water purification facility process diagram and sludge sampling.

Economic and Environmental Geology 2023; 56: 409-419https://doi.org/10.9719/EEG.2023.56.4.409

Fig 2.

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Figure 2.XRD Images of the studied sludges samples ((a) D-sludge, (b) H-sludge, (c) S-sludge, (d) T-sludge, (e) Y-sludge).

Economic and Environmental Geology 2023; 56: 409-419https://doi.org/10.9719/EEG.2023.56.4.409

Fig 3.

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Figure 3.SEM-EDS analysis of the studied sludge samples ((a) D-sludge, (b) H-sludge, (c) S-sludge, (d) T-sludge, (e) Y-sludge).

Economic and Environmental Geology 2023; 56: 409-419https://doi.org/10.9719/EEG.2023.56.4.409

Table 1

Inorganic material analysis method for sludge.

Inorganic classification	Pretreatment	Anlaysis
Metals (11)	As, Cu, Pb, Zn, Ni, Al, Fe, Mn	Aqua regia digestion	ICP-OES (model 8300, Perkin-Elmer Inc.)
	Cd	Aqua regia digestion	AAS (model ICE-3000, Thermo scientific Inc.)
	Hg	-	Hg analysis (model DMA-80, Milestone Inc.)
	Cr6+	Alkaline digestion	UV/Vis (model Lamda 25, Perkin-Elmer Inc.)
Non-metals (2)	CN	Distillation
Non-metals (2)	F	Distillation

Table 2

Comparison of Leaching test.

	KSLT	TCLP
Max particel size(mm)	5.0	9.5
Leaching Medium	HCl	Acetate buffered solution
pH of leaching Medium	5.8 ~ 6.3	No.1 4.93 ± 0.05 No.2 2.28 ± 0.05
Time of extraction	6 hour	18 hour
Liquid : Solid ratio	10 : 1	20 : 1
Temp.	room temp.	22 ± 3 ℃
Speed	200 rpm	30 ± 2 rpm
Shaking method	rotational shaking	end-over-end fashion
Filter size	1 µm	0.6 ~ 0.8 µm

Table 3

Analysis method and GC/MS analysis conditions for OPPs and VOCs.

Item		Organic compounds(OPPs)
Pretreatment		Liquid extraction
Equipment		GC/MS (model 7890B/5977B, Agilent Inc.)
GC analysis condition	Column	DB-5MS(Cross-linked 5% phenylmethylsilicon, 30 m × 0.25 mm I.D × 0.25 μm, film thickness)
	Carrier gas(flow)	He(1.0 mL/min)
	Split ratio	1/10
	Injector temp.	300℃
	Detector temp.	280℃
	Oven temp.	70℃(4min holding)-300℃(10℃/min)-300℃(5min holding)
Item		VOCs (model 8890A/5977B, Agilent Inc.)
Pretreatment		Purge&Trap
Equipment		GC/MS
Purge &Trap analysis condition	Trap	Vocarb 3000
	Purge gas(flow)	He gas(37 mL/min)
	Desorb gas(flow)	He gas(20 mL/min)
	Purge time	11 min
	Dry purge time	0.5 min
	Bake time	4 min
	Purge Temp.	Ambient
	Desorb Temp.	245 ℃
	Bake Temp.	280 ℃
GC analysis condition	Column	DB-5MS(Cross-linked 5% phenylmethylsilicon, 30 m × 0.25 mm I.D × 0.25 μm, film thickness)
	Carrier gas(flow)	He(1.0 mL/min)
	Split ratio	1/10
	Injector temp.	200℃
	Detector temp.	280℃
	Oven temp.	40℃(2min holding)-125℃(7℃/min)-230℃(12℃/min)-230℃(3 min holding)

Table 4

pH, moisture content and particle size distribution of the studied sludges.

Sludge name	pH	Moisture content(%)	Chemical	Particle size(µm) distribution				(unit:%)
Sludge name	pH	Moisture content(%)	Chemical	> 75	75 ~ 45	45 ~ 38	38 ~ 25	25 >
D	7.15	50.9	Ca(OH)₂	0.24	1.58	0.85	2.35	94.98
H	7.69	52.0	Ca(OH)₂	1.19	1.67	0.52	1.03	95.59
S	5.88	74.5	None Use	0.26	0.49	0.54	0.72	98.00
T	5.86	82.4	PAC	0.85	0.74	0.22	0.59	97.59
Y	7.89	74.6	Ca(OH)₂	0.76	2.14	0.66	0.66	95.77

Table 5

Metal and non-metal concentration of the studied sludges (Unit : mg/kg).

	D	H	S	T	Y	LOQ(1)	Standard⁽²⁾
Item	D	H	S	T	Y	LOQ(1)	Worrisome	Countermeasure
As	15.77	7.32	4.00	31.19	2.15	1.5	25	75
Cd	4.06	3.83	3.91	2.41	5.05	0.10	4	12
Cu	2.9	1.7	3.6	46.6	12.3	1.0	150	450
Pb	3.9	4.1	6.8	10.2	9.7	1.5	200	600
Zn	137.9	297.5	1,157.2	588.7	249.6	1.0	300	900
Ni	10.9	102.1	55.6	73.6	196.4	0.4	100	300
Hg	N.D.⁽³⁾	N.D.⁽³⁾	N.D.⁽³⁾	0.03	0.01	0.01	4	12
Cr⁶⁺	0.55	N.D.⁽³⁾	N.D.⁽³⁾	0.75	N.D.⁽³⁾	0.5	5	15
CN	N.D.⁽³⁾	N.D.⁽³⁾	N.D.⁽³⁾	N.D.⁽³⁾	N.D.⁽³⁾	0.2	2	5
F	67	123	207	1,195	231	10	400	800
Al	1,189	2,743	45,082	129,344	13,980	-	-	-
Fe	123,567	136,267	317,529	106,132	338,011	-	-	-
Mn	3,840	11,743	3,473	5,819	6,326	-	-	-

(1) Limit of quantification.

(2) Criteria for agricultural soil from soil environment conservation act of Korea.

(3) N.D.(Not Detected) : less than LOQ.

Table 6

Contents of elements in soils and the earth's crust (Unit : mg/kg).

Element	Soil		Crust
Element	Average	Range	Average
Al	71,000	10,000 ~ 300,000	82,000
Fe	40,000	2,000 ~ 550,000	41,000
Mn	1,000	20 ~ 10,000	950

Table 7

Leaching test(KSLT and TCLP) result of the studied sludges.

	KSLT⁽¹⁾					TCLP⁽²⁾					LOQ⁽³⁾	Standard⁽⁴⁾
	D	H	S	T	Y	D	H	S	T	Y	LOQ⁽³⁾	Standard⁽⁴⁾
pH	7.9	8.3	7.8	7.7	7.8	-	-	-	-	-	-	5.8~8.5
Total coliform	0	0	0	0	0	0	0	0	0	0	-	5,000
NO₃-N	2.1	0.2	2.0	3.8	0.2	1.0	0.2	1.0	1.8	0.1	0.1	20
Cl	1.4	2.7	8.0	4.6	13.9	47.5	39.7	54.6	114.1	49.6	0.1	250
Cd	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.004	0.01
As	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.05	0.05
CN	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.010.01
Hg	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.0005	0.001
Diazinon	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.0005	0.02
Parathion	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.0005	0.06
Phenol	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.005	0.005
Pb	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.04	0.1
Cr	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.007	0.05
Benzene	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.015
Toluene	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	1
Ethylbenzene	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.45
Xylene	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.75
TCE	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.03
PCE	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.01
1,1,1-TCA⁽⁶⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	N.D.⁽⁵⁾	0.001	0.15

(1) Korea standard leaching test.

(2) Toxicity characteristic leaching procedure.

(3) Limit of quantification.

(4) Criteria for domestic water from groundwater conservation act of Korea.

(5) N.D.(Not Detected) : less than LOQ.

(6) 1,1,1-trichloroethan.

Aug 30, 2024 Vol.57 No.4, pp. 353~471

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Evaluation of Characteristics of Sludge generated from Active Treatment System of Mine Drainage

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광산배수의 적극적 처리시설에서 발생하는 슬러지 특성 평가

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Research Paper

Evaluation of Characteristics of Sludge generated from Active Treatment System of Mine Drainage

Abstract

광산배수의 적극적 처리시설에서 발생하는 슬러지 특성 평가

요 약

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