Co-Treatment of Landfill Leachate in WWTPs
Co-Treatment of Landfill Leachate in WWTPs
Research article
a r t i c l e i n f o a b s t r a c t
Article history: Landfill leachate is the result of water percolating through waste deposits that have undergone aerobic
Received 14 January 2016 and anaerobic microbial decomposition. In recent years, increasingly stringent wastewater discharge
Received in revised form requirements have raised questions regarding the efficacy of co-treatment of leachate in municipal
7 September 2016
wastewater treatment plants (WWTPs). This study aimed to (1) examine the co-treatment of leachate
Accepted 24 November 2016
with a 5-day biochemical oxygen demand (BOD5): chemical oxygen demand (COD) ratio less than or
slightly greater than 0.26 (intermediate age leachate) in municipal WWTPs (2) quantify the maximum
hydraulic and mass (expressed as mass nitrogen or COD) loading of landfill leachate (as a percentage of
Keywords:
Landfill leachate co-treatment
the total influent loading rate) above which the performance of a WWTP may be inhibited, and (3)
Ammonium quantify the impact of a range of hydraulic loading rates (HLRs) of young and intermediate age leachate,
Activated sludge loaded on a volumetric basis at 0 (study control), 2, 4 and 10% (volume landfill leachate influent as a
Nitrification inhibition percentage of influent municipal wastewater), on the effluent ammonium concentrations. The leachate
Municipal solid waste loading regimes examined were found to be appropriate for effective treatment of intermediate age
landfill leachate in the WWTPs examined, but co-treatment may not be suitable in WWTPs with low
ammonium-nitrogen (NH4-N) and total nitrogen (TN) emission limit values (ELVs). In addition, inter-
mediate leachate, loaded at volumetric rates of up to 4% or 50% of total WWTP NH4-N loading, did not
significantly inhibit the nitrification processes, while young leachate, loaded at volumetric rates greater
of than 2% (equivalent to 90% of total WWTP NH4-N loading), resulted in a significant decrease in
nitrification. The results show that current hydraulic loading-based acceptance criteria recommendations
should be considered in the context of leachate NH4-N composition. The results also indicate that co-
treatment of old leachate in municipal WWTPs may represent the most sustainable solution for
ongoing leachate treatment in the cases examined.
© 2016 Elsevier Ltd. All rights reserved.
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0301-4797/© 2016 Elsevier Ltd. All rights reserved.
R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72 65
biodegradable municipal waste sent to a landfill, and (3) places COD) loading of landfill leachate (as a percentage of the total
responsibility on landfill owners to budget for the aftercare of a influent loading rate) above which the performance of a WWTP
landfill site for a minimum of 30 years after operation has ceased. may be inhibited and (2) quantifies the impact of a range of volu-
Prior to the implementation of this Directive, landfilling across the metric loading rates (VLRs) of young and intermediate age leachate,
EU was unregulated and poorly planned (EC, 2007). The Directive loaded on a volumetric basis at 0, 2, 4 and 10% (expressed as volume
has resulted in dramatic improvements in the manner in which landfill leachate treated in the WWTP as a percentage of the total
landfills, and specifically landfill leachate, is managed (McCarthy influent wastewater to the WWTP), on NH4-N removal. The study is
et al., 2010; Brennan et al., 2015). While there has been a decline thus focused on the identifying the optimum leachate loading
in landfilling in recent years, leachate generation is a legacy prob- strategy adoptable which will minimize the adverse effects of
lem, and the treatment of leachate is the major management issue landfill leachate presence in the WWTP and ensure effective
facing landfill operators (Zhang et al., 2009; Brennan et al., 2015). treatment of wastewater and leachate.
Many landfills are not located close to suitable receiving waters
(Knox et al., 2015). Therefore, the most sustainable option may be to 2. Materials and methods
transfer leachate to wastewater treatment plants (WWTPs) for final
treatment. 2.1. Study sites
Leachate contains high levels of 5-day biochemical oxygen de-
mand (BOD5), chemical oxygen demand (COD), ammonium- Three activated sludge WWTPs, two of which were represen-
nitrogen (NH4-N), chloride (Cl), sodium (Na), potassium (K), ni- tative of WWTPs co-treating leachate in Ireland and another which
trogen (N), boron (B), solvents, phenols, hardness and metals, had not received landfill leachate in over one year and hereafter
including iron (Fe), manganese (Mn), zinc (Zn), copper (Cu), cobalt referred to as Sites 1, 2 and 3, were selected for use in this study.
(Co), chromium (Cr), nickel (Ni), cadmium (Cd) and lead (Pb) (Tatsi Landfill leachate (LL) accepted at Site 1 and 2 (intermediate) and a
and Zouboulis, 2002; Chofqi et al., 2004; Ag dag and Sponza, 2005; young landfill leachate from another landfill (young) were identi-
Marzougui and Ben Mammou, 2006). Young leachate (generated in fied and hereafter referred to as LL 1, 2 and 3.
operational landfills or landfills closed for less than five years
(Renou et al., 2008)) is highly biodegradable and exhibits COD and 2.2. WWTP monitoring
NH4-N concentrations of up to 80,000 and 3100 mg L1, respec-
tively, and BOD5:COD ratios of up to 0.7 (Stegmann et al., 2005). As a Sites 1 and 2 were selected and monitored to determine the
result, biological treatment methods are reasonably efficient in the impact of leachate loading regime on WWTP performance. Their
removal of COD, NH4 and metals (Kurniawan et al., 2006). operational information is given in Table 1. Both WWTPs received
Conversely, older (stabilised) leachate is less biodegradable and leachate (Table 2) at average VLRs, of 1.2 and 2.3%. Leachate loading
contains methanogenic leachate with BOD5:COD ratios < 0.2 regimes examined during the study were: (1) drip-feed (2) no-
(Stegmann et al., 2005), and therefore is not as efficiently treated leachate addition and (3) shock loading (i.e. relatively large
using biological methods. In the current paper, landfills are defined leachate volumes added to the WWTP in a brief pulse). Drip-feed
as young (operational/closed less than five years), intermediate and no-leachate scenarios were examined at Site 1, whereas
(closed more than five year but less than 10), and old (closed more shock loading was examined at both Site 1 and 2 (Table 3).
than ten years) (after Renou et al., 2008). Refrigerated automatic wastewater samplers (Aqua Cell, UK) were
To date, there has been limited work regarding the impacts of used to collect grab samples at eight-hour intervals at the head of
co-treatment of landfill leachate and municipal wastewater in the works prior to primary settlement and at effluent discharge
WWTPs (Renou et al., 2008), and studies have been largely limited points (effluent wastewater samples) of Sites 1 and 2. Influent and
to laboratory-scale batch experiments (Diamadopoulos et al., 1997; effluent flows were recorded using on-site flow recording equip-
Çeçen and Aktaş, 2004; Capodici et al., 2014; Wu et al., 2015; Mojiri ment. For operational reasons, it was not practical to monitor each
et al., 2014). These studies have generally concluded that WWTP loading regime for a time period longer than the sludge age of the
removal efficiency is not adversely affected, provided the total WWTP, and this must be taken into account when interpreting
hydraulic loading of leachate does not exceed 10% of the total differences between leachate loading regimes.
municipal wastewater entering the WWTP. However, at these
volumetric loading rates effluent NH4-N and total nitrogen (TN) 2.3. Analysis of wastewater and landfill leachate
may be significantly impacted due to their relatively high concen-
trations in landfill leachate (Diamadopoulos et al., 1997; Ye et al., Samples were analysed for BOD5, COD, CODs, filtered total ni-
2014; Ferraz et al., 2014). The lack of recent studies examining trogen (TNf), filtered total inorganic carbon (TICf), filtered total
co-treatment of leachate in operational municipal WWTPs is a organic carbon (TOCf), ortho-phosphorus (PO4-P), nitrate-nitrogen
concern for WWTP managers, as wastewater effluent is subject to (NO3-N), nitrite-nitrogen (NO2-N), alkalinity, sulphate, chloride,
increasingly stringent legislation in the EU. There is a concern that NH4-N and suspended solids (SS). All analyses were conducted in
recommendations based on laboratory studies and, not site-specific accordance with the standards method for the examination of
data, may result in failures to achieve compliance. water and wastewater (APHA, 2012). Conductivity and pH were
Studies have demonstrated that co-treatment of young leachate determined using a SAC950 sample changer and a Titralab 870.
with municipal wastewater does not adversely affect WWTP per- Total metal concentrations for Cu, Cd, Cr, As, Pb, Hg, and Ni were
formance (Diamadopoulos et al., 1997; Kalka, 2012; Ye et al., 2014); determined by Inductively Coupled Plasma Mass Spectrometry
however, the effect of old landfill leachate (BOD5:COD < 0.01; (ICP-MS) (Agilent 7500a Technologies Inc. USA) following micro-
Renou et al., 2008) has not been widely examined with the wave digestion (CEM Discover SPD Microwave Digester) using
exception of Del Borghi et al. (2003), who concluded that old Trace Metal Grade Nitric Acid (Fisher, UK).
leachate should mixed with young leachate before treatment. The
current study (1) examines the co-treatment of leachate with a 2.4. Nitrification inhibition batch experiments
BOD5: COD ratio less than or slightly greater than 0.26 (interme-
diate age leachate) in municipal WWTPs and attempts to quantify Laboratory batch experiments, conducted to supplement the
the maximum hydraulic and mass (expressed as mass nitrogen or results of the WWTP study, examined the impact of various landfill
66 R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72
Table 1
Study site wastewater treatment plant operational information (Annual data 2013).
WWTP: wastewater treatment plant; P.E.: population equivalent; LL1 and 2: landfill leachate from sites 1, and 2 respectively.
Table 2
Study site landfill leachate characterisation.
BOD5: 5-day biochemical oxygen demand; COD chemical oxygen demand; Sig.: significance level; letters denote leachate concentrations which are not significantly different
to each other when comparing between leachates.
Table 3
Wastewater treatment plant influent and effluent daily loads (kg d1) and percentage removal efficiency at each study site WWTP.
WWTP Reg. Average volume m3d1 BOD5 (kgd1) COD (kgd1) TICf (kgd1) TOCf (kgd1) TNf (kgd1) NH4-N (kgd1) COD:TNf
Inf Eff % Inf Eff % Inf Eff % Inf Eff % Inf Eff % Inf Eff %
WWTP: Wastewater treatment plant; Reg.: landfill leachate loading regime; D: drip feed; N: No leachate; S: shock load; L: low loading; H: high loading; BOD: biochemical
oxygen demand; COD: chemical oxygen demand; TICf: total filtered inorganic carbon; TOCf: total filtered organic carbon; TN: total nitrogen; NH4-N: ammonium nitrogen.
Table 4
Metal concentrations in WWTP influent, effluent and landfill leachate accepted at each study site WWTP.
Site Influent (before leachate added to aeration 0.3a (0) 1.7a (1.09) 0.06a(0) 6.3a (2.9) 1.06a (0.13) 5.7a (4.6) 0.01a (0.01)
1 tank)
Effluent 0.3a (0) 1.1a (0.51) 0.11a(0.17) 5.6a (1.47) 1 (0)a 4.1a (1.02) 0.01a (0)
Leachate at point of entry to sewer 0.6a (0) 3.17 (1) 0.12a(0) 57 (5) 33 (1) 93 (23) 0.03 (0)
Site Influent (including leachate which was in 0.3a (0) 4.41 (2.15) 0.08a (0.03) 5.7 (1.85) 1.55a (1.14) 6.2a (5.7) 0.12 (0.05)
2 sewer)
Effluent 0.3a (0) 0.91a (0.03) 0.06a(0) 4.57 (0.29) 1.01a (0.03) 4.1a (2.8) 0.04a (0.03)
Leachate at point of entry to WWTP 0.23a (0.1) 2.25a (1.85) 0.06(0.03) 31 (16.5) 22 (10.03) 63 (29) 0.02a (0.01)
Nitrification inhibiting value** 1 0.5 0.1 0.5 0.05e0.1 1 0.1e0.35
Standard deviation in parenthesis; p < 0.05: significance level; letters denote leachate concentrations which are not significantly different to each other when comparing
between leachates.*metals on priority substances list (EC, 2008a); **Hanmer et al. (1983).
68 R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72
Fig. 1. Bar chart showing leachate daily and instantaneous volumetric loading rates (VLR and VLRi), BOD5, COD, TN and NH4-N mass loads as a percentage of WWTP influent mass.
Units: %; D: drip feed; S: shock load; L: low loading; H: high loading; BOD: biochemical oxygen demand; COD: chemical oxygen demand; TN total nitrogen; NH4-N: ammonium
nitrogen; VLR: volumetric loading rate. WWTP: wastewater treatment plant; *denotes VLRi which in the instantaneous volumetric rate determined by expressing the volume of
leachate treated as a percentage of the volume of effluent treated during the time the leachate was discharged to the WWTP/sewer from the tanker or on-site storage tank.
Fig. 2. Boxplot showing wastewater treatment plant effluent concentrations. Units: mg L1; D: drip feed; N: No leachate; S: shock load; L: low loading; H: high loading; BOD:
biochemical oxygen demand; COD: chemical oxygen demand; NH4-N: ammonium nitrogen; nitrate (NO3-N).
the final discharge to receiving waters is within the maximum set by the relevant authority. Wastewater treatment plant ELVs
permissible effluent concentrations or emission limit values (ELVs) depend on the size and water quality status of the waterbody
R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72 69
Table 5
Beaker experiment initial leachate and MMLS characterisation.
Activated sludge from Site 1 3664 4.76 62.5 0.63 3265 2585
Activated sludge from Site 3 3232 5.93 34 6.94 1475 1075
Leachate from landfill 1 (LL1) 1236 134 700 1.034 135 60
Leachate from landfill 3 (LL3) 11,373 2800 7820 1.1 360 195
Units: mg L1; WW: Wastewater; LL: landfill leachate; COD: chemical oxygen demand; NH4-N: ammonium nitrogen; TON: total oxidized nitrogen (NO3-N þ NO2-N); MLSS:
mixed liquor suspended solids; VSS: volatile suspended solids.
Fig. 3. Nitrification inhibition experiment ammonium (NH4-N), nitrate (NO3-N) and alkalinity trends at 0, 2, 4 and 10% leachate loading rates. Units: mg L1; Error bars denote
standard deviation; WW: wastewater; LL: landfill leachate; NH4-N: ammonium nitrogen; NO3-N: Nitrate nitrogen.
receiving the treated effluent and are unique to each WWTP. loading regimes. At Site 2 final discharge NO3-N concentrations
Effluent concentrations were lower at Site 1 with an ELV of 1 mg were greater during the low leachate loading period, possibly
NH4-N L1 compared to Site 2 with an ELV of 10 mg NH4-N L1; indicating the inhibition of ammonium oxidizing bacteria during
however, concentrations exceeded ELVs for Site 1 for all loading the high leachate loading period.
regimes examined and not Site 2. There was a correlation between When treating wastewater, it is usually stated that the ratio of
WWTP VLRi and effluent NH4-N for Site 2 (R2 ¼ 0.68; p < 0.05) but COD:N: in the wastewater to be treated should be approximately
not for Site 1. These results demonstrate the challenges faced in 20:1 for aerobic treatment. At Site 1 COD:TNf varied between 10
treating landfill leachate in WWTPs with low ELVs. Future re- and 33 for the drip-feed treatment, 5e32 for shock and 16e19 for
ductions to ELVs pose a significant threat to continued co- no leachate treatment. Clearly leachate addition altered with the
treatment of landfill leachate worldwide. C:N balance within the WWTP particularly during the shock
Leachate-derived NH4-N accounted for 18% and 32% of TN loading period. At Site 2, however, there was not as significant
treated at Sites 1 and 2, respectively. Therefore, leachate co- variation between treatments.
treatment has the potential to have an adverse impact on aera- The batch experiments were in agreement with site monitoring
tion requirements, nitrification efficiency and WWTP operating results and demonstrate that intermediate age leachate loaded at
cost, as demonstrated at Site 2. Observed final discharge NO3-N volumetric ratios up to 4% or approximately 50% of total WWTP
concentrations indicate that nitrification occurred at Site 1 (Fig. 2), NH4-N loading do not significantly inhibit nitrification processes
although there were no significant differences between loading (Fig. 4). These findings have significant implications for WWTPs
regimes. Nitrate-N concentrations in the final discharge were accepting young leachate similar to LL3 with high NH4-N concen-
highest during the drip-feed phase, indicating that leachate trations, as co-treatment at recommended VLRs may inhibit nitri-
improved plant performance compared to no-leachate and shock fication processes, as demonstrated in the current study. When
70 R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72
Table 6
Wastewater and leachate chemical oxygen demand (COD), pH, dissolved oxygen (DO), free ammonia and COD: ammonium ratio for all beaker experiments conducted.
48 hr 0.125 hr 48 hr 0.125 hr 48 hr
Site 1 w/w þ LL1 0% 3750 (1490) 6.3 (0) 5.3 (0) 9 (0.4) 9.9 (0.2) 0.00 424:1
2% 3250 (1070) 6.5 (0.2) 5.5 (0) 9.1 (0.2) 10 (0.6) 0.01 287:1
4% 2660 (2090) 6.8 (0.1) 5.3 (0.1) 8.6 (0.2) 9.8 (0.2) 0.02 161:1
10% 4630 (695) 7.4 (0) 5.3 (0.1) 7.5 (1.5) 9.7 (0.2) 0.04 658:1
Site 1 w/w þ LL3 0% 2020 (2290) 6 (0.2) 5.6 (0.2) 8.3 (1.2) 11.5 (0.4) 0.00 362:1
2% 2430 (1780) 7.1 (0.2) 5.5 (0.7) 8.6 (1.3) 11.2 (0.3) 0.15 41:1
4% 2570 (977) 7.6 (0.2) 6.8 (0.7) 9.5 (0.2) 10.4 (0.4) 0.91 23:1
10% 2580 (1960) 8.1 (0.1) 9.4 (0.1) 9 (1) 10.2 (1.5) 8.27 8:1
Site 3 w/w þ LL1 0% 3910 (1340) 8 (0.2) 8 (0) 7.9 (0.1) 2.5 (0.3) 0.09 876:1
2% 4000 (2320) 7.8 (0.2) 8 (0.1) 8.1 (0.2) 1.9 (0) 0.15 335:1
4% 3850 (2160) 7.5 (0.1) 8 (0.1) 6 (1) 1.6 (0.3) 0.06 421:1
10% 5910 (411) 7.3 (0.3) 7.8 (0.2) 9.5 (15.2) 1.5 (0.1) 0.07 342:1
Site 3 w/w þ LL3 0% 5040 (2010) 7 (0.1) 6.8 (0.2) 4.2 (0.7) 8.3 (1.7) 0.02 676:1
2% 4610 (994) 7.6 (0.1) 6.7 (0.3) 3 (2) 8.5 (0.8) 0.48 77:1
4% 2360 (1560) 7.9 (0.2) 6.9 (0.7) 4.1 (0.6) 8.1 (1.7) 1.71 22:1
10% 6360 (928) 8.4 (0.2) 8.8 (0.1) 5.8 (2.2) 8.9 (0.6) 15.9 18:1
Fig. 4. Bar chart showing leachate volumetric loading rate (VLR), COD and NH4-N mass loads as a percentage of WWTP influent mass for laboratory batch experiments. Units: %;
COD: chemical oxygen demand; NH4-N: ammonium nitrogen; WWTP: wastewater treatment plant.
using a volumetric loading rate of >4% (which corresponded to an MLSS in beaker experiments increased initial NH4-N concentra-
initial concentration of approximately over 350 mg NH4-N L1 tions compared to the control. Addition of leachate to wastewater
when LL3 was added to wastewater from Sites 1 and 3) nitrification MLSS was observed to increase initial alkalinity concentrations
inhibition occurred. It was not possible to determine an appropriate (t ¼ 0.125 h) compared to the control, but these increases were not
NH4-N based leachate loading recommendation. However, a statistically significant. Addition of intermediate age leachate had
loading rate of 2% (approximately 90% of total WWTP NH4-N load) no impact on final alkalinity (t ¼ 48 h), but young leachate added at
may be more appropriate for the young leachate. This could vary all rates examined, significantly increased alkalinity compared to
between leachates depending on NH4-N concentration and pres- the control (p < 0.05). Alkalinity was observed to decrease steadily
ence of other inhibitory compounds which were not observed in in all beakers, reaching a plateau at approximately 6 h. This in-
levels likely to inhibit nitrification in this study (Table 4). The re- dicates most of the nitrification occurred within the first 6 h of the
sults of the beaker experiment were generally in agreement with batch experiment.
the results from the site monitoring conducted during the current Effluent NO3-N concentrations indicate that nitrification
study (Fig. 2) and previous studies (Kalka, 2012; Ye et al., 2014). occurred in all beakers (Fig. 3) with the exception of leachate from
These results demonstrate that hydraulic loading-based acceptance Site 1 co-treated with wastewater from Site 1 and young leachate
criteria recommendations are not appropriate when co-treating co-treated with wastewater from Site 1 and 3 when added at 10%
leachate with municipal wastewater, unless leachate NH4-N (p < 0.05). It is likely that insufficient alkalinity in the wastewater
composition is considered and known in advance of acceptance. collected from Site 1 caused nitrification inhibition, as there was
Addition of intermediate and young leachate to wastewater insufficient alkalinity present to ensure that complete nitrification
R.B. Brennan et al. / Journal of Environmental Management 188 (2017) 64e72 71
occurred (Tchobanoglous et al., 2004). There are a number of and all stakeholders for facilitating sample collection and providing
possible reasons for the observed inhibition in young leachate (10%) data for the study.
treatments for both wastewaters. The most likely of these include
leachate toxicity, elevated free ammonia concentrations and
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