DSpace at VNU: Application of a partial nitritation and anammox system for the old landfill leachate treatment

A lab-scale experiment including partial nitritation using a sequencing batch reactor PN-SBR followed by a anammox hybrid reactor HAR, which consists of suspended biomass layer in the bo

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Application of a partial nitritation and anammox system for the old

Phan The Nhata, Ha Nhu Bieca, Nguyen Thi Tuyet Maia, Bui Xuan Thanhb,*,

a Faculty of Environment and Natural Resources, Ho Chi Minh City University of Technology, Building B9, 268 Ly Thuong Kiet Street, District 10,

Ho Chi Minh City, Viet Nam

b Division of Environmental Engineering and Management, Ton Duc Thang University, No 19 Nguyen Huu Tho Street, Tan Phong Ward, District 7,

Ho Chi Minh City, Viet Nam

a r t i c l e i n f o

Article history:

Received 15 January 2014

Received in revised form

29 May 2014

Accepted 30 May 2014

Available online xxx

Keywords:

Partial nitritation

Old landﬁll leachate

SBR and hybrid anammox reactor

a b s t r a c t

This study shows high nitrogen removal efficiency of a combination of partial nitritation and Anaerobic Ammonium Oxidation (anammox) process for old landfill leachate treatment A lab-scale experiment including partial nitritation using a sequencing batch reactor (PN-SBR) followed by a anammox hybrid reactor (HAR), which consists of suspended biomass layer in the bottom part and bio-carrier bed in the upper part run at the influent total ammonia concentrations (TAN) of 500 mg N/L and 1000 mg N/L The result of PN-SBR experiment showed that the NO2eN:NH4eN ratio achieved about 1.22 and 1.02 at HRT

of 12 h (influent TAN of 500 mg N/L) and HRT of 19 h (influent TAN of 1000 mg N/L), respectively Simultaneously, the HAR was operated at the nitrogen loading rate (NLR) of 4.2 and 8.3 kg N/m3.d, corresponding to influent TAN of 500 mg N/L and 1000 mg N/L, respectively The effluent of the system containing 9.7 ± 3.5 mg NH4eN/L, 1.7 ± 0.4 mg NO2eN/L and 23 ± 4 mg NO3eN/L (equivalent to

35± 4 mg TN/L) at NLR of 1.02 for PN-SBR and NLR of 4.2 kg N/m3.d for HAR This efﬂuent quality was good enough to meet Vietnamese treated landﬁll leachate quality The system obtained TN removals of

93 ± 1% and 81 ± 1.2% at NLRs of 4.2 kg TN/m3.d (phase I) and 8.3 kg TN/m3.d (phase II), respectively The total biomass of HAR including attached biomass and suspended one was maintained up to 20,400 mgVSS/L at the end of the experiment when the removal rate of anamnox biomass obtained 0.4 kg TN/kgVSS.d While, PN-SBR was kept at 2300 mg MLVSS/L and SRT of 10e12 days at NLR of 4.2 kg TN/m3.d, which the nitrogen conversion rate of AOB was 0.53 kg TAN/kgVSS.d In terms of COD removal, it is found that PN-SBR removed only 14% of inﬂuent COD, whereas HAR removed 30% of COD

1 Introduction

Sanitary landﬁll is the most common municipal solid waste

disposal in Vietnam Leachate generated from the landﬁlls has

caused serious water pollution due to high concentrations of

ammonia and slowly or non-biodegradable organic matter High

total ammonia concentration (TAN) results in high toxicity by free

ammonia which inhibits anaerobic degradation of solid wastes and

increases dissolved oxygen depletion in the receiving water The

ammonia concentration in the leachate varies with the age of the

landﬁll and it is in the range of 100e5500 mg N/L (Sri Shalini and

Joseph, 2012) In Vietnam, all leachate treatment plants have not

met the leachate quality standards (QCVN 25:2009/BTNMT) in

terms of the allowable ammonia (25 mgN/L) and total nitrogen concentrations (60 mg N/L) (Monre, 2009) In Vietnam, the current leachate treatment plants use mainly the conventional nitrification-denitrification process, which is costly due to large oxygen supply demand for nitrification and carbon source requirement for denitrification In recent years, a partial nitritation coupled with anammox process have proven as a feasible tech-nology for nitrogen removal in comparison to the conventional nitrificationedenitrification process (Van Dongen, 2001; Fux et al., 2002; Schmidt et al., 2003) This process consumed less 50% of oxygen demand, did not use organic carbon sources, produced less sludge amount and less CO2emission (Reginatto et al., 2005) The arrangement of partial nitritation and anammox processes was done in single reactors or in two separate reactors in series The two-step process is recommended to avoid heterotrophic growth in the anammox reactor as well as to enhance the NH4eN removal in the case of high influent TKN concentration (Van Hulle et al., 2007)

* Corresponding author.

E-mail addresses: phanthenhat@gmail.com (P.T Nhat), bxthanh@tdt.edu.vn ,

bxthanh@hcmut.edu.vn (B.X Thanh), npdan@hcmut.edu.vn (N.P Dan).

Contents lists available atScienceDirect

International Biodeterioration & Biodegradation

j o u r n a l h o m e p a g e : w w w e l s e v i e r c o m / l o c a t e / i b i o d

http://dx.doi.org/10.1016/j.ibiod.2014.05.025

International Biodeterioration & Biodegradation xxx (2014) 1e7

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Some studies shown application of partial nitritation and anammox

processes for leachate treatment were potential control for

nitro-gen removal (Liang and Liu, 2007; Xiao et al., 2009; Xu et al., 2010;

Yapsakli et al., 2011) However, these processes only run at low

nitrogen loading rates in the previous studies and it ranged from

0.17 to 0.96 kg N/m3.d (Liang and Liu, 2008; Xu et al., 2010;

Rucalleda, 2011; Wang et al., 2011) Therefore, this study aimed to

evaluate the feasibility of the partial nitritation followed by

anammox process at high nitrogen loading rates for the old landﬁll

leachate treatment A partial nitritation SBR and a hybrid anammox

reactor were used in this study

2 Materials and methods

2.1 Feed leachate

Landﬁll leachate used in the study was collected from Go Cat

municipal solid waste landﬁll in Ho Chi Minh city, Vietnam, which

was closed in 2007 Its characteristics are shown inTable 1.Table 1

indicates that the typical characteristics of old landﬁll leachate

contained high NH4eN concentration and low BOD5:COD ratio

(Kjeldsen et al., 2002)

Feed leachate was diluted with tap water to obtain the inﬂuent

ammonia concentration ranging from 500 to 1000 mg N/L

2.2 Experimental set-up and operational conditions

2.2.1 Experimental set-up

A lab-scale partial nitritation-anammox system including a

PN-SBR followed by HAR was used in this study The schematic diagram

is shown in Fig 1 The PN-SBR is a cylindrical reactor with the working volume of 66.5 L Its size is 0.6 m high and 0.42 m in in-ternal diameter Air was supplied from the bottom of the PN-SBR through five air diffusors, and the air flow was adjusted by a manual valve to maintain the DO concentration higher than 3 mg/L The diluted feed raw leachate stored in 300 L tank, was pumped to the PN-SBR A mechanical stirrer at 30 rpm was used to enhance the complete mixing with aeration The supernatant decanted from PN-SBR was stored in a container with volume of 90 L, and then it was pumped to the HAR The HAR was made of acrylic tube with an internal diameter of 114 mm and the ratio of height to diameter is 5.7 Its working volume was 5 L The HAR comprised suspended biomass layer located in the bottom part, a spiral structure column that was made from stainless steel in the middle part and afixed bio-carrier bed in the upper part The spiral column consisted of 7 pitches to separate the nitrogen air from anammox sludge The distance between pitches was 4 cm, the length of whole spiral column was 28 cm Slope of each pitch was 300 The biomass carrier consisted of 8 polyester non-woven porous sheets, which have a total one-sided area of 1116 cm2, thickness of 0.5 cm and height of

31 cm (Japan Vilene, US patent 5,185,415, 1993) This carrier was designed to enhance biomass attachment and to prevent the wash-out of biomass from the reactor A gas collector was installed at top

of HAR

2.2.2 Enrichment of sludge 2.2.2.1 AOB sludge The seed sludge was activated sludge from an aeration tank of the Go Cat leachate treatment plant An enrich-ment of AOB was conducted in PN-SBR 546 g TSS of the seed sludge was seeded into the reactor to obtain VSS concentration of

1500 mg/L The ratio of VSS and TSS was 0.25 AOB sludge was enriched using the leachate diluted with tap water to achieve

NH4eN concentration of 500 mg N/L The PN-SBR run at DO higher than 3 mg/L and HRT of 21 h for 45 days Enrichment of AOB was completed until the conversion efﬁciency of NH4eN to NO2eN reached more than 90% The efﬂuent NO2eN and NO3eN concen-tration after enrichment were 486 mg N/L and 15 mg N/L, respectively

2.2.2.2 Anammox sludge The HAR was inoculated with 9 g MLVSS

of anammox sludge, which was taken from the current polyester non-woven carrier reactor (PNBCR) (Nhat et al., 2012) The

Table 1

Characteristics of old landﬁll leachate in the study.

(1)Influent pump; (2) feed raw leachate tank; (3) stirrer; (4) air pump; (5) gas collector;

(6) polyester non-wovenbiomasscarrier; (7)spiral column and (8) suspended anammox blanket

PN-SBR (a)

HAR (b)

3 4 Influent

2

Supernatant tank ( 90 L)

Effluent

6

8

Sludge

7 5

Fig 1 Schematic diagram of the lab-scale PN-SBR and HAR system.

P.T Nhat et al / International Biodeterioration & Biodegradation xxx (2014) 1e7 2

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dominant bacterial species in the consortium was identiﬁed as the

anammox Candidatus Kuenenia stuttgartiensis and uncultured anoxic

sludge bacterium KU2 (Nhat et al., 2012) The enriched anammox

biomass was adapted with synthetic wastewater (NH4Cl 215 mg N/

L, NaNO2248 mg N/L, KHCO3125 mg/L, KH2PO454 mg/L) Trace

element solutions were added based on the previous studies (Van

de Graff et al., 1996) The HAR run at the nitrogen loading rate of

8 kg N/m3/d during the enrichment of 60 days The enrichment was

completed when the nitrogen the TN removal efﬁciency was above

90%, corresponding to the obtained removal rate (NRR) of 7.2 kg N/

m3/d Then, the inﬂuent of HAR was switched to the efﬂuent of

PN-SBR fed with the real leachate

2.2.3 Operational conditions

2.2.3.1 Partial nitritation-Sequencing batch reactor (PN-SBR)

PN-SBR was operated with 10 min of feed, 45 min of settle and

5 min of decant The adjustment of the aerobic reaction time of

reactor depended on the efﬂuent NO2-eN to NH4 þ-N ratio HRT was

determined by the aerobic reaction time, total cycle time and

vol-ume exchange ratio pH of the inﬂuent was controlled at 7.5 ± 0.2

by adding HCl 20% solution DO in the reactor was maintained

higher than 3 mg/L The study was operated at the inﬂuent total

ammonia concentration (inﬂuent TAN) of 500 and 1000 mg N/L

The study aimed to determine a proper HRT of reactor at every

inﬂuent TAN concentration in order to obtain the suitable NO2-eN

to NH4þeN ratio for anammox process Operational conditions were

presented inTable 2

2.2.3.2 Hybrid anammox reactor (HAR) The experiment was run

under dark condition by using a black plastic sheet enclosing fully

the reactor body to prevent algal growth Na2SO3salt was added

into PN-SBR efﬂuent tank to reduce DO less than 0.5 mg/L Amount

of 20 mg Na2SO3was used to reduce about 1 mg DO Inﬂuent pH was adjusted in the range of 6.8e7.1 by HCl 20% solution Opera-tional conditions of the experiment show inTable 2

2.3 Analytical methods

pH and DO were measured by using pH meter (HI 8314, Hanna) and DO meter (InoLab 740 with terminal 740 WTW, Germany), respectively Total suspended solids (TSS), volatile suspended solids (VSS), COD, NH4eN, NO2eN and NO3eN and alkalinity were measured according to Standard Methods for examination of Water and Wastewater (APHA, 1998) Sample ﬁltration was done using Whatmanﬁlter papers with pore size of 0.45mm

3 Results and discussion

3.1 Partial nitritation SBR (PN-SBR) After 45 days of enrichment, NH4eN was converted to NO2eN over 90% at the inﬂuent NH4eN concentration of 500 mg N/L and HRT of 21 h To get suitable inﬂuent for anammox process, the partial nitritation should be run to reach to the stoichiometric

NO2eN:NH4eN ratio of 1.32 HRT of SBR was adjusted at values less than 21 h (19 h, 15 h and 12 h) At HRT of 19 h, NO2eN: NH4eN ratio was still high (2.75± 0.87, n ¼ 4) under steady-state condition At the loading rate of 0.7 kg TAN/m3.d, the mean efﬂuent TAN and

NO2eN concentrations were 142 ± 35 mg N/L and 370 ± 28 mg N/L, respectively The ratio decreased to 1.53± 0.05 (n ¼ 6) at HRT of

15 h (NLR of 0.8 kg TAN/m3.d) The steady state condition reached after 03 days of running at HRT of 12 h The obtained NO2eN:

NH4eN ratio was 1.22 ± 0.1 (n ¼ 5) that was close to the stoichio-metric ratio for anammox process The mean efﬂuent TAN and

NO2eN concentrations were 224 ± 9 and 274 ± 14 mg N/L, respectively In this phase, the efﬂuent NO3eN concentration was low (15± 2 mg N/L), equivalent to 3% of inﬂuent TAN It means that the partial nitritation which run at long HRT (15 h) and at NLR of 1.0 kg TAN/m3.d did not exist nitrate accumulation

In phase II, the inﬂuent TAN concentration was increased to

1000 mg N/L From 45th to 54th day, the NO2eN: NH4eN ratio was low 0.67± 0.02 (n ¼ 4) at HRT 19 h (Fig 2) It may be due to the short HRT (19 h) coupled with high NLR (1.3 kg TAN/m3.d) that AOB were not able to convert 50% of TAN to nitrite As HRT increased up

Table 2

Operational conditions of PN-SBR and HAR system.

Phase Time (days) The inﬂuent TAN

concentration (mg N/L)

HRT (h) TAN loading rate

(kg/m 3 d) PN-SBR HAR PN-SBR HAR

15 12

0.8 1.0

4.2

21

1.2

8.3

2.75

1.53

1.22

1.02

0.67 0.0 1.0 2.0 3.0 4.0

0 200 400 600 800 1000 1200

Eff N-NO3 Eff NH4:NO2 ratio Stoichiometrical ratio

Fig 2 Conversion of TAN and the efﬂuent NO2eN to NH4eN ratio at the various HRTs in the PN-SBR experiment.

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to 21 h at NLR of 1.2 kg TAN/m3.d, NO2eN: NH4eN ratio of

1.02± 0.18 (n ¼ 12) was obtained The efﬂuent TAN and NO2eN

concentrations were 469 ± 58 mg N/L and 516 ± 40 mg N/L,

respectively The efﬂuent NO3eN concentration was low (20 ± 7)

mg N/L The result of this study was similar to that of Taichi

Yamamoto et al (2008), who used successfully partial nitritation

reactor for swine wastewater digester liquor at TAN loading rate of

1.0 kg N/m3.d

With the above result, it is expected that PN-SBR may run

effectively at higher inﬂuent TAN concentration at longer HRT and

at NLR which should be kept by 1.2 kg TAN/m3.d However, increase

of inﬂuent TAN concentration may result in rise of free ammonia

(FA) in SBR as well as rise of alkalinity demand as carbon sources for

AOB Some previous studies claimed that nitritation process

running at the NLRs over 1 kg TAN/m3.d was inhibited AOB growth

at FA concentration of about 150 mg N/L (Anthonisen et al., 1976;

Kurniawan et al., 2006; Ganigue et al., 2012) In this study, the

average FA concentration in the PN-SBR was less than 20 mg N/L

that did not inhibited AOB

Table 3shows the biomass concentration and sludge retention time in both phases At NLR of 1.22 kg TAN/m3.d, the nitrogen conversion rate of AOB was 0.53 kg TAN/kg MLVSS.d It is found that scum happened in Phase I (SRT of 20 days), whereas it insigni ﬁ-cantly occurred in Phase II The average efﬂuent SS after 45 min of settling was 19± 5 mg/L that shown a good settling ability of AOB at SRT of 12 days

3.2 Hybrid anammox reactor (HAR)

In enrichment, the HAR was run with the synthetic wastewater

at 8.0 kg TN/m3.d After two months, the obtained TN removal rate was 7.9 kg TN/m3/d The HAR was then run with the efﬂuent from PN-SBR High nitrogen removal rate (3.6 kg TN/m3/d) was obtained

at NLR of 4.0 kg TN/m3.d after 45 days of run This presented that the components of the leachate with TN of 500 mg N/L from PN-SBR did not cause negative impact on anammox bacteria.Fig 3a,b shows the time courses of TN (TANþ NO2eN) removal efﬁciency and TN removal rate of the HAR during 90 days of experiment The obtained TN removals were 93 ± 1% and 81 ± 1.2% at NLRs of 4.3 kg TN/m3.d (phase I) and 8.3 kg TN/m3.d (phase II), respectively

At NLR of 4.0 kg N/m3.d, the efﬂuent TAN, NO2eN, and NO3eN of HAR were 9.7± 3.5 mg N/L, 1.7 ± 0.4 mg N/L and 23 ± 4 mg N/L, respectively This efﬂuent quality was good enough to meet QCVN 25:2009/BTNMT

At NLR of 8.3 kg N/m3.d (HRT of 3 h and inﬂuent TN concen-tration of 1000 mg N/L), the efﬂuent TAN, NO2eN, NO3eN and TN

Table 3

Biomass concentration and sludge retention time in the experiment.

Phase SRT, days SS, mg/L MLSS, mg/L MLVSS, mg/L SVI, mL/g VSS

(n ¼ 6)

7712 ± 750 (n ¼ 6)

3479 ± 244 (n ¼ 6)

34 ± 2 (n ¼ 6)

II 10e12 days 19 ± 5

(n ¼ 13)

5583 ± 570 (n ¼ 7)

2298 ± 133 (n ¼ 7)

43 ± 4 (n ¼ 7)

(a)

(b)

0.0 2.0 4.0 6.0 8.0 10.0

3.day

0 200 400 600 800 1000 1200

Operating time (day)

Eff NO3 (HAR)

Fig 3 Time courses of the whole system: (a) Nitrogen loading rate (NLR) and nitrogen removal rate (NRR); (b) Nitrogen concentration.

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concentrations were 76± 11 mg N/L, 80 ± 9 mg N/L, 39 ± 5 mg N/L

and 196± 12 mg N/L, respectively This efﬂuent quality was not met

threshold values of the leachate quality standards It is expected

that the efﬂuent nitrogen concentration may reach the QCVN

25:2009/BTNMT as the HAR is run at lower NLR, corresponding to

longer HRT

The produced NO3eN was about 10% of inﬂuent TN in anammox

process (Furukawa et al., 2009) In the anammox process, the

stoichiometric ratio of NH4eN and NO2eN consumption and the

NO3eN production (molar NH4:NO2:NO3 ratio) is 1:1.32:0.26

(Strous et al., 1998) The obtained molar NH4:NO2:NO3ratios in this

study were 1:1.27:0.03 at phase 1and 1:1.13:0.05 at phase 2 The

different ratios were reported by some previous researches on

leachate treatment The study ofRuscalleda (2011)andLiang and

Liu (2008)presented the ratio of 1: 1:42: 0:15 and 1:1.09: 0.007,

respectively The signiﬁcant difference between the obtained ratios

in this study and the stoichiometric value is nitrate production This

may be due to the presence of heterotrophic denitrifying bacteria in

the HAR Indeed, nitrate reduction coupled with COD removal was

found during all the operational periods

Liang and Liu (2008)who used an up-ﬂow ﬁxed bed annamox

bioﬁlm reactor for old landﬁll leachate treatment shown that the

obtained NRR was 0.2 kg N/m3.d at TN concentrations of

1000e1500 mg N/L The research ofFurukawa et al (2009)got NRR

of 4.2 kg N/m3.d for a PEG gel carrier anammox reactor used to treat

anaerobic swine wastewater digester liquor at NLR of 5.3 kg N/m3.d

In comparison with the above researches, an extremely high NRR

(7.3 kg N/m3.d) at NLR of 8.3 kg N/m3.d was achieved in this study

Biomass concentration increased from 9000 mg/L at the beginning of enrichment to 28,960 ± 980 mg MLSS/L and 20,400 ± 1000 mg MLVSS/L at the end of the experiment The maximum total nitrogen removal rate of anamnox biomass was 0.4 kg TN/kgVSS.d The average efﬂuent SS during the phase II was

10± 6 mg/L This presents the sludge wash-out was not remarkably during the experiment It is explained that the combination be-tween suspended growth using a spiral column and the bio-carrier enhanced the sludge wash-out

Figs 4a and b presents the TAN conversion of PN-SBR, HAR and

TN removal of the whole system The ammonia removal of the overall system depended much on ammonia conversion of PN-SBR

In phase I, the ammonia removal of 99± 1% in the overall system was achieved when conversion of NH4eN of PN-SBR was 61 ± 8% Whereas, in phase II, the ammonia removal (91± 3%) and conver-sion to nitrite (49± 6%) of the whole system were little bit lower

Fig 4b shows that the TN removal efﬁciency was 85 ± 7% and

81± 1% in Phase I and Phase II, respectively The highest TN removal

of the whole system was reached at the end of the phase I when the molar NH4:NO2 ratio of PN-SBR was 1.22 Thus, control of molar

NH4:NO2 ratio of PN-SBR is very important to aim to high TN removal efﬁciency of the overall system

3.2.1 COD Removal

Fig 5shows the removal of COD of overall system during 100 days of experiment The COD removal efﬁciency of overall system in phase I and II were 50± 3% and 46 ± 12%, respectively The COD removal by PN-SBR was low, it was only 18± 4% in phase I and

(a)

(b)

0 10 20 30 40 50 60 70 80 90 100

Operation time (day)

50 55 60 65 70 75 80 85 90 95 100

Operating time (day)

Fig 4 Time course of nitrogen removal of PN-SBR and HAR system experiment: (a) Ammonia; (b) TN (TAN þ NO2 - eN þ NO3 - eN).

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12± 5% in phase II It is due to low ratio of BOD5to COD in the raw

leachate (around 0.1) The average BOD5of leachate (425± 72 mg

BOD5/L) was 12% of total COD BOD5 content was completely

removed in the PN-SBR The result is similar to that of the study of

Wang et al (2014)which presented the low COD removal (30%) and

high BOD5removal (80%) in the PN-SBR

The COD removal of the HAR ranged from 14 to 46%, whereas

biodegradable COD were fully removed in the PN-SBR Similarly,

Liang and Liu (2008)reported that old landﬁll leachate treatment

using anammox reactor obtained COD removal of 23e41% Bacterial

community of the HAR may remove refractory organics such as

fulvic-like compounds from the PN-SBR efﬂuent Denitrifying

bac-teria could not directly use aquatic humic substance (AHS) in the

leachate.Liang and Liu (2008)indicated that some kinds of

het-erotrophs living in community of annamox biomass were able to

degrade AHS into readily biodegradable organic matters which

were then utilized by denitriﬁer living in the community

4 Conclusions

The system including a PN-SBR followed by a HAR was able to

remove efﬁciently total nitrogen from the old landﬁll leachate The

efﬂuent quality was met the Vietnamese leachate quality

stan-dards at NLR of 1.0 kg TAN/m3/d for PN-SBR and 4.0 kg TN/m3.d for

HAR The HAR obtained the extremely high NRR of 7.3 kg TN/m3/

day at NLR of 8.3 kg TN/m3/day The achievement of molar

NH4:NO2ratio of 1.2e1.4 for PN-SBR helped to enhance TN rem

oval efﬁciency of the overall system Bacterial community of HAR

was able to degrade slowly biodegradable or non-biodegradable

COD

Acknowledgments

The Authors gratefully thank to Vietnam Brewery Ltd Company

forﬁnancial support of this study

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0 200 400 600 800 1000 1200

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Time course (day)

Fig 5 Removal of COD in the PN-SBR and HAR system.

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