Beruflich Dokumente
Kultur Dokumente
www.elsevier.com/locate/scitotenv
Abstract
Due to the complex nature of landfill leachates, the leachate treatment plants have difficulty to meet the current Taiwan EPAs
effluent standards. Three typical types of landfills, closed landfill A, mixed landfill B (disposal of MSW with bottom ashes from
MSW incinerators) and direct MSW landfill C, (disposal of MSW only), are investigated in this research in order to have a better
understanding of characteristics of leachates. Factors investigated in this research include landfill age, pH, BOD, COD, TS, DS,
VS, seasons, metals (Pb, Ca, Cd, Hg, Cr, Cu, Fe, K, Mg, Mn, Na, Ni, and Zn), humic substances (humic acid, fulvic acid, and nonhumic substance), aromaticity and toxicity. Results show that the active landfills B and C had the significant higher concentration
of COD, VSS, TS, PtCo, TOC and conductivity. The mixed landfill B had the higher DS, TS, Na, Ca, Mg and conductivity than
that of direct MSW landfill C. Direct MSW landfill C had the highest contents of Fe, Cr, Ni and acute toxicity among these
landfills. A significant degree of variation was encountered and factors which may influence leachate quality were identified and
discussed.
D 2005 Elsevier B.V. All rights reserved.
Keywords: Landfill leachate; Temporal variation; Humic acid; Metal; Toxicity
1. Introduction
The municipal solid waste (MSW) has been a major
environmental problem in Taiwan. The MSW generated
in Taiwan has reached 7 million tons per year. Traditionally, most of the municipal solid wastes (MSW)
were disposed directly into sanitary or simple landfills
in Taiwan. However, in recent years, due to the difficulty of finding new locations for landfills, the MSW
treatment policy of Taiwans EPA was moved toward
incineration of MSW to extend the usage time of landfills. For example, the percentage of incineration of
MSW increased rapidly from 50% to 70% for the past
* Corresponding author. Tel.: +886 4 26318652; fax: +886 4
26525245.
E-mail address: fan@sunrise.hk.edu.tw (H. Fan).
0048-9697/$ - see front matter D 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2005.09.033
26
100
Percentage(%)
80
60
40
20
0
2001
2002
2003
Year
2. Methods
Table 1
Characteristics of landfills
Site
Location
Status
Operation since
Waste compositions
A
B
Urban
Urban
Closed
Active
19881994
1995
1117
10
Rural
Active
1993
12
MSW
MSW (20%60%)
Bottom ashes (40%80%)
MSW
oxygen. Leachates were collected monthly from February 2001 through July 2003. In the laboratory, leachate was filtered through a 0.2 um membrane and stored
at 4 8C in the dark.
The parameters analyzed in this research include pH,
SS (suspended solid), VSS (volatile suspended solids),
TS (total solid), TOC (total organic carbon), COD
(chemical oxygen demand), BOD (biological oxygen
demand), metals (Pb, Ca, Cd, Hg, Cr, Cu, Fe, K, Mg,
Mn, Na, Ni, and Zn), and humic substances (humic
acid, fulvic acid, and non-humic substance).
Humic acid, fulvic acid and non-humic substance
were extracted from landfill leachate through resin
XAD8. The procedure used for separation and purification of humic and fulvic acid was based on the
method described by Christensen et al. (1998) and
Thurman and Malcolm (1981).
The leachates were freeze-dried (Freeze Dryer FD81, Eyela Tokyo Rikakiai Co. LTD) and then analyzed
by Elementar Elemental Analyzer (Vario EL) for contents of carbon, hydrogen, oxygen, nitrogen and sulfur.
Freeze-dried samples of leachate were analyzed from
4000 to 600 cm 1 using a Fourier-Transform Infrared
Spectrometer (Bomem, A8.3, CA).
Acute toxicity of leachate was tested by Microtox
Model 500 Analyzer. The leachate pH was maintained
between 6 and 8 and was filtered through 0.45 Am filter
(Cellulose nitrate, Micro Filtration System, Dublin,
CA) before it was analyzed.
3. Results and discussion
3.1. Waste management in Taiwan
Currently, there are more than 300 landfills (55%
active sanitary landfills, 25% active simple landfills and
19% closed landfills) and 21 major incinerators in
Taiwan (Taiwan EPA, 2003). Most of the landfills are
located in west coast of Taiwan where population is
concentrated. Details of the locations of these landfills
are listed in Fig. 2. In Taiwan, since more than 30% of
water are obtained from groundwater reservoirs, serious
environmental consequences such as soil and groundwater contamination might result from improper handling of these landfill leachates, especially that some of
the landfills are located in the water resource preservation areas in Taiwan. Therefore, it is vital to further
understand the characteristics of landfill leachate for the
proper treatment of the leachate. This study selected
three typical types of landfills located in central Taiwan.
Landfill sites A, B and C are typical cases of closed
landfill, mixed landfill (MSW and bottom ash) and
27
28
Taoyuan
Taipei
Hsinch
Yilanu
Miaoli
Taichung
Changhua
Penghu
Nantou
Yunlin
Hualien
Chiayi
Tainan
Kaohsiung
Taitung
Pingtung
Fig. 2. Location of sanitary landfills (D), simple landfills (5) and major incenirators in (o) Taiwan (Taiwan EPA, 2003).
29
Table 2
Chemical characteristics of leachate at various landfills
Parameters (mg L
1 a
pH
COD
VSS
PtCo color
TOC
SS
BOD
DS
TS
Conductivity
BOD / COD
COD / TOC
a
b
c
Site A
Site B
Site C
Mean
SD
Mean
SD
Mean
SD
Scheffes testb
7.74
689.6
51.1
1781.6
248.8
33.9
49.6
3906.9
3940.9
8571.8
0.06
2.99
0.38
327.1
74.0
631.4
109.3
18.3
29.8
1337.8
1343.2
2883.4
0.07
1.64
7.91
2483.3
165.8
5513.4
867.3
155.9
164.6
9463.6
9619.5
23753.8
0.06
2.82
0.26
1046.7
116.2
1860.9
403.5
71.3
132.0
2638.5
2630.6
7249.3
0.03
1.32
7.86
3038.0
124.9
5452.5
1025.2
192.5
173.8
6594.4
6786.9
19590.0
0.05
3.52
0.28
949.1
60.0
2715.2
770.7
335.6
94.2
2092.5
2111.0
5772.1
0.02
1.15
c
A b B; A b C
A b B; A b C
A b B; A b C
A b B; A b C
AbC
A b B; A b C
AbCbB
AbCbB
AbCbB
5000
Site A
Site B
Site C
COD (mg/L)
4000
3000
2000
1000
0
1/1/01
1/1/02
7/1/02
1/1/03
7/1/03
1/1/04
Date
500
400
SS (mg/L)
7/1/01
Site A
Site B
Site C
300
200
100
0
1/1/01
7/1/01
1/1/02
7/1/02
1/1/03
7/1/03
1/1/04
Date
speaking, it is more suitable to use a biological treatment process when BOD / COD N 0.5 or COD /
TOC N 2.8 (Chain, 1977). The average ratios of
BOD / COD in landfills A, B, and C were 0.08,
0.06, and 0.05, respectively. This lower BOD / COD
value indicated that these landfills had reached a stable
status and probably were not suitable for biological
treatment processes which were the most commonly
used treatment methods in Taiwan. As a result, this
might be the reason that most of the landfills in
Taiwan have difficulty to fulfill the COD effluent
standards of 200 mg L 1. Consequently, it might be
necessary to include additional physical/chemical processes to achieve the desired removal efficiency. However, there were no statistically significant differences
of BOD / COD ratios among these sites.
The COD / TOC ratio of sites A, B and C were
about 2.99, 2.82, and 3.52, respectively. Although the
average value of site C was larger than both sites A
and B, the difference did not reach statistical significance level.
3.2.2. Correlations
Pearson correlation coefficients among the analyzed
chemicals are shown in Table 4. The landfill age was
negatively correlated with pH, COD, SS, VSS, TS,
color, TOC, BOD, conductivity, and SS. pH was correlative with landfill age, COD, TS, color, TOC, conductivity, and DS. SS was positively correlated with
COD, VSS, TS, color, TOC, conductivity and DS. The
COD content of the leachate samples was positively
correlated with pH, SS, VSS, TS, color, TOC, BOD,
conductivity, and DS. It was negatively correlated with
30
Table 3
Chemical properties of landfill leachatesa
1 a
Parameter (mg L
Age
pH
Conductivity
Salinity
COD
BOD5
Total solids
Suspended solid
Volatile solids
Fixed solids
Kjeldahl N
Ammoniacal N
Nitrate/nitrite N
Color (unit PtCo)
TOC
Total P
K
Na
Ca
Mg
Cd
Cr
Cu
Fe
Mn
Ni
Pb
Zn
a
b
c
Site A
Site B
Site C
JB, HKb
GDB, HKb
Kuwaitc
1016
7.038.50
3.5814.16
3201340
1297
18306120
4100
8370
40.1150
5802680
90439
0.293.75
198778
3201342
47.2137.5
27.8103
b0.15
0.010.18
0.014.38
0.265.44
0.185.27
0.040.14
b0.02
0.041.61
9
7.308.40
7.0540.68
4004340
26492
178014970
38332
51526
28303
2872
9.520.9
16209480
4471637
2.4315.9
1841799
2973524
67.2133.7
23163
b0.01
0.120.52
0.0011.48
0.2615.3
0.020.74
0.010.26
0.00050.09
0.0030.56
11
6.828.37
5.0029.60
8404210
16312
317010490
601750
72264
26.4219
180201
2.9626.7
158013875
3273992
4.815.14
3122243
4313142
15.961
15.7157
b0.01
0.041.26
0.020.9
0.3928
0.020.75
0.010.28
0.020.18
0.030.66
3.5
7.28.0
8.512.0
7.215.1
4891670
26805580
6851580
17704010
6751840
5941610
0.060.31
2.7214.1
270632
4841190
3563
b0.01
0.030.15
b0.05
1.143.25
0.050.24
0.070.18
0.030.12
0.242.55
11
7.28.4
2.511.8
4.09.5
1471590
9204500
4981580
3982923
1371060
65883
21.6179
0.363.78
78416
132743
926
b0.02
0.020.23
0.010.13
1.265.00
0.051.30
0.040.17
b0.10
0.130.39
6.98.2
5.16.9
5.78.1
5.6122 254.12300
70290
5.2268
233410
100270
00.2
00.1
0.3554.1
4.21185
879
00.2
00.46
0.04.8
18.867
5000
COD (mg/L)
4000
3000
2000
Site A
Site B
Site C
1000
100
200
300
400
Germanyc
USAc
500
BOD (mg/L)
600
acteristics on site, since some of the chemical parameters can be obtained easier than others.
3.2.3. Metals
Thirteen metals (Na, K, Ca, Mg, Fe, Cr, Ni, Mn, Pb,
Cd, Hg, Cu and Zn) in leachate were analyzed in this
research and listed in Table 5. In general, the concentrations of Na, K, Ca and Mg were the highest among these
13 metals in leachates. For example, the average sodium
concentrations of landfills A, B and C were about 783,
2028 and 1261 mg L 1, respectively. The closed landfill
A had the lowest concentration of Na, K, Fe, Cr and Ni
and the highest Mn contents among these three sites.
The mixed landfill B had the highest Na and Mg contents among these three sites which might be due to the
contents of bottom ash. Landfill C had the highest Fe
and Cr and the lowest Ca contents. As mentioned above,
it seemed that mixed landfill site B had the higher
contents of Na, Ca and Mg and the lower Fe and Cr
than active municipal landfill C had. Although there is
no violation to Taiwans effluent standards found in
31
Table 4
Pearson correlation coefficients of chemical contents
Landfill age
Landfill age
pH
COD
SS
VSS
TS
Color
TOC
BOD
Conductivity
DS
pH
1.00
0.19
1.00
COD
SS
0.57*
0.44*
1.00
0.28*
0.02
0.34*
1.00
VSS
0.43*
0.10
0.36*
0.66*
1.00
TS
Color
0.49*
0.42*
0.72*
0.29*
0.42*
1.00
0.57*
0.31*
0.79*
0.59*
0.46*
0.68*
1.00
TOC
BOD
0.49*
0.15
0.64*
0.36*
0.39*
0.43*
0.55*
1.00
Conductivity
0.44*
0.27**
0.76*
0.25
0.07
0.62*
0.58*
0.54*
1.00
0.60*
0.48*
0.78*
0.25**
0.39*
0.86*
0.71*
0.58*
0.64*
1.00
DS
0.48*
0.42*
0.71*
0.24**
0.41*
1.00
0.65*
0.43*
0.61*
0.86*
1.00
Table 5
Metal concentrations of leachates at various landfills
Parameters (mg L
Na
K
Ca
Mg
Fe
Cr
Ni
Mn
Pb
Cd
Hg
Cu
Zn
a
b
Site A
Site B
Scheffes testb
Site C
Mean
SDa
Mean
SD
Mean
SD
782.65
455.42
98.71
49.76
1.74
0.07
0.09
1.46
0.01
0.02
0.01
0.26
0.36
318.29
174.98
48.25
19.18
1.30
0.04
0.03
1.25
0.01
0.05
0.01
0.86
0.40
2027.89
1158.93
87.84
77.39
5.15
0.28
0.16
0.40
0.02
b0.01
0.02
0.23
0.20
686.90
362.78
18.28
26.03
3.28
0.11
0.06
0.18
0.02
0.02
0.34
0.14
1261.28
924.24
56.66
53.56
8.24
0.73
0.18
0.36
0.03
b0.01
0.03
0.11
0.22
603.74
446.60
27.25
29.24
5.86
0.31
0.06
0.16
0.04
0.05
0.20
0.15
Standard deviation.
Significance level (a = 0.05).
AbCbB
A b B; A b C
C b A; C b B
A b B; C b B
AbBbC
AbBbC
A b B; A b C
B b A; C b A
32
Site A
Site B
Site C
4000
COD (mg/L)
3000
2000
1000
10
12
14
16
600
500
Site A
BOD (mg/L)
Site B
Site C
400
300
200
100
0
4
10
12
14
16
500
2
Site A
Site C
300
Cu (mg/l)
SS (mg/L)
Site A
Site B
Site C
Site B
400
200
100
0
4
10
12
14
16
Age (yr)
10
12
14
16
12
14
16
Age (Yr)
2
Site A
Site B
Site C
Zn (mg/l)
10
Age (Yr)
Parameter
Mean
(mg L
HA
FA
NHS
B
%
1
94
100
142
28
30
42
Mean
(mg L
C
%
1
72
202
390
11
30
59
Mean
(mg L
101
123
257
%
1
)
21
26
53
33
Table 7
Elemental composition (normalized to 100% of organic components) and ratios of leachate (molar ratio)
Sample
C%
H%
O%
N%
S%
H / Ca
O / Ca
N / Ca
Site A
Site B
Site C
Fisher sci.b
Landfill Gc
Landfill Pc
Landfill Nc
Aquatice
Terrestriale
NLFg
SELAg
EOg
11.44
24.33
28.47
46.09
56.2
57.1
56.1
5360
5462
60.48
61.73
63.09
4.15
4.57
4.21
5.55
8.8
7
7.2
3.75.1
2.95.8
6.97
7.44
7.35
65.94
59.15
59.88
46.13
26.7
30.2
29.3
33.440.8
29.536.8
28.11
25.89
26.27
15.3
9.96
6.05
0.78
8.3
5.7
7.4
2.02.1
1.64.8
2.32
3.71
1.79
3.17
1.99
1.38
1.45
NDd
ND
ND
f
4.35
2.25
1.77
1.44
1.54
1.48
1.88
0.741.15
0.561.29
1.37
1.44
1.39
4.32
1.82
1.58
0.75
0.39
0.4
0.36
0.420.58
0.360.51
0.35
0.31
0.31
1.15
0.35
0.18
0.01
0.11
0.09
0.13
0.0290.034
0.0220.076
0.03
0.05
0.02
a
b
c
d
e
f
g
Molar ratio.
Humic acid obtains from Fisher Scientific Co.
Landfills in Korea(Kang et al., 2002).
ND= Not detected.
Typical values of Aquatic and Terrestrial humic acids.
Data not available.
Landfills in Oklahoma, USA; NSF, Norman Landfill; SELA, Southeast Landfill Authority; EO, East Oak (Nanny and Ratasuk, 2002).
34
Table 8
Absorption coefficients of leachates
Parameter
Site A
Site B
Site C
1.63
0.11
0.01
11
2.27
1.18
0.21
6
2.26
1.41
0.28
5
Site A
Site B
Site C
Humic acids (Fisher Sci.)
10
Kulelka Munk
1000
2000
3000
4000
35
Table 9
Seasonal effect of leachates
Site
Parameter
Season
Mean (mg L
pH
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
Spring
Summer
Fall
Winter
7.8
7.4
7.8
8.0
764
444
592
956
4884
2664
3194
4856
9285
5935
8564
10776
4848
2634
3161
4820
136
148
242
128
82
135
331
138
11843
7627
8510
10434
11707
7479
8268
10306
COD
TS
Conductivity
DS
SS
VSS
TS
DS
SD.
Min
Max
Scheffes testb
0.4
0.3
0.2
0.4
369
247
96
258
1327
781
425
657
3264
1790
1615
1973
1315
786
423
649
49
78
81
30
19
83
115
51
1838
3070
1067
828
1833
3047
1139
831
7.1
7.0
7.6
7.6
310
160
510
509
2480
1830
2600
3960
5670
3580
5800
8220
2463
1791
2578
3946
72
38
153
68
58
52
228
80
9710
1780
7610
9370
9608
1742
7361
9226
8.2
7.8
8.1
8.5
1340
900
720
1258
6120
4030
3620
5700
14160
9390
9600
13030
6100
4026
3589
5650
190
283
332
160
104
261
526
224
14970
11180
9860
11975
14899
11055
9693
11855
Winter N Summer
Winter N Summer
Spring N Summer
Spring N Summer
36
Table 10
Toxicity of leachates at various landfills
Landfill
Range (EC50)a
Classb
A
B
C
N100
N100
3.019
Non-toxic
Non-toxic
Confirmed toxicitySevere toxic
3.7. Toxicity
Chemical analysis of environmental samples provides a measurement for the total concentration of
potentially harmful substance. However, chemical techniques may also be unable to detect certain bunknownQ
compounds. Assessment of potential environmental
risk of contaminated groundwater cannot be evaluated
by chemical means alone (Boyd et al., 1997). Therefore, microtox acute tests were applied in this research
to evaluate the toxicity of the leachate. Microtox acute
tests had the advantages of simple, fast and sensitive.
The test used the luminescent bacteria (Vibrio fischeri)
as a toxicity indicator. The metabolic process and light
production of bacteria were both intrinsically linked
respiration via the use of NADH and oxygen. Therefore, the end product of the luminescent bacteria also
included an appreciable quantity of light. Anything that
will effect the respiration of the luminescent bacterium
would cause a corresponding response in light level.
The sample was toxic if it caused a decrement in light
compared to the control. Therefore, the light could be
measured to determine changes in light level caused by
a toxic response (Boyd et al., 1997).
The results of microtox acute tests are shown in
Table 10. The EC50 (15 min) for landfills A, B and C
were 0.5, N 100, and 0.1, respectively. EC50 (15 min)
indicated the toxicant concentration caused the lamination of bacteria to reduce 50% at a 15-min reaction
time. In general, the EC 50 can be classified as follows:
(1) EC50 N 100, non-toxic. (2) 100 N EC50 N 40, potential
toxicity (3) 40 N EC50 N 10, confirmed toxicity, and (4)
EC50 b 9 severe toxicity (Marsalek et al., 1999). As in
Table 10, the toxicity of sites A and B was not significant, however the toxicity of site C was highly toxic.
This result might indicate that the mixed landfilling was
helpful on reducing the toxicity of leachate. In Taiwan,
there are more than 75 simple landfills without proper
lining systems. Most of these simple landfills were
located in remote mountain areas and some of them
were located in water resource preservation area. There-
37