Recent Developments in Landfill Leachate Treatment Aerobic Granularreactor and

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Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Contents lists available at ScienceDirect

Environmental Nanotechnology, Monitoring & Management


journal homepage: www.elsevier.com/locate/enmm

Recent developments in landfill leachate treatment: Aerobic granular


reactor and its future prospects
Vikalp Saxena a, Susant Kumar Padhi a, *, Pritam Kumar Dikshit b, Lopa Pattanaik c
a
Department of Civil Engineering, Shiv Nadar University, Greater Noida, Uttar Pradesh 201314, India
b
Department of Biotechnology, Koneru Lakshmaiah Education Foundation, Vaddeswaram, Guntur 522502, Andhra Pradesh, India
c
Department of Biotechnology and Bioinformatics, NIIT University, Neemrana, Rajasthan 301705, India

A R T I C L E I N F O A B S T R A C T

Keywords: Landfill leachate comprises highly toxic and hazardous compounds posing adverse health effects to the
Landfill leachate ecosystem and human populations. These leachates must be subjected to suitable treatment before discharging to
Biological process the environment. However, the higher operational cost and presence of recalcitrant matter in the leachate make
Aerobic granular reactor
the conventional physico-chemical processes incompetent for treatment. Recent advancements in biological
Integrated process
processes over physico-chemical processes result in the development of aerobic granular reactor (AGR) for
treating landfill leachate. Small footprint, less energy demand, high microbial activity, long-term operational
stability with better removal of organic pollutants, and resistance to high shock load make AGR a promising
technique for treating leachate. Longer granulation time and instability of aerobic granules are some of the major
shortcomings that limit its commercial application. Additionally, the single-stage treatment of landfill leachate
using AGR poses several difficulties, such as low organic and recalcitrant pollutant removal efficiency, which
needs post-treatment. Hence, an integrative approach is imperative for treating landfill leachate with a high
organic load to meet the effluent standard. The present study highlights an in-depth critical review of various
biological processes, recent developments in AGR, and the factors affecting its performance, mass balance, and
the kinetics involved during landfill leachate treatment. Subsequently, the integrated process for the treatment of
landfill leachate has been summarized along with the future prospects of AGR.

1. Introduction composition of wastes, which further impedes the functionality of con­


ventional sewage treatment processes to meet the desired discharge
In developing countries, landfilling is one of the most economical limit (Syron et al., 2015). A separate treatment facility for leachate and
and commonly used methods adopted for dumping solid waste, which sewage in developing countries is not economically feasible. Therefore,
generates leachate due to degradation of wastes and permeation of the the co-treatment of leachate and sewage seems a viable option that can
rainwater through the decomposed wastes (Sanguanpak et al., 2015). meet effluent standards without installing separate treatment facilities
Furthermore, the excessive moisture content in the landfill wastes tends (Zhang et al., 2021a).
to overflow through the porous media resulting in leachate generation. The physico-chemical process is widely used to remove the recalci­
Leachates are the black color liquid mixture produced during landfill trant organic compounds and nitrogen present in higher concentrations
stabilization, comprising biodegradable and non-biodegradable toxic in landfill leachate (Brasil et al., 2021). It is used as pre or post-treatment
compounds (Ramalho et al., 2022; Bejgarn et al., 2015). Landfill to enhance the biological treatment efficiency of leachate by improving
leachates are majorly composed of biodegradable organic matter, humic its effluent quality (Rohers et al., 2021). However, these processes are
and fulvic acids, heavy metals, nitrogenous matter, and chlorinated expensive and require high energy for operation and maintenance
organics (Shehzad et al., 2015). These contaminants pollute the surface (Farooq and Ahmad, 2017). Kurniawan et al. (2021) reported that sta­
water, groundwater, soil, etc., causing severe threats to ecosystem and bilized landfill leachate contains refractory pollutants with less biode­
animal life (Moody and Townsend, 2017). gradable matter that can be removed by physico-chemical processes.
The leachate characteristics vary widely concerning space, time, and Landfill leachate also contains various heavy metals, such as Cd, Hg, Cu,

* Corresponding author.
E-mail address: susant.padhi@snu.edu.in (S. Kumar Padhi).

https://doi.org/10.1016/j.enmm.2022.100689
Received 30 October 2021; Received in revised form 3 March 2022; Accepted 27 March 2022
Available online 30 March 2022
2215-1532/© 2022 Elsevier B.V. All rights reserved.
V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Cr, Mn, Pb, and Zn, effectively removed by activated carbon (Budihardjo This review summarizes the general characteristics of landfill
et al., 2021). However, the major drawback is its short service life, leachate and the biological techniques adopted for its treatment with a
making it unsustainable for long-term applications. The heavy metals major focus on AGR. It critically examines various factors affecting the
are in soluble form in leachate, and due to their complex composition, it performance of AGR, mass balance, and the kinetics involved during
is difficult to remove by sand filter (Kietlińska and Renman, 2005). landfill leachate treatment. Further, the enhancement of leachate
The urgent need of the hour is a sustainable leachate treatment treatment by integrating physico-chemical techniques with various
technique with low energy and chemicals consumption with maximum biological processes is highlighted. Afterward, the future prospects of
treatment efficiency. Various innovative methods such as biological AGR by combining it with other post-treatment techniques for treating
techniques (Miao et al., 2019), and membrane separation techniques landfill leachate are discussed. The elucidations of the present review
such as microfiltration (Cheng et al., 2018), ultrafiltration (Dolar et al., will be beneficial for the scientific community for further research on
2016), nanofiltration (Amaral et al., 2016), and reverse osmosis (Smol AGR for landfill leachate treatment.
et al., 2016) are used by researchers for the treatment of landfill
leachate. The biological treatment method is the most reliable, simple, 2. Characteristics of landfill leachate
cost-effective, and widely applicable for treating emerging contaminants
in leachate (Tałałaj et al., 2019; Bove et al., 2015). Various process In many developing countries, municipal solid waste (MSW) is pri­
parameters like solid analysis, chemical oxygen demand (COD), total marily disposed of in open dumps without liner, leachate collection, and
organics or inorganic carbon (TOC/TIC), and total nitrogen (TN) are treatment facilities (Negi et al., 2020). This leads to the generation of
some of the most relevant indicators, which substantiate the biological brown-colored concentrated leachate with high chemical oxygen de­
treatment process. The biological treatment methods have lesser mand (COD) with low biochemical oxygen demand (BOD) to COD ratio
removal efficiency for specific pollutants. However, it can be improved (Calabrò et al., 2010). The major pollutants found in the leachate are
in a controlled environment with optimized conditions (Miao et al., categorically sub-divided into dissolved organic matter, inorganic
2019). These optimum conditions help to increase the microorganism macro components, heavy metals, and xenobiotic organic compounds
growth in the biological process, leading to higher COD, color, and other (Christensen et al., 1994). The presence of organic substances, ammo­
pollutants removal from leachate (Tałałaj et al., 2019). However, the niacal nitrogen, and heavy metals in the landfill leachates are of great
major concern is the treatment of recalcitrant pollutants present in the concern to the environment (Yusof et al., 2009). Additionally, the
landfill leachate using conventional biological methods like the acti­ composition of landfill leachates varies with the nature of solid waste,
vated sludge process (ASP). the presence of different microbial populations, soil characteristics, and
Aerobic granular reactor (AGR) is one of the most promising and landfill age (Baettker et al., 2020). The leachate that occurs in less than
innovative biological techniques employed over the last few decades to five year is termed as young landfills leachate and the pH level of these
treat landfill leachate at higher efficiency (Ren et al., 2017a). The leachates lies in the neutral range. However, it might be acidic due to the
spherical compact and dense microbial biomass is created over a period anoxic digestion of the organic waste present in it. The leachate is
of time in AGR operating in sequencing batch mode or continuous mode classified as old if it is more than ten years aged, and pH is basic in
(Adav et al., 2008). The sequencing batch mode is preferred in AGR for nature. Table 1a shows the characteristics of leachate based on its age.
developing aerobic granules with excellent biomass settleability, high The rainwater, chemical composition and moisture content in waste,
biomass retention, sustained high organic loading, and less sludge and landfill age are the most critical factors that govern leachate char­
generation (Sarma et al., 2017). Several factors like feeding time, star­ acteristics (Abuabdou et al., 2020). It has been reported that the prin­
vation period, hydrodynamic shear effect, and organic loading rate cipal pollutants in leachate are organics and ammonia; with the increase
directly influence the formation as well as stability of aerobic granules in in landfill age, the COD concentration decreased amidst an increase in
the AGR (Di Bellaa & Torregrossa, 2014). So far, AGR is widely used on a ammonia concentration (Kulikowska and Klimiuk 2008). In general,
laboratory scale, except few studies that reported the application of AGR young landfill leachates are easily treatable than the old ones. Thus,
in pilot-scale treatment (Pronk et al., 2015). The first full-scale AGR with leachate characterization is essential before designing/adopting any
more than 40 plants operated across the Netherland was reported by treatment technique. The variation in the composition of landfill
Pronk et al. (2017). The results showed a 25–75% reduction in land leachates generated is summarized in Table 1b.
footprints and a 20–50% reduction in energy with enhanced biological
nutrient (nitrogen and phosphorus) removal than the conventional ASP. 3. Treatment of landfill leachate
The AGR showed promising results, which can sustain a high shock load
(~14 kg COD/m3 d) compared to ASP when treating industrial waste­ Three different processes, viz. (i) physico-chemical, (ii) biological,
water and landfill leachate (Zheng et al., 2020). However, a limited and (iii) integrated, are usually adopted for the treatment of landfill
investigation reported the stability of aerobic granules during large- leachates, as shown in Fig. 1 (Luo et al., 2020). Coagulation-flocculation,
scale treatment. In addition, the effect of various operational parame­ adsorption, chemical oxidation, advanced oxidation processes (photo­
ters for removing nutrients and its optimization during pilot-scale chemical, fenton, and ozonation), electrochemical technique, and
treatment has a significant challenge that needs to be addressed to
promote this technology for an extensive application.
The primary issue of landfill leachate is its high degree of variability Table 1a
in both quality and quantity (Bove et al., 2015). Leachate character­ Leachates characteristics based on its age (Abuabdou et al., 2020).
ization and its risk assessment are also challenging to predict, which is Parameters Young Intermediate Old
required for selecting an appropriate technique for leachate treatment Age (years) <5 5–10 >10
(Tałałaj et al., 2019). In addition, landfill leachate contains a high COD (mg/L) >10000 4000–10000 <4000
concentration of NH3-N, which is of particular concern during the NH3-N (mg/L) <400 – >400
treatment. The physico-chemical process effectively removes refractory BOD/COD >0.3 0.1–0.3 <0.1
pH 6.5–7.5
organic compounds, inorganic macro-components, and heavy metals
<6.5 >7.5
Organic 80% VFA 5–30% VFA, humic, and Humic, and
from leachate. In contrast, dissolved organics and nutrients in leachates compounds fulvic acids fulvic acids
are efficiently removed by biological processes (Teng et al., 2021). Biodegradability High Medium low
Therefore, an integrated approach involving biological with pre or post- Heavy metals Low- low low
physico-chemical processes is a viable option that provides better medium

effluent quality (Huang et al., 2015; Zhang et al., 2019a). VFA: Volatile fatty acid.

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Table 1b 4. Biological process for leachate treatment


Variation in the composition of landfill leachates.
COD BOD BOD/ pH Total NH3-N References In biological treatment processes, microorganisms play an essential
(mg/L) (mg/ COD nitrogen (mg/L) role in the biodegradation of organic contaminants, which are simple,
L) ratio (TN) (mg/ economical, attractive, and eco-friendly in nature (Padhi and Gokhale
L)
2014). The biological treatment method efficiently treats landfill
720 590 0.82 6.7 1030 910 (Tałałaj et al., leachate with a high concentration of organic matter and NH3-N while
2021) producing carbon dioxide (CO2) and sludge as the end product. How­
2180 135 0.06 7.84 450 400 (Tałałaj et al.,
2021)
ever, biological treatment efficiency depends on the optimum operating
3960 372 0.09 7.8 – 2323 (Collado et al., conditions required for the maximal growth of microorganisms. Various
2020) biological methods are used for the aerobic treatment of landfill
5548 3077 0.55 8.7 – 3247 (Collado et al., leachate, which includes (i) activated sludge process, (ii) aerated la­
2020)
goons, (iii) rotating biological contactors (RBC), (iv) trickling filters, (v)
9765 3027 0.3 7.1 1923 1810 (Zhang et al.,
2019a) moving-bed biofilm reactor (MBBR), (vi) hybrid bioreactor (HBR), and
2235 192.5 0.08 8 618.7 511.8 (Hu et al.,
2018) Table 2
2194 45 0.02 8.2 – 2980 (da Costa et al.,
The advantages and disadvantages of various physico-chemical processes (Far­
2018)
1931 863 0.44 7.8 – 2185 (da Costa et al.,
ooq and Ahmad, 2017).
2018) Physico-chemical Advantages Disadvantages
5650 2640 0.46 8.2 – 1680 (Maiti et al., treatment
2016) methods
2848 150 0.05 7.9 1480 1319 (Amaral et al.,
2015) Coagulation- • Simple and eco-friendly • A huge amount of sludge is
6560 3320 0.5 8.2 2020 1740 (Müller et al., Flocculation produced and not
(TKN) 2015) (C/F) economic
4290 2080 0.48 7.9 1980 1750 (Huang et al., Adsorption • Good removal of a variety • Short service life
2014) of pollutants • Not efficient to remove
5890 2050 0.34 8 1170 1030 (Wang et al., heavy metals, Na+, NO3-,
2013) and F
2390 420 0.17 8 1420 1210 (Ferraz et al., Chemical • Fast and adaptable process • High energy requirement
2013) oxidation and costly
3847.7 388 0.11 8.1 5236 3158.98 (Boumechhour Photo-chemical • Less or no sludge and odour • Secondary pollutants are
(TKN) et al., 2013) oxidation free process generated
Electrolysis • Highly effective for • Large amount of by-
removal of colour from products are generated, so
leachate not applied on full scale
membrane separation are widely used physico-chemical processes
Ozonation • Powerful oxidant able to • The cost of treatment is
adopted for leachate treatment (Luo et al., 2020). These techniques are degrade the COD efficiently very high and ozone is
mainly used to remove contaminants, primarily refractory organics, highly corrosive in nature
non-biodegradable organics, and heavy metals. However, these tech­ Fenton process • Soluble and insoluble • Produced a significant
niques are quite outrageous and responsible for generating secondary colouring agents can be amount of sludge
removed effectively
pollutants (Silva et al., 2013). The advantages and disadvantages of Membrane • Effective for • Expensive and huge
physico-chemical treatment process are summarized in Table 2. separation decolourization of leachate amount of sludge is
generated

Fig. 1. Processes for landfill leachate treatment.

3
V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

(vii) sequence batch reactor (SBR). The characteristics, advantages, and total organic carbon removal. In contrast, the total nitrogen and NH3–N
disadvantages of these biological treatment methods are summarized in removal efficiencies were increased with increased calcium concentra­
Table 3. tion in the leachate. In a recent study, ASP integrated with a fungal
bioreactor containing Penicillium sp. was used to treat mature landfill
4.1. Activated sludge process leachate, unveiling good potential for removing COD (41%) and nutri­
ents at optimal conditions (Islam et al., 2020). The ASP is a promising
The activated sludge process (ASP) is the most common and highly technology for treating landfill leachate, except for removing nitrogen,
effective method in treating leachate. This process consists of an aera­ which is low compared to other processes (Wang et al., 2018). In
tion chamber for efficient mixing and better contact of microorganisms addition, excessive sludge generation, huge electricity requirement for
with the pollutants in influents while transforming it to new active operation, and microbial inhibition at high NH3-N concentration are
biomass along with water, nutrients, and carbon dioxide (Fig. 2a) (Luo some added limitations of ASP while treating leachate (Torretta et al.,
et al., 2020). Webler et al. (2019) treated tannery landfill leachate using 2017).
a modified continuous flow anoxic/aerobic ASP operated at an optimum
temperature (20–26 ◦ C), pH (6.5–8.5), dissolved oxygen (5–8 mg/L), 4.2. Aerated lagoons
and food microorganism (F/M) ratio (0.09–0.21 g BOD5/g MLVSS d) to
promote oxidation of organics and nitrification. Approximately 100% of Aerated lagoons or stabilization ponds used for on-site treatment of
BOD and 87% of COD removal were observed under these optimized landfill leachates are user-friendly, cost-competitive, and effective at
conditions in this process. Çeçen & Gürsoy (2001) reported the various environmental conditions (aerobic/anaerobic/facultative) over
adsorption of heavy metals from the landfill leachate onto activated the period of time (Luo et al., 2019). A schematic of aerated lagoon used
sludge and the results of this study indicated higher biosorption capacity for landfill leachate treatment is shown in Fig. 2b (Martins et al., 2013).
at a shorter duration. Another study that used ozonation in the pre- The temperature plays an essential role in microbial activity, which
treatment process decreased COD/BOD ratio of leachate from 16 to 6, further regulates the biological oxidation of leachate in lagoons. How­
which was later co-treated with municipal sewage in the ASP (Geenens ever, it requires a large footprint despite no external energy consump­
et al., 2001). This method was found to be economical and efficient for tion and less construction cost (Frascari et al., 2004). Optimization of
landfill leachate treatment. Furthermore, the ASP associated with HRTs also plays a crucial role in the full-scale applications of the aerated
microfiltration successfully treated landfill leachate, resulting in 52%, lagoons used for leachate treatment (Mehmood et al., 2009). The COD
94%, and 75% removal of COD, BOD, and NH3-N, respectively (Setiadi removal efficiency varies by the leachate type (young or old) and can be
& Fairus, 2003). Co-treatment of sanitary landfill leachate with domestic as high as 95% for young leachate (Renou et al., 2008). A two-stage
wastewater in a bench-scale ASP containing powdered activated carbon process, an anaerobic lagoon (HRT: 2 days) followed by a facultative
(PAC) revealed a positive effect on treatment during shock loading system (HRT: 240 days) at 22.8 ◦ C, achieved up to 40% COD, 64% BOD,
(Cecen and Aktas, 2004). In another study, response surface methodol­ 77% NH3-N, and 63% NO3-N reduction (Renou et al., 2008). In another
ogy (RSM) was adopted to evaluate the effect of PAC augmented ASP to study, Mehmood et al. (2009) achieved 75% average COD removal and
treat semi-aerobic leachate at different hydraulic retention times (HRTs) 80% nitrogen removal using an aerated lagoon with varying HRTs
(0.92, 1.57, and 2.22 d) and COD concentrations (700–3000 mg/L) (11–254 days). This study further revealed that longer HRT enhances the
(Aghamohammadi et al., 2007). The addition of PAC in ASP enhanced performance of the aerobic lagoon. A study performed using series of
two-fold higher removal of COD along with color and NH3–N. In order to shallow (~0.5 m deep) waste stabilization ponds showed good removal
treat leachate with high COD concentration (48,000–62,000 mg/L), the of NH3-N (99%) and COD (67%) at 39.5 days HRT with the initial
combination of anaerobic and aerobic ASP was found to be more suit­ loading of 364 kg/ha/d NH3-N and 3676 kg/ha/d COD, respectively
able than single-stage operation (Kheradmand et al., 2010). In aerobic (Leite et al., 2011). A pilot-scale system, consisting of three ponds in
ASP, 94% of COD, 48–64% of NH3–N, and 49–60% of alkalinity removal series operated for 111 weeks to treat landfill leachate showed good
were achieved. However, no alkalinity and NH3–N removal were removal of NH3-N with 75–99% efficiency and 35–82% removal of COD
observed in the anaerobic ASP. The study by Xia et al. (2017) focused on at an initial soluble COD concentrations of 1230 to 4020 mg/L (Martins
the inhibitory effects of calcium over the biological treatment of landfill et al., 2013). In order to evaluate the symbiotic relationship between
leachate using an ASP. The study revealed that increased calcium con­ microalgae and bacteria during landfill leachate treatment, stabilization
centration of more than 4500 mg/L in leachate significantly reduced the ponds are integrated in series and operated for 43 weeks (Costa et al.,

Table 3
Characteristics, advantages and disadvantages of the various biological treatment methods.
Biological Methods Characteristics Advantages Disadvantages References

Activated sludge • Suspended growth process • High organic removal • Huge sludge generation (Wang et al., 2018)
process • Odour free treatment • Poor biomass settle ability
Aerated lagoons • Suspended growth process • Easy operation and • Difficult to treat recalcitrant (Britz 2020; Leite et al., 2011)
• Symbiotic interactions exist between maintenance compounds
microalgae and bacteria • Low-cost investment with good • Require large footprint
removal efficiency
Rotating biological • Both attached and suspended growth • High contact time resulting in • Require continuous electricity (Padhi and Gokhale 2017; Bove
contactors (RBC) process high effluent quality supply et al., 2015)
• Partially submerged in leachate • High stability at shock loading • High investment, operation, and
maintenance costs
Trickling filters • Attached growth process • Low power requirement • High clogging problem and (Luo et al., 2020; Bressani-
• Highly effective for removal of generates the odour Ribeiro et al., 2018)
ammonia (NH3-N)
Moving-Bed biofilm • Both attached and suspended growth • No clogging problem • Periodic monitoring required (di Biase et al., 2019; Bassin &
reactor (MBBR) process • No sludge recycling required • Skilled experts required for Dezotti, 2018)
operation and maintenance
Sequence batch reactor • Suspended growth process • High biomass settle ability • Required skilled labour for (Jagaba et al., 2021; Tomar &
(SBR) • Fill and draw process by maintaining • Low sludge generation operation Chakraborty 2019)
the different cycle • Sustain high shock load • Sophisticated operating procedure

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Fig. 2. Schematic of (a) ASP (Luo et al., 2020), (b) stabilization pond (Martins et al., 2013), (c) RBC (Bove et al., 2015), (d) trickling filter (Matthews et al., 2009), (e)
MBBR (Ødegaard, 2006), (f) HBR (Saxena et al., 2021), and (g) SBR (Islam et al., 2020) used for leachate treatment.

5
V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

2014). These ponds are sub-divided in three stages based on varying 4.4. Trickling filters
aeration periods (12 h and 18 h), resulting in approximately 75% BOD
and NH3-N removal efficiency. A good balance of the microbial diversity A trickling filter or biofilter is a type of biological fixed bed reactor
and efficient leachate treatment was found in the stabilization pond that contains inert packing material for the growth of microorganisms,
mainly due to phytoplankton, nitrifying bacteria, and Ciliate organisms. which is opened from the top to maintain aerobic conditions. The
Natural treatment techniques such as stabilization pond and its opera­ leachate is trickled from the top comes in contact with the packing
tion achieve higher nitrogen removal than other biological processes material forming a biofilm layer over the media, as shown in Fig. 2d
(Jinadasa et al., 2018). (Matthews et al., 2009). A trickling filter is generally adopted to treat
landfill leachate with low organic strength (Torretta et al., 2017). A low-
4.3. Rotating biological contactor cost nitrification process was performed in a lab-scale biofilter at low
temperature, achieved 90% nitrification of leachate, followed by deni­
Rotating biological contactor (RBC) mainly consists of a closely trification (Jokela et al., 2002). Another study evaluated the perfor­
packed series of large flat surfaces or perforated drums with bio-support mance of landfill leachate treatment in a trickling filter with shredded
medium for biofilm growth connected to a horizontal shaft (Cortez et al., tire chips and tire crumbs as packing media. The results showed better
2008; Padhi and Gokhale 2014). The RBC with microorganisms in the removal of COD (70–90%) and NH3-N (15–68%) for the tire crumb
form of biofilm is partially or fully submerged in wastewater or leachate packed filter, which is also economical for small-scale treatment
to be treated (Fig. 2c). Several operating parameters such as rotation (Mondal et al., 2007). The effect of operating parameters such as
speed, HRT, types of support media used for biofilm development, leachate characteristics (organic carbon and ammonia) and temperature
loading rates, oxygen demand, and recirculation of solids, etc., influence (3–30 ◦ C) over the treatment efficiency and process dynamics of trick­
the performance of RBC (Cortez et al., 2008; Padhi and Gokhale 2017). ling filters confirmed that the NH3-N removal was unaffected by these
The geared motor is generally used for rotating the shaft at a uniform parameters. In contrast, organic carbon removal increases with
speed, allowing consistent growth of biofilm over the surface of the increasing temperature (Mattews et al., 2009). In comparison between
supporting medium, imparting better oxygen and mass transfer, result­ the performance of lab-scale trickling filter and SBR, a significant
ing in efficient removal of organic matter present in the waste streams reduction of suspended solids (73%), turbidity (72%), COD (49%), BOD
(Rodgers and Zhan, 2003). Cortez et al. (2011) reported high removal (77%), and NH3-N (60%) was observed for trickling filter (Aluko and
efficiencies (~100%) for NO3-N from mature landfill leachate using a Sridhar, 2013). Conversely, effluent quality was better in SBR with 76%
RBC. Kurniawan et al. (2010) indicated that RBC is not efficient for COD, 84% BOD, and 65% NH3-N removal. Aged refuse-based biofilter
treating high-strength landfill leachate as it clogs the media due to (ABR), a modified trickling filter, is a promising technology resulting in
excessive biomass growth. An integrated process consists of an anaer­ less sludge generation with 64–99% COD, 90% BOD5, and 66 to 99%
obic filter followed by RBC was used to treat high strength NH3-N in NH3-N removal (Hassan & Xie, 2014). Ferraz et al. (2014) performed co-
landfill leachate, which indicated more than 95% NH3-N removal at an treatment of domestic sewage with landfill leachate using a submerged
initial concentration of 2140 mg/L along with 49% overall COD removal aerobic bio-filter, which resulted in better removal of BOD (~98%),
(Henderson and Atwater, 1995). A comparative study on NH3-N removal COD (~80%), suspended solids (~90%), and NH3-N (~90%). A com­
from landfill leachate using a pilot-scale RBC and SBR operated for 14 posite biological trickle reactor was used to treat mature landfill
months indicated better performance of SBR than RBC with ~100% leachate at optimum conditions (temperature: 30 ◦ C and hydraulic
NH3-N removal at 400 g/m3 d NH3-N loading (Henderson et al., 1997). loading: 40 L/m3d), where the removal of COD, TN, NH3-N, and PO4-P
Siegrist et al. (1998) reported about 70% nitrogen removal from were 85, 76, 99, and 96%, respectively (Zhu et al., 2021). It can be
ammonium-rich landfill leachate using a RBC and negligible organic concluded from these studies that the trickling filter shows better per­
carbon removal using coagulation and flocculation as a pre-treatment. formance for treating landfill leachate with high strength NH3-N con­
An integrative approach (nitrification, Anammox, and denitrification) centration, but its performance is limited for COD removal.
for removing total inorganic nitrogen in a RBC resulted in a maximum
removal rate of 3 g N/m2 d and 3.9 g N/m2 d for NH3-N and NO2–, 4.5. Moving bed biofilm reactor
respectively (Cema et al., 2007). Feasibility of leachate treatment using
a RBC compared with up-flow anaerobic sludge bed reactor operated at The moving bed biofilm reactor (MBBR) is a modified form of ASP
different HRTs showed a maximum of 52% COD removal in RBC (HRT: consisting of a moving bed such as plastics or sponges in the aeration
24 h and rotation speed: 6 rpm) at a hydraulic organic loading of 24.7 g tank to enhance biofilm growth (Fig. 2e) (Ødegaard, 2006). Welander
COD/m2 d and 62% COD removal in the anaerobic reactor (HRT: 54 h) et al. (1997) used suspended-carrier biofilm technology to treat
at a volumetric organic loading of 3273 g COD/m3 d (Castillo et al., municipal landfill leachate by nitrifying a maximum up to 40 g NH3-N/
2007). An anoxic RBC is recommended for achieving 95% landfill m3 h at 14 h HRT and 20 ◦ C with 10% carrier fraction with respect to
leachate denitrification with a high concentration of NO3-N (up to 100 reactor volume. The MBBR is suitable for treating leachate with a high
mg/L) and carbon to nitrogen ratio (C/N) of<2 (Cortez et al., 2011). nitrogen removal efficiency of up to 90% but incompetent for treating
However, high effluent COD required further treatment to remove the COD (20%) (Welander et al., 1998). Loukidou and Zouboulis (2001)
organic content. A two-stage RBC treated landfill leachate with an NH3- used activated carbon in MBBR for landfill leachate treatment and
N load of 3.6 g/m2 d showed complete nitrification. However, the achieved 60–80% COD and 85–90% NH3-N removal for influent COD
further increase in NH3-N load up to 6.63 g/m2 d decreased the nitrifi­ and NH3-N at concentrations of 5000 mg/L and 1800 mg/L, respec­
cation efficiency up to 71%, which also changed the microbial popula­ tively. Simultaneous removal of COD and NH3-N was investigated using
tion in RBC (Kulikowska et al., 2010). A pilot-scale anoxic RBC was a MBBR with both aerobic and anaerobic environments for landfill
operated for 88 days to treat landfill leachate, which removed COD leachate treatment (Chen et al., 2008). Methanogenesis in anaerobic
(2278–7695 mg/L) and NH3-N (366–1444 mg/L) of 85 and 99%, MBBR leads to the removal of COD, whereas aerobic MBBR plays as a
respectively (Song et al., 2020). RBC alone may not be efficient for polishing treatment for the removal of both COD and NH3-N. The
treating landfill leachate. Hence, combining physico-chemical and bio­ maximum COD removal of 91% was observed in anaerobic MBBR,
logical processes with RBC is required for effective treatment (Castillo which decreased to 86% with an increase in loading rate. However, in
et al., 2007; Cortez et al., 2008). aerobic MBBR, only 3–12% of COD removal was observed, but a sig­
nificant amount of NH3-N was removed with more than 97% efficiency
at an HRT of 1.25 days.
A combination of MBBR and membrane bioreactor was used for

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

oxidation of NH3-N (initial concentration: ~50 mg/L) to nitrite, up-gradation for its large-scale continuous applications are the major
achieving more than 90% removal efficiency during this process (Can­ challenges of this process. Wei et al. (2012) used SBR to treat leachate,
ziani et al., 2006). In another study, an anoxic MBBR is coupled with a confirmed that high influent NH3-N concentration has a detrimental
membrane bioreactor used to treat landfill leachate, in which the effect on COD removal. Miao et al. (2015) used SBR under anaero­
maximum removal of COD, NH3-N, and NO3-N were 74, 99, and 89%, bic–aerobic-anoxic conditions for a period of 70 days and achieved high
respectively, at the optimum conditions (NO3-N concentration: 1000 nitrogen removal of more than 98% at the C/N ratio of 4. A recent study
mg/L, HRT: 48 h, and SRT: 90 d) (Duyar et al., 2021). The high meta­ on the treatment of mature urban leachate using coagulation/sedi­
bolic activity of microorganisms attached to the supporting media pro­ mentation followed by advanced oxidation and SBR was performed,
vides a stable performance to the MBBR. Also, the small footprint of which resulted in up to 98% COD and 85% total nitrogen removal
MBBR has the competencies for reducing volume up to 70% without (Gomes et al., 2019). Leachate treatment using SBR confirmed an
compromising its effectiveness for treatment. The MBBR does not consist effective reduction of COD by 76%, BOD5 as high as 84%, NH3-N
of a fixed filter media, which results in no clogging while removing removal of about 64%, and more than 60% removal of the metals
organic and nitrogen matter from leachate. The only major disadvantage (cadmium, iron, and zinc) (Aluko and Sridhar, 2013). A summary of
of using this process is the high energy requirement in aeration for the different biological methods adopted to remove COD and NH3-N from
smooth operation of MBBR. landfill leachate is given in Table 4.

4.6. Hybrid bioreactor


4.8. Aerobic granular reactor
The hybrid bioreactor (HBR) consists of both aerobic and anaerobic
systems that are efficient for treating high-strength landfill leachate The aerobic granular reactor (AGR) is a type of SBR that has evolved
(Saxena et al., 2021). The HBR is one of the popular systems comprised to replace the conventional waste treatment approach in the past two
of both suspended and attached growth microorganisms to treat decades. Landfill leachate treatment using the conventional ASP is
leachate wastewater (Fig. 2f) (Saxena et al., 2021). In the suspended incompetent in achieving the desired removal of organic matter and
system, the microbial colonies in the form of flocs tend to move freely in total nitrogen (TN) (Wang et al., 2018). The schematic of AGR and the
the mixed liquor due to the continuous aeration in the reactor (Lippi conversion process in aerobic granules during leachate treatment is
et al., 2018). Alternatively, in the attached growth system, inert sup­ shown in Fig. 3 (Wei et al., 2012; Wilén et al., 2018). The aerobic
porting media consisting of rock or plastic is used to retain bacteria, granules in AGR consists of a multilayer sphere with decreasing oxygen
wastes, and extracellular polymers (Shah et al., 2017). The small and and substrate gradients from the periphery towards the core of the
porous carriers help in retaining more biomass allowing the reactor to granule (Fig. 3). Generally, nitrifiers and heterotrophic bacteria are
operate at shorter hydraulic retention times (HRTs) (Chen et al., 2019). located in the oxygen penetrated outer layers (Wilén et al., 2018). In
According to the study conducted by Zhang et al. (2017), polyurethane contrast, denitrifiers and phosphate-accumulating organisms (PAOs) are
foams are considered an ideal media for the attached growth of micro­ found in the inner layers.
organisms because of their high porosity, which allows the biomass to AGR operated at low HRT with simultaneous anaerobic/aerobic
grow over the surface as well as inside pores. This study also revealed environment to treat landfill leachate with varying waste loads. It is
that polyurethane foams are used to obtain a quicker reactor start-up efficient in terms of performance and granule stability in lab-scale
while offering higher removal of COD and NH3-N, by improving the studies. However, the full-scale application is still in the developing
overall performances as compared to other bio-carriers such as poly­ stage, which needs further investigation (Wilén et al., 2018). The
ethylene. Song et al. (2019) reported that polyurethane sponge is an knowledge gap needs to be satisfied to widespread this technique
ideal choice of bio-carrier due to simultaneous nitrification and deni­ commercially. Granule inhibition due to certain factors such as the hy­
trification properties. drodynamic pattern in the pilot-scale reactor can lead to operational
Loukidou & Zouboulis (2001) used a lab-scale SBR with different bio- failure, which is successfully applied to lab-scale reactor counterpart if
carriers (polyurethane sponge and granular activated carbon) operating the process is not appropriately optimized (Pishgar et al., 2018). The
as a hybrid system to treat sanitary landfill leachate. High nitrogen summary of various AGRs used for the treatment of landfill leachate is
removal from landfill leachate was observed by using granular activated shown in Table 5.
carbon (GAC) as bio-carrier in addition to the removal of biodegradable
organics. Moreover, it generates a large amount of residual suspended 4.8.1. Aerobic granules formation
solids, which tends to increase the operational costs of the process. In The AGR has more advantages over the conventional ASP, such as
contrast, the highly porous polyurethane sponge aids in more biomass high settleability, high retention of biomass, denser, compact, and ho­
accumulation leading to an extended operation period than GAC. Mir­ mogenized microbial structure, but it needs a longer start-up period for
ghorayshi et al. (2021) used a hybrid airlift bioreactor (HAB) to remove its formation and maturation (Hamza et al., 2018). Zhang et al. (2016)
carbon and nitrogen simultaneously from composting leachate. At the proposed four-step granulation mechanism (Fig. 4a), which involves (i)
optimum conditions (HRT: 28–30 h and air flow rate 1.7–2 L/min), the initial adhesion of cells to start granulation, (ii) micro aggregates for­
COD (3600 mg/L) and NH3-N (598 mg/L) removal were 90% and 80%, mation, (iii) extracellular polymeric substance (EPS) biosynthesis by
respectively, which shows the feasibility of HAB for leachate treatment. accumulated microbes, and (iv) granule maturation.

4.7. Sequencing batch reactor 4.8.2. Factors affecting granulation


Various factors such as inoculum type, substrate composition,
The sequencing batch reactor (SBR) is the modified version of ASP organic loading rate, settling duration and cycle time, HRT, superficial
capable of removing various pollutants while treating landfill leachate. up-flow air velocity, dissolved oxygen, and temperature affect granu­
Aerobic granular reactor (AGR) is one such type of SBR consisting of lation and performance of AGR (Fig. 4b) (Awang and Shaaban, 2016;
mainly four steps: (i) feeding, (ii) aeration, (iii) settling, and (iv) Lee et al., 2010). Upgrading the hydrodynamic shear force, changing the
decanting (Jagaba et al., 2021). The schematic of SBR for landfill operating conditions, inoculum, anaerobic/aerobic starvation period,
leachate treatment is shown in Fig. 2g. It has various advantages over and settling time reduce the granulation time and enhance granulation
the conventional ASP, like good sludge settleability, high biomass (Long et al., 2015).
retention, and compact microbial granules that can resist high shock
loading (Hamza et al., 2018). In contrast, the formation of granules and 4.8.2.1. Inoculum. During the start-up phase, active biomass, usually

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Table 4
Summary of different biological methods for removal of COD & NH3-N from landfill leachate.
Biological methods Operating conditions COD NH3-N Remarks References
removal removal (%)
(%)

Hybrid bioreactor • COD: 150-1200 mg/L • 77-80 • 60-94 • Resist high shock load at short HRT (Saxena et al.,
(HBR) • NH3-N: 2-49 mg/L • Retains high biomass 2021)
• PO4-P: 97-281 mg/L
• HRT: 3-48 h
Moving-bed biofilm • NH3-N: 50-1500 mg/L • - • 60-85 • Inoculating the MBBR with bio-carriers obtained from municipal (Xiong et al.,
reactor (MBBR) (sequencing batch mode) wastewater treatment plant showed great potential to mitigate the 2018)
• NH3-N: 900-1500 mg/L • 50-80 secondary landfill leachate
(continuous mode)
• HRT: 10-20 days
Activated sludge • COD: 811±75 mg/L • 52-83 • 60-80% • TAN removal of ~99% was observed at 300 mg/L concentration (Ren et al.,
process (ASP) • Total ammoniacal (TAN) • A relative decreasing COD removal due to a lower COD/TAN ratio 2017b)
nitrogen (TAN): 131-454
mg/L
• Operated for 3 cycles for
day
SBR • COD: 4950-5331 mg/L • 82-84 • 44-92 • COD removal decreased with an increase in NH3-N concentration (Wei et al.,
• NH3-N: 366-1105 mg/L • NH3-N removal depends upon its influent concentration in leachate 2012)
• SRT: 25-35 d
• DO: 0.76-4 mg/L
Lagoons • COD: 1740 mg/L • 75 • 80 • Longer HRT enhanced the performance of the aerobic lagoon (Mehmood
• NH3-N: 1241 mg/L et al., 2009)
• HRT: 11-254 days
• Aeration: 6-8 h/day
Rotating biological • COD: 2500-9000 mg/L • 52 • - • HRT, rotation speed, submergence of discs, and temperature mainly (Castillo et al.,
contactors (RBC) • HRT: 14-34 h influence the performance of RBC 2007)
• Rotation per minute: 3-9
Trickling filters • Hydraulic loading: 2.25- • 76-90 • 15-68 • Tire chips used in trickling filter showed better organics removal but (Mondal &
4.5 m3/m2 d required steady and proper aeration for enhancing the growth of Warith 2008)
• Organic loading: 0.28- biofilm
1.12 kg BOD5/m3 d

TAN: Total ammoniacal nitrogen, SRT: Sludge retention time, DO: Dissolved oxygen.

Fig. 3. Schematic of AGR and the conversion process in aerobic granules during leachate treatment (Wei et al., 2012; Wilén et al., 2018).

floccular or activated sludge, is collected from the landfill site or the municipal wastewater treatment plants as the seed inoculum in AGR
oxidation ditch of the landfill leachate treatment plant with an MLSS (Ivanov et al., 2006). Interestingly, aerobic granules can also be formed
concentration of 3–4 g/L and inoculated in the AGR (Wang et al., 2013). by seeding anaerobic granules in SBRs (Linlin et al., 2005). The presence
Pishgar et al. (2019) utilized return activated sludge from a wastewater of various bacteria in seed sludge such as Paracoccus, Devosia, Pseudox­
treatment plant with MLSS concentration of 2.8 g/L, ensuring the anthomonas, and Acinetobacter are effective in self-aggregation, resulting
presence of diverse microbial communities for enhancing granulation. in the formation of granules (Adav et al., 2008).
On the other hand, Verawaty et al. (2012) used mixed inoculum con­
sisting of crushed granules and floccular sludge to accelerate granula­ 4.8.2.2. Substrate composition. Substrate concentration directly in­
tion. In most of the research, floccular sludge was collected from fluences the microbial growth and synthesis of EPS (Liu and Liu, 2006).

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Table 5
AGR for landfill leachate treatment.
Operating conditions COD removal (%) TANa/ TNb PO4-P removal Findings References
removal (%) (%)

• Organic loading rate: 4651-19100 mg/L • 39-80 • 45-74a • 41-66 • The removal of COD, TN, and PO4-P was (Seid-mohammadi
• TAN: 286-596 mg/L higher during longer HRT et al., 2022)
• HRT: 2.1-6 h
• Lechate diluted with wastewater at 20% and
50% volumetric ratio
• COD: 5300±78 mg/L • 87-89 • 98b • 37-64 • High nitrogen removal is due to diverse (Bueno et al., 2021)
• Total Nitrogen (TN): 2630±355 mg/L microbial communities in aerobic
• Leachate diluted with wastewater at granules
volumetric ratios 5-20%
• Phosphorus load: 0.02-0.03 g/d
• COD: ~1000-5500 mg/L • 70-90 • 35-90a • - • TAN removal inhibited at high nitrogen (Wei et al., 2021)
• TAN: ~100-1200 mg/L loading rate (NLR)
• Operated for 220 days (leachate diluted with • Granular sludge increases the microbial
tap water for cultivation of granules for diversity but decreases with increase in
initial 54 days) NLR
• COD: ~500-1300 mg/L • 31 (volumetric • 99.7a • Negligible • The granular sludge in AGR is resistant to (Ren et al., 2018)
• TAN: 1200 mg/L ratio: 50-90%) toxicity of ammonia
• Leachate diluted with wastewater at 10- • 14 (volumetric • Poor PO4-P removal could be associated
100% volumetric ratio ratio: 40-65%) with competition between denitrifiers
• Phosphorus: 3-6 mg/L and PAOs
• Leachate diluted with primary effluent (10- • 64 • 95-100a • 84 • High TAN removal efficiency (Ren et al., 2017a)
90% volumetric ratio) • Simultaneous nitrification-denitrification
• COD: 2.2-3 kg COD/m3 day play a significant role in nitrogen removal
• TAN: 0.31-1.8 kg N/m3 day
• COD: 810±83 mg/L • 67-87 • 99a • ~49 • AGR showed better removal of TAN from (Ren et al., 2017b)
• TAN: 128-494 mg/L leachate than the ASP
• Phosphorus: 2-6 mg/L

TAN: Total ammoniacal nitrogen and TN: Total nitrogen.

Fig. 4. (a) Mechanism of aerobic granulation (Zhang et al., 2016) and (b) the factors affecting granulation and performance of AGR.

The performance of AGR was investigated with various carbon sources strong granules but require a long cultivating period (Lee et al., 2010; de
such as glucose, acetate, ethanol, and phenol. The formation of more Sousa Rollemberg et al., 2018). Pijuan et al. (2011) reported the use of
filamentous granules with low settling properties was observed in the pre-cultivated granular sludge as inoculum in AGR for landfill leachate
presence of glucose in the medium. Conversely, acetate in the medium treatment (Pijuan et al., 2011).
produces dense and stable granules; phenol and propionate generate

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

4.8.2.3. Organic loading rate. The organic loading rate (OLR) plays a 4.8.2.6. Superficial up-flow air velocity. Superficial up-flow air velocity
significant role in forming and characterizing granules while regulating (air flow divided by the cross-sectional area of the reactor), also known
their morphological properties and microbial communities. The OLR is as the hydrodynamic shear force effect, is one of the significant factors in
directly proportional to the size of the granules and inversely propor­ aerobic granules formation. The compactness and denseness of granules
tional to the degree of the granules formed. In addition, AGR with the are directly proportional to the shear force applied (Chen et al., 2007).
highest OLR shows the lowest biological diversity (Adav et al., 2008). Granules from the flocculant sludge were successful for low hydrody­
Moderate OLR ranging between 1 and 3 kg COD/m3 d tends to form namic shear at a lower strength of COD (340 mg/L) (Devlin et al., 2016).
stable aerobic granules (Tay et al., 2004). However, a recent study Typically, in the AGR, the superficial up-flow air velocity is maintained
shows the stability of aerobic granules up to an OLR of 15 kg COD/m3 d, in the range of 1–2 cm/s. At low superficial up-flow air velocity (0.8 cm/
but the disintegration of granules was observed with an increase in OLR s), loose microbial structure and unstable granules with poor settling
of 18 kg COD/m3 d, which led to the failure of the AGR (Long et al., properties were reported, but an increased nitrogen removal rate was
2015). Activated sludge growing at OLR decreasing from 5.5 to 3.5 kg observed (Lochmatter and Holliger, 2014).
COD/m3 d form complete granulation with size up to 438 μm and EPS to
protein ratio over 2 (Zhang et al., 2019b). Anaerobic feeding, followed 4.8.2.7. Dissolved oxygen and temperature. Aerobic granules in AGR can
by the aerobic phase, shows a fast granulation. In contrast, the granules be formed in a wide range of dissolved oxygen (DO) concentrations (1–7
formed in a fully aerobic environment have higher stability but take mg/L) (Winkler et al., 2018). But DO lower than 5 mg/L causes granule
longer duration at varying organic loading rates (1.8–6.65 kg COD/m3 instability (Wilén et al., 2018). Due to the strong diffusion limitations of
d) (Carrera et al., 2019). DO in granules, it plays a vital role in the simultaneous removal of
organic carbon, nitrogen, and phosphorus. High DO increases the
4.8.2.4. Settling duration and cycle time. The AGR operates at a shorter nitrification rate, whereas low DO increases the denitrification rate. DO
settling time (2–10 min), allowing rapid settling of microbial aggregates, concentrations can be controlled during the cycle in AGR to achieve high
enabling the washout of sludge with poor settling quality (Sepúlveda- effluent quality (Pronk et al., 2015).
Mardones et al., 2019). By repeating the same process, dense granules AGR successfully operated at a temperature range of 8–30 ◦ C. The
formation occurs with a highly active microbial community. A high aerobic granules are irregular in shape and unstable at a lower tem­
exchange ratio with a short duration of decanting leads to increase perature with low nutrient removal efficiency. At low temperatures, the
granulation. Wilén et al. (2018) reported faster granulation by short­ microbial activity is low, so DO can penetrate the inner anoxic layer of
ening the settling time from 15 to 5 min in 11 days. AGR is more granules, hampering the denitrification process (De Kreuk et al., 2005).
economical as the treatment and sedimentation happen in the same Although, AGR operated with a high removal efficiency of organic
system (Nancharaiah et al., 2018). The settling period, volumetric ex­ carbon, nitrogen, and phosphorus at a lower temperature range of
change ratio, and discharge time coupled together to settle the sludge 10–12 ◦ C (Jiang et al., 2016). However, at higher temperatures
faster is termed as minimum settling velocity (Vs), which must be above (20–30 ◦ C), a decrease in biological phosphorus removal was observed
4 m/h to form aerobic granules (Liu et al., 2005). The Vs is a function of due to favourable growth conditions for glycogen accumulating organ­
concentration of sludge (X). The Vs decreases with increase in X. The isms (GAOs) than the PAOs (Lopez-Vazquez et al., 2009).
relationship between Vs and X is represented by Eq. (1) (Bueno et al.,
2021): 4.8.3. Mass balance of COD, nitrogen, and phosphorus in AGR
Microorganisms in the aerobic granules utilize the nutrients in the
Vs = V m e − kX
(1)
form of COD, nitrogen, and phosphorus present in the landfill leachate.
where, Vs is settling velocity of sludge (m/h), Vm the maximum The COD mass balance in the AGR can be determined by using Eqs. (2)-
settling rate of sludge (m/h), X the suspended solid concentration in (4) (Lee et al., 2008):
sludge (g/L), and k the empirical settling parameter (L/g).
CODin (gCOD/d) = CODOut (gCOD/d) + CODremoved (gCOD/d) (2)
During the feeding in AGR, the cycle time between 4 and 12 h is
usually maintained (Adav et al., 2008). Shorter cycle time led to the loss CODremoved (gCOD/d) = CODbiomass (gCOD/d) + CODoxidised (gCOD/d) (3)
of the biomass, while a longer cycle time of more than 24 h fails in
forming nitrifying granulation (Liu and Tay, 2004). In order to get better CODbiomass (gCOD/d) = 1.42xVSSwasted xLeachateflowrate (4)
performance and stability in AGR, the cycle time should comprise a
short anoxic phase (10% of total cycle time) and medium aerobic phase where, 1.42 represents the COD of biomass (gCOD/gVSS) (Tchoba­
(55% of total cycle time), which is indispensable to promote fast bio- noglous et al., 2003). The CODoxidized can be determined by subtracting
granulation and high-rate of pollutant removal (de Sousa Rollemberg the CODbiomass from CODremoved.
et al., 2020). NH3-N transforms to NO2-N, which is finally converted into NO3-N.
The nitrogen mass balance in the AGR can be computed by using Eq. (5)
(Tomar et al., 2022):
4.8.2.5. Hydraulic retention time. The hydraulic retention time (HRT) is
one of the critical design parameters for forming aerobic granules and NH 3 − Nin = [NH 3 − Nout + NO2 − Nout + NO3 − Nout ]
(5)
treating landfill leachate. However, limited studies were conducted on +[Nitrogenbiomass ]
the optimization of HRT during the operation of AGR. Muda et al. (2011)
investigated the influence of different HRTs (6, 12 h, and 24 h) on Nitrogen used for biomass growth (Nitrogenbiomass) can be calculated
characteristics, microbial activities, and kinetic properties of aerobic using Eq. (6) (Tchobanoglous et al., 2003):
granules. This study observed that reducing granular biomass and 0.12VSSwasted
Nitrogenbiomass = (6)
granule size with increasing HRTs is due to the prolonged aeration Q
imparting granules disintegration. Another study with varying HRTs (4,
0.12 is the nitrogen fraction of sludge and Q the leachate flow rate
6, 8, 12, and 16 h) observed similar results, with a stable microbial
(L/d)
community and better performance obtained at 8 h HRT in AGR (Wang
The amount of phosphorus removed (PO4-Premoved) in the AGR can
et al., 2021). In contrast, Liu et al. (2016) reported that granulation is
be determined using Eqs. (7) (Lee et al., 2008):
independent of HRT, although sludge retention time and sludge for­
mation are directly affected by HRT. PO4 − Premoved = (PO4 − Pin ) − (PO4 − Pout ) (7)
where, Q is the leachate flow per cycles (L/cycle), PO4-Pin and PO4-

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Pout are the inlet and oulet concentrations of PO4-P in leachate, biodegradation rate (mg/L h) as shown in Eq. (14).
respectively.
rmax C
r= (14)
Ks + C
4.8.4. Kinetic models
Kinetic studies are essential to determine the factors influencing the where, rmax is the maximum biodegradation rate (mg/L h) and Ks the
reaction rate. The Monod model is widely used to determine the kinetic half-saturation constant (mg/L).
coefficients in various biological reactors besides the correlation be­ At steady sate, the accumulation term dC/dt equals zero. Integrating
tween bacterial growth and limiting substrate concentration. In addi­ Eq. (13) under the given conditions from Ci to Co and solving equations
tion, the changes in COD removal rate in the reactors can be evaluated (13) and (14), resulting Eq. (15) (Saxena et al., 2021):
by using the Monod model. Leachate consists of toxic and recalcitrant
compounds; its COD concentration is also very high, which shows the V/Q
=
Ks 1
+
1
(15)
inhibition effect on microbial growth represented by the substrate Ci − Co rmax Cln rmax
inhibitory models like Haldane. These models and their modified form
can be applied to predict the performance of AGR as well as optimize the where, Ci is the inlet and Co the outlet COD concentrations (mg/L), Cln
process on laboratory scale (Seid-mohammadi et al., 2021). the log mean concentration [(Ci − Co)/ln(Ci/Co)], rmax the maximum
biodegradation rate (mg/L h), and Ks the half-saturation constant (mg/
L). The kinetic coefficients rmax and Ks can be estimated from a plot
4.8.4.1. Monod and Haldane model. The Monod (Eq. (8)) and Haldane
between (1/Cln) and [(V/Q)/(Ci − Co)].
model (Eq. (9)) are usually applied to understand the kinetics of the
degradation of pollutants during leachate treatment. These models can
be simplified as (Wei et al., 2012): 4.9. Integrated process for landfill leachate treatment
dS μ
rs = − = max XS (8) Owing to the high organic strength of landfill leachate, it needs post-
dt Ks + S
treatment in addition to the biological process as it is promising due to
or its operational simplicity and highly cost-effective concerning removal
dS μmax efficiency. Young landfill leachate with a high BOD/COD ratio (0.5–1)
rs = − = XS (9) can be readily biodegradable, providing higher removal efficiency for
dt Ks + S + SK2
i organic and nitrogenous compounds (Miao et al., 2019). However,
where, rs is the substrate degradation rate (mg/L h), S the limiting mature landfill leachate contains a low BOD/COD ratio with high NH3-N
substrate concentration (mg/L), X the biomass concentration (mg/L), concentrations, which causes severe pollution, imparting detrimental
µmax the maximum specific growth rate (1/h); Ks the half-saturation effects to biological processes by reducing the removal efficiency.
constant (mg/L); Ki the inhibition constant (mg/L). When COD is Hence, the biological process solely cannot be efficient, which needs
determined as the total amount of biodegradable organic matter, Ks can other advanced oxidation processes in combination with the biological
be relatively large, resulting in less S value than Ks (Wei et al., 2012). process to enhance the treatment.
Both the Monod model and Haldane model become (Eq. (10)): Integrating ASP and reverse osmosis (RO) efficiently treats landfill
leachate by completely removing COD and NH3-N (Babaei et al., 2021).
dS μmax
rs = = XS = KXS (10) The ASP helps degrade the organic matters present in leachate and af­
dt Ks terward, the leachate enters the RO process to separate the residual
By integrating Eq. (10), it yields: particles present in it (Fig. 5a). In a recent study, integrating reverse
osmosis (RO) with ASP and RBC separately was very efficient for
S = S0 e− KXt
(11) treating landfill leachate (Tałałaj et al., 2019). The ASP followed by RO
Considering that the influent COD of leachate in AGR is composed of successfully removed ~99% of COD and NH3-N. Similarly, the combi­
toxic inhibitors and inert or recalcitrant organic matter (Sn), S and S0 in nation of RBC-RO removed 99% of COD, BOD, and NH3-N. Kargi and
the Eq. (11) can be replaced with (S-Sn) and (S0-Sn), respectively. Eq. Pamukoglu (2003) used pre-treatment for landfill leachate by chemical
(11) is further simplified as: precipitation with lime to reduce the COD and air stripping for ammonia
removal. Subsequently, the final treatment was performed in a fed-batch
S = (S0 − Sn )e− KXt
+ Sn (12) reactor with 76% COD and 23% NH3-N removal at 30 h HRT. A pilot-
Sn in the model gives the biodegradation of landfill leachate and the scale anoxic RBC integrated with an aeration tank was used to treat
final COD concentration remains after the biodegradation. The modified landfill leachate for 88 d, which resulted in the maximum removals of
model considers the biodegradability of landfill leachate and inhibition 85, 99, and 84% for COD, NH3-N, and total nitrogen (TN), respectively
of pollutants and makes it more direct to be utilized. (Song et al., 2020). da Costa et al. (2018) used the solar photo-fenton
process during pre-treatment to enhance the biodegradation of young
4.8.4.2. Modified Monod model. The kinetic coefficients that describe and mature leachate by reducing its toxicity. Nitrogen removal using
the kinetic behavior of AGR can be determined from the steady-state Anammox is an efficient and reliable technique from old and stabilized
outlet concentrations for various inlet concentrations of COD using a landfill leachate, whereas conventional nitrification–denitrification
modified Monod model. The assumptions are oxygen limitation is not processes are preferred for young landfill leachate (Miao et al., 2019).
present in AGR, and at a steady state, the growth rate of the microor­ The effectiveness of coagulation/ultrafiltration (UF) and adsorption/UF
ganism is in equilibrium with its decay rate. Hence, the kinetic co­ as a pre-treatment for stabilized landfill leachate, followed by nano­
efficients were considered to be constant over the period. The kinetic filtration (NF) and RO was studied by Dolar et al. (2016). Coagulation
coefficients can be determined using the plug flow model at steady-state was better than adsorption to remove the COD (65%), TOC (86%), and
using the Eq. (13) (Padhi and Gokhale 2016). turbidity (87%), followed by ultrafiltration, which is primarily used to
reduce the membrane fouling. In the post-treatment using NF-RO, more
dC
= − Q
dC
+r (13) than 80% COD and TOC removal were observed, showing its effective­
dt dv ness for treating landfill leachate. Tałałaj et al. (2021) investigated the
effectiveness of SBR-RO for treating young and stabilized landfill
where, C is the COD concentration (mg/L), Q the flow rate of leachate
leachate. For young landfill leachate, the COD, BOD, and NH3-N
(L/h), t the time (h), V the working volume (L) of AGR, and r the
removal were 97.4, 99.8, and 99.9%, respectively. The removal

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V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

Fig. 5. Integrated process (a) ASP-RO (Babaei et al., 2021) and (b) of AGR-MBR for leachate treatment (Zhang et al., 2021).

efficiencies for both the leachates were almost similar. However, a very leachate. Liébana et al. (2018) used a hybrid reactor by integrating AGR
high NH3-N removal (>99%) was observed using the integrated SBR-RO with MBR to increase the treatment efficiency, which is also energy-
process. Table 6 represents the various integrated process used for efficient and requires a small footprint. Aerobic granules cultivated in
landfill leachate treatment. a MBR along with moving bio-carriers with a 10% filling ratio show the
stability of granules for more than two months (Dai et al., 2020). It has
4.10. Future prospects of AGR been reported that a significant reduction in membrane fouling was
achieved by using AGR as pre-treatment followed by MBRs (Truong
Slow granulation and low granule stability have restricted the et al., 2018). Wang et al. (2020) reported that ferrous-assisted AGR in­
commercial application of AGR (Lin et al., 2020). However, an inte­ tegrated with MBR and RO produced high-grade treated effluent,
grated process enhanced the performance of AGR while treating landfill removing more than 99.9% of dissolved organics, 99.7% of NH3-N, and
leachate (Dai et al., 2020). Very limited research is available for inte­ 100% of total phosphorus. Although integrating AGR with MBR seems
grating AGR with other treatment processes for treating landfill beneficial for achieving desirable effluent quality, the membrane fouling

Table 6
Integrated process for treatment of landfill leachate.
Integrated treatment methods Influent COD concentration COD removal Influent NH3-N concentration NH3-N removal References
(mg/L) efficiency (%) (mg/L) efficiency (%)

SBR-adsorption 3200 43 1800 96 (Babaei et al., 2021)


SBR-RO 2180 96 910 99.9 (Tałałaj et al., 2021)
ASP-RO 1153 99 6440 99 (Luo et al., 2020)
CW-adsorption 2301 86 627 99 (Luo et al., 2020)
RBC-RO 3176 99 884 99 (Tałałaj et al., 2019)
Membrane bioreactor-RO 400–1500 97 200–1400 96 (Tałałaj et al., 2019)
SAMBR-AMBR 1730 96 44 ~100 (Trzcinski & Stuckey
2016)
Trickling filters- 765 53 342 94 (Oumar et al., 2016)
electrocoagulation

SAMBR: Submerged anaerobic membrane bioreactor, AMBR: Aerobic membrane bioreactor.

12
V. Saxena et al. Environmental Nanotechnology, Monitoring & Management 18 (2022) 100689

in MBR remained a major drawback for its further application. The Bassin, J.P., Dezotti, M., 2018. Moving bed biofilm reactor (MBBR). In: Dezotti, M.,
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of about 1–1.2 mm could effectively improve flux and reduce membrane weathering plastics: an exploratory screening study with Nitocra spinipes.
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ing any treatment processes. This study critically reviewed landfill Mercury removal using modified activated carbon of peat soil and coal in simulated
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post-treatment techniques like MBR could be a promising solution by Effect of oxygen concentration on biological nitrification and microbial kinetics in a
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AGR for treating landfill leachate, the full-scale application is still very Rio, A.V., 2019. Does the feeding strategy enhance the aerobic granular sludge
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CRediT authorship contribution statement Çeçen, F., Aktaş, Ö., 2004. Aerobic co-treatment of landfill leachate with domestic
wastewater. Environ. Eng. Sci. 21 (3), 303–312.
Vikalp Saxena: Data curation, Formal analysis, Writing-original Çeçen, F., Gürsoy, G., 2001. Biosorption of heavy metals from landfill leachate onto
activated sludge. J. Environ. Sci. Health A 36 (6), 987–998.
draft. Susant Kumar Padhi: Conceptualization, Supervision, Valida­
Cema, G., Wiszniowski, J., Żabczyński, S., Zabłocka-Godlewska, E., Raszka, A., Surmacz-
tion, Visualization, Writing-review & editing. Pritam Kumar Dikshit: Górska, J., 2007. Biological nitrogen removal from landfill leachate by
Visualization, Writing-review & editing. Lopa Pattanaik: Writing- deammonification assisted by heterotrophic denitrification in a rotating biological
review & editing. contactor (RBC). Water Sci. Technol. 55, 35–42.
Chen, S., Sun, D., Chung, J.S., 2008. Simultaneous removal of COD and ammonium from
landfill leachate using an anaerobic–aerobic moving-bed biofilm reactor system.
Declaration of Competing Interest Waste Manage. 28, 339–346.
Chen, W.H., Tsai, C.Y., Chen, S.Y., Sung, S., Lin, J.G., 2019. Treatment of campus
domestic wastewater using ambient-temperature anaerobic fluidized membrane
The authors declare that they have no known competing financial bioreactors with zeolites as carriers. Int. Biodeterior. Biodegrad. 136, 49–54.
interests or personal relationships that could have appeared to influence Chen, Y., Jiang, W., Liang, D.T., Tay, J.H., 2007. Structure and stability of aerobic
granules cultivated under different shear force in sequencing batch reactors. Appl.
the work reported in this paper. Microbiol. Biotechnol. 76, 1199–1208.
Cheng, W., Quan, X., Huang, X., Cheng, C., Yang, L., Cheng, Z., 2018. Enhancement of
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