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Hydrogen sulfide generation and emission in urban sanitary sewer in China:


What factor plays the critical role?

Article  in  Environmental Science: Water Research & Technology · March 2019


DOI: 10.1039/C8EW00617B

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Hydrogen sulfide generation and emission in


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Cite this: DOI: 10.1039/c8ew00617b


urban sanitary sewer in China: what factor plays
the critical role?†
Zhiqiang Zuo, a Jian Chang,d Zhengsheng Lu,a Moran Wang,a Yucong Lin,b
Min Zheng, ae David Z. Zhu,c Tong Yu,c Xia Huang a and Yanchen Liu *a

Identifying hydrogen sulfide (H2S) hotspots is critical for preventing/controlling odor and corrosion prob-
lems in sewer systems. However, relatively little is known regarding H2S hotspots and variation characteris-
tics in China's urban sewer networks. A comprehensive field investigation was carried out on the impacts
of sewer structures, season, water flow and wastewater quality on H2S emission. The results indicated that
H2S diurnal variation mainly followed the dry weather flow fluctuation in gravity sewer networks. The man-
hole downstream of septic tanks was identified as a H2S emission hotspot due to potential significant sul-
Received 4th September 2018, fide generation in the septic tanks. The effect of temperature on H2S emission was related to variations in
Accepted 15th March 2019
the sulfide production rate and flow turbulence at different locations in the sewer system. Significant re-
duction in sulfide concentration was observed with rainfall-derived high water flow rate. The local water
DOI: 10.1039/c8ew00617b
quality was identified as a key factor for sulfide generation from different sites along the sewer system.
rsc.li/es-water These findings are useful in understanding and predicting H2S emission in China's sewer systems.

Water impact
Hydrogen sulfide (H2S) generated in the sanitary sewer system is harmful to public health and the environment, yet little is known about H2S emission
characteristics in China's urban sewer network. In the study, a comprehensive field investigation, including impacts of sewer structure, temperature, water
flow and wastewater quality was carried out. The findings of this study will be useful in understanding H2S emission in China's sewer systems.

1. Introduction in 2009.2 On the other hand, H2S is toxic to humans and seri-
ously endangers sewage workers' lives3 and has a significant
Hydrogen sulfide (H2S) generated in sanitary sewer systems adverse impact on nearby residents.4
is harmful to public health and the environment due to its Sewer development in China has received more attention
corrosive effect, odour nuisance and toxicity. Sewer corrosion in recent years, e.g., the investment in sewer construction
is caused by sulfuric acid (H2SO4) oxidized from H2S reached $36.7 billion, accounting for more than 50% of the
adsorbed on moisture pipe walls, which creates significant total investment in the infrastructure construction program
challenges to infrastructure management,1 e.g., the US na- of municipal wastewater treatment, reclamation, and reuse
tional sewer rehabilitation was estimated to cost $3.2 billion during the period of 2010–2015.5 More than 75% of the Chi-
nese sewer systems was constructed in the past 20 years.6
a
State Key Joint Laboratory of Environment Simulation and Pollution Control, However, more and more young sewer pipelines are likely fac-
School of Environment, Tsinghua University, Beijing 100084, China. ing the risk of H2S-related pipe damage. Hvitved-Jacobsen
E-mail: liuyc@mail.tsinghua.edu.cn; Tel: +86 10 62796953
b
et al.7 reported that a sulfide concentration within the range
Center for Statistical Science and Department of Industrial Engineering,
Tsinghua University, Beijing 100084, China
of 0.1–0.5 mg S L−1 triggers minor problems of concrete cor-
c
Dept. of Civil and Environmental Engineering, Univ. of Alberta, Edmonton, AB, rosion, while sulfide concentrations higher than 2.0 mg S L−1
T6G 2W2 Canada result in severe concrete corrosion. It has been reported that
d
Beijing Municipal Engineering Design and Research Institute, Beijing, 100082, the lifespan of a sewer pipe can be significantly shortened
China
e
due to concrete corrosion rate ranging between 1.1–10 mm
Advanced Water Management Centre, the University of Queensland, QLD,
Australia
per year.8 Thus, it is imperative to conduct H2S prevention
† Electronic supplementary information (ESI) available. See DOI: 10.1039/ strategies immediately in the H2S hotspot in order to prolong
c8ew00617b sewer pipe lifetime. Unfortunately, the H2S hotspot is largely

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unidentifiable in sewer systems, which has caused many H2S ation and emission of a typical urban sewer system in China.
poisoning incidents over the past years in China.9 In order to A comprehensive sewer investigation was conducted in Yixing
minimise sewer corrosion and reduce health risk, it is impor- city in south-east China, which included the impacts of sewer
tant to understand the characteristics of H2S variation in the structure, season, water flow and wastewater quality on H2S
sewer system. emission. The findings of this study will be useful in under-
Extensive studies aiming for H2S prediction and control in standing H2S emission in China's sewer systems.
sewer networks have been done over the past years in some
developed countries.8,10–13 The understanding of sewer pro- 2. Materials and methods
cesses and mechanisms has been improved in China, but the
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management and maintenance of the sewer system is less de- 2.1 Field sewer description
veloped due to lack of applicability and experiences.9 While The field study was conducted in four typical regionally sepa-
septic tanks commonly serve as terminal treatment facilities rated sewer systems, which were located in a Yixing city,
in many places, in China, septic tanks are ubiquitous in ur- Jiangsu province. As shown in Fig. 1, sewer system (a)
ban neighbourhoods. It normally takes the function of anaer- contained a pressure main #1a to #1 connected to a gravity
obic digestion of wastewater treatment before discharging main #1 to #7. The gravity trunk line was 2.8 km long and
into main pipe,14 yet little remains known about the impact had 7 manholes, of which #3, #5 and #7 manholes connected
of septic tank on H2S generation and emission. Overall, the with lateral pipes collecting sewage from nearby neighbor-
complex and particular sewer characteristics in China would hoods (area 1, 2 and 3). In these neighborhoods, septic tanks
significantly increase the difficulty of identifying H2S such as #3c and #5c were used in sewer systems for treating
hotspots in the sewer network. wastewater before discharging sewage into the main pipe.
The sewer network in China requires improvement in its The size of the septic tank was approx. 2.5 m (L) × 1.8 m (W)
overall performance as soon as possible. For that reason, rele- × 1.1 m (H), and its retention time was about 1 hour. The di-
vant studies about sewer networks have been focused on sev- ameters of the sewer gravity pipe line and branch pipe line
eral sewer problems such as illicit connection,15–17 water in- were 800 mm and 300 mm, respectively. Sewer system (b)
filtration18,19 or pipe rehabilitation technologies.20–22 showed the other gravity sewer system (#8–#10), which
However, very few studies have been done to assess the H2S connected with two lateral pipes. These two sewer systems (a)
problem in China's sewer network, which has been largely and (b) were separated and connected to different sewage
neglected by authorities and the general public. The main ob- treatment plants. In the meantime, H2S measurement was
jective of this paper is to reveal the critical role in H2S gener- also conducted in the selected two other pressure main

Fig. 1 Map of the studied sanitary sewer system. Map (a) included a pressure main connecting with a gravity sewer system, map (b) showed a gravity
system and map (c and d) showed two pressure mains, respectively. These four sewer systems were separated and connected to different WWTPs.

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systems (c) and (d). The detailed information regarding pipe 2.4 Data statistical analysis
diameter, length, slope, pipe material and water flow are In order to analyze the relationship between wastewater qual-
shown in Table 1 and Fig. 2. ity and sulfide generation, the linear regression is a useful
method to reveal relationships between explanatory variables
2.2 Field program and the response variable. The formula is:

A field survey of H2S distribution in various sewer parts was y = β0 + β1X1 + β2X2 + β3X3 + ⋯βKXK (1)
conducted first. The gaseous H2S was measured with the
OdaLog® H2S gas sensors (Modal OdaLog type L2, manufac- where y is the sulfide concentration and X is the explanatory
Published on 22 March 2019. Downloaded by University of Queensland on 4/4/2019 7:46:37 AM.

ture) in all the manholes of four sewers. The H2S gas sensors variable, including sulfate, COD, velocity, conductivity, pH
were installed 1 m under the manhole cover and automati- and ORP in the study. β0 is the intercept term and βi is the
cally collected and stored data at 5 min intervals for at least linear slope of Xi, which are the estimated parameters in the
24 consecutive hours. regression equation.
Further, the impacts of several important factors, includ- A stepwise regression is used to select explanatory variables
ing sewer structure, temperature, water flow and wastewater based on the Akaike information criterion (AIC). The selected
quality, on H2S generation and emission were evaluated (seen variables are shown to be significantly helpful for decreasing
in Table 2). H2S and water quality measurement along a pipe- the AIC based on bidirectional elimination, which will better
line with a septic tank was carried out in a gravity sewer sys- fit the data when the selected variables are relatively small.
tem. The H2S diurnal variation was monitored along two Further, multi-collinearity, which means that the independent
pipelines (#3a–#3 and #5a–#5) with septic tanks in different assumption in the regression model is broken with two explan-
seasons. Wastewater samples were collected from these man- atory variables showing strong correlation, is generally
holes using a 5 L bucket and immediately transported to the concerned in linear regression models. The variance inflation
laboratory for chemical analysis. Further, the effect of water factor (VIF) is calculated to verify whether there is multi-
flow on H2S emission was investigated in the #3a and #7 collinearity between variables. The VIF of Xi equals:
manhole and H2S in the manhole was detected. A rain gauge
was installed for monitoring rainfall in the field. Finally, the 1
VIFi  (2)
long-term effect of wastewater quality on H2S and sulfides 1  Ri 2
was investigated. The study selected #8a and #9a manholes
in the sewer system (b) to conduct H2S and water quality where Ri2 equals the coefficient of determination of the regres-
measurement for 10 days. H2S was detected and wastewater sions. The explained variable (y) is Xi and explanatory variables
samples were collected from these two manholes every two are X1, X2…Xi−1, Xi+1…Xp. With VIFi higher than 10, Xi has sig-
hours and analyzed in the laboratory. Wastewater velocity, nificant multi-collinearity with other explanatory variables.
pH, electrical conductivity and ORP were measured using pH
gauge (Mettler FE20), ORP gauge (LE501) and electrical con-
ductivity gauge (FE 30 K). 3. Results and discussion
3.1 H2S distribution in typical structure units along the
2.3 Chemical analysis sewer-shed
Measurement of COD, sCOD, sulfate, sulfide, ammonium The H2S concentrations at different sewer locations are
and phosphate concentration were performed in accordance shown in Fig. 3. It was clear that two H2S hotspots could
with standard methods.23 Volatile fatty acids (VFAs) were ana- be identified, consisting of the outlet of the pressure mains
lyzed using Agilent 6890N gas chromatograph (GC). (#1, #11 and #12) and the downstream manholes (#3, #5
and #7) of the septic tanks in the neighborhoods, where
the concentration of H2S could reach up to 100–400 ppm.
Table 1 The parameters of sewer pipes in the field experiment
It was no surprise that the outlets of the pressure mains
Pipe Length Diameter Slope Flow Pipe were the H2S hotspots in sewers because it was well known
number (m) (m) (m m−1) (m s−1) material that the biofilm in the pressure main was the source of
Pressure main pipe sulfide production.24 In this study, the manholes down-
1a–1 1000 0.5 −0.004 0–0.35 Ductile iron stream of the septic tanks were first found to be H2S
11a–11 5500 0.4 −0.001 0–0.5 Ductile iron hotspots. Most of the other sewer manholes were not sig-
12a–12 1000 0.5 −0.003 0.6–1.8 Ductile iron
Gravity main pipe nificant sources for H2S emission in the sewer system.
1–7 2450 0.8 0.001 0.1–0.3 Concrete However, a relatively high H2S concentration was found at
8–10 600 0.8 0.001 0.1–0.3 Concrete some manholes along the branch pipe, such as #9a. The
Gravity branch pipe
reason was probably due to the variation of wastewater
3a–3 47 0.3 0.001 0–0.15 PVC-U
5a–5 40 0.3 0.001 0–0.15 PVC-U quality characteristics, such as COD, sulfate concentration,
b1–5b 28 0.3 0.001 0–0.15 PVC-U ORP, DO, conductivity, velocity and so on.

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Fig. 2 Side view of the studied sewer trunk; not to scale and pipe slope not reflected.

3.2 H2S variation along pipes with septic tanks in residential seasons. Fig. 4(a) shows that H2S concentration in the #3 man-
areas hole was the highest while H2S concentration in the septic tank
The variation of H2S along pipes with septic tanks in residential #3c was the lowest, and H2S concentration in the upstream
areas was investigated. Fig. 4(a) and (b) show the H2S variation manhole #3a was lower than that in manhole #3b (#3 > #3b >
along the sewer pipeline #3a to #3 and #5a to #5 in different #3a > #3c). Similar variation was observed in Fig. 4(b) (#5 >

Table 2 Overview of test scenarios in the fieldwork

Scenarios Manhole Season & weather


Measurement of gaseous H2S All manholes July & dry day
(1) H2S variation along pipe with septic tank in residential area 3a, 3b, 3c, 3, July, Oct, Dec & dry day
5a, 5b, 5c, 5
(2) Effect of water flow on H2S generation and emission 3a, 7 Sept & dry and rain day
(3) Effect of water quality on H2S generation 8a, 9a May & dry and rain day

Fig. 3 Gaseous H2S concentration at different sewer locations. The symbol “–” means the H2S maximum and minimum value; “×” means the H2S
99% and 1% value and “ϒ” means the H2S mean value.

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#5b > #5a > #5c). This indicated that H2S concentration in stream of the septic tank, where drop structures commonly
sewers displayed significant spatial variation. existed. As a result of the high turbulence in the drop struc-
Water quality variation in these manholes is presented in tures, H2S in the liquid phase was released to the gas
Fig. 4(c). The results showed that sulfide was generated phase.25 Therefore, the manholes downstream of septic tanks
within 3 mg S L−1 in the septic tanks (#3c or #5c). Simulta- were considered to be important H2S emission sources.
neously, COD concentration was decreased by approximately
100 mg COD per L, whereas soluble COD and VFA appeared
to increase. This indicated that the septic tank played a criti- 3.3 Effect of temperature on H2S emission
cal role in the biochemical process of the sulfur cycle. In The effect of temperature on H2S concentration in different
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spite of the high sulfide production in septic tanks, H2S was manholes was further evaluated. The sewer temperature was
difficult to release from wastewater to the atmosphere due to measured, which was not affected significantly by the atmo-
the observed supernatant scum, which increased the diffi- spheric temperature variation over the course of a day. As
culty of air–water mass transfer. However, sulfide produced shown in Fig. 5, H2S concentration would reach a higher level
in septic tanks would be transported to the manhole down- at a higher temperature in these manholes. However,

Fig. 4 The data of hydrogen sulfide in the area 1 (#3a, #3b, #3c and #3) and area 2 (#5a, #5b, #5c and #5) in different seasons (a) and (b),
respectively, and concentrations of water quality in three connected manholes in these two areas (c). Manhole #3b and #5b were the upstream
manholes of septic tanks while manholes #3 and #5 were the manholes downstream of septic tank.

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Table 3 The parameters summarized from the data in the #9a manhole

Dry weather Rainfall


Std. Std.
Parameter Mean Dve. Max. Mean Dve. Max.
H2S (ppm) 19.8 10.0 47.0 1.2 2.2 8.0
Water level (cm) 5.6 1.5 11.2 61.6 18.8 87.6
Water flow (cm s−1) 3.68 3 14 0.15 3.4 3.8
Sulfide (mg S L−1) 1.5 1.6 5.2 0.8 0.5 1.5
Sulfate (mg S L−1) 13.4 4.2 25.7 14.5 4.0 21.2
COD (mg L−1) 355.6 137.4 766.0 326.6 246.4 785.6
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Conductivity 1875 429 1875 3333 623 4655


pH 6.6 0.2 7.0 6.2 0.6 6.9
ORP 17.2 9.9 42.0 28.5 13.7 50.0

icantly by temperature. Meanwhile, the drop structure in the


manhole downstream of the septic tank would cause a
greater temperature effect on sulfide emission. The effect of
temperature on H2S emission was associated with the varia-
tions in the sulfide production rate and flow turbulence at
different locations in the sewer system.
Fig. 5 Effect of temperature on H2S emission in the manhole (#3a,
#3b, #5a and #5b) upstream and manhole (#3 and #5) downstream of
septic tank. 3.4 Effect of water flow on H2S variation
The long-term H2S monitoring data in the manhole down-
stream of the septic tank (#7) and branch manhole (#3a) are
influences of temperature on H2S in the downstream man- shown in Fig. 6(a) and (b), respectively. H2S increased from
holes (#3b and #3) were more serious than those on H2S in 8:00 AM, reached a peak (approximately 10 ppm) at 4:00 PM
the upstream manhole (#3a). This indicated that the sulfide and then decreased to 0 ppm at 10:00 PM during 5th–7th Au-
production rate in septic tanks would be affected more signif- gust in the branch manhole (#3a). On the other hand, in the

Fig. 6 Long-term H2S monitoring data in the manholes #3 and #7. The water level in the #7 manhole is presented.

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Fig. 7 Comparison of the long-term H2S and water quality data in the manholes #8a and #9a. The liquid pollutants include sulfide, COD, sulfate,
water flow, Cond., pH and ORP.

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manhole downstream of the septic tank (#7), H2S concentra- manhole #8a and #9a were calculated to be 2.72 and 2.64 g S
tion had two peaks with one at 7:00–9:00 AM and one at m−2 per day), respectively. These similar results indicated
7:00–12:00 PM. However, the actual H2S peak concentration that the difference in the sulfide concentration between these
had not been detected due to the detection limit of the H2S two manholes was not determined by the maximum sulfide
gas (0–320 ppm). Guo et al.25 reported that only one peak production activity (Fig. 7).
appeared at midnight. This indicated that H2S concentration The step-wise regression mechanism and VIF test were
displayed local temporal variation features in different sewer used to pick up important variables and detect multi-collin-
locations. It was observed from the water level in the #7 man- earity, and explain sulfides in the full variable regression
hole that the water level had two peaks at 7:00 am and 8:00 model. The results are shown in Table S1.† Sulfides had sta-
Published on 22 March 2019. Downloaded by University of Queensland on 4/4/2019 7:46:37 AM.

pm, which correlated with H2S peaks. Indeed, a low water tistically significant relationships with COD (P = 1.19 × 10−3),
level could significantly accelerate accumulation of the pro- conductivity (P = 1.34 × 10−4) and velocity (P = −7.21 × 10−3)
duced sulfide in the septic tanks. With water flow increasing while other factors were deleted by step-wise processing. The
in the morning and evening, the high turbulence when VIP scores were lower than 2, indicating that multi-
wastewater fell from the branch pipe to the main pipe would collinearity was not significant in the model. According to the
result in significant sulfide release from liquid to gas. These above results, it could be concluded that sulfide production
results revealed the key role of water flow on H2S diurnal would increase as velocity decreased or COD and conductivity
change. Low flow enhances sulfide accumulation and high increased. These findings were helpful for identifying the H2S
flow enhances H2S emission. level in sewers because COD, conductivity, and velocity can be
During heavy rainfall, H2S concentration would be obvi- measured easily, which provides a potential cost-effective ap-
ously reduced, such as 7th August in the #3a manhole or proach to understand risks due to H2S in sewers.
13th September in the #7 manhole. The sulfide concentration
was consistently low in the next few dry-weather days after a 3.6 Critical impact of septic tanks on carbon loss in sewer
rainfall event. Further, the effect of rainfall on H2S concentra- systems
tion, water quality and water level was analyzed based on Septic tanks in the neighborhoods played a critical role on
long-term measurement in the #9 manhole (shown in sulfide production in sewer networks, which is higher than
Table 3). The increase in the water level could reduce the sul- the limit value (2.0 mg S L−1) that causes severe concrete cor-
fide production rate, which was associated with the low sul- rosion.7 Moreover, COD concentration was reduced by ap-
fide concentration. Also, the increase in the water level could proximately 10–20% in the septic tank but sCOD and VFAs
significantly reduce the turbulence of dropping flow from the had an increase due to anaerobic digestion reactions (Fig. 4).
connected upstream pipe in the manhole. Moreover, the In China, carbon loss during sewage transport in sewers has
sewer sediment was the important source for sulfide genera- become a serious problem, which results in the COD concen-
tion,26,27 which was probably eroded by the rainfall-related trations of WWTP influent to be lower than 300 mg L−1. Some
sharp flow. These could mitigate H2S production and emis- studies31,32 also reported that the septic tank was considered
sion from the sewer system during the rainfall event. to be an important source for the decrease in COD, which
resulted in low carbon resources in the downstream wastewa-
3.5 Effect of water quality on H2S generation ter treatment plant. This study demonstrated the critical role
of septic tanks in carbon loss and sulfide production. How-
The variations in long-term measurement of gaseous H2S ever, very limited studies have investigated how to reduce the
along with the water quality parameters like sulfide level, loss of carbon sources and the sulfide production in septic
COD, sulfate level, water flow, pH, conductivity, ORP and gas- tanks. Therefore, control strategies still need to be effectively
eous H2S between the #8a and #9a manholes are shown in developed to achieve H2S control and carbon maintenance in
Fig. 7. The H2S concentration in the #9a manhole was higher sewers with septic tanks.
than that in the #8a manhole. Simultaneously, the sulfide
level, COD and conductivity were higher but water flow, pH 4. Conclusions
and ORP were lower in the #9a manhole than those in the
#8a manhole. These results were consistent with the general In this study, we conducted a comprehensive investigation
understanding of the sulfide-production process in sewers. on hydrogen sulfide production and emission in sewer sys-
High concentrations of COD would contribute to higher sul- tems in China. H2S spatial distribution was determined by
fide production rates while the sulfate would not limit sulfide sewer structures and wastewater quality in the local sites of
formation if it was higher than 5–15 g S m−3.28 Low velocity the sewer-shed. The manholes downstream of septic tanks in
would also result in a greater deposition of sediments and neighborhoods were identified as H2S emission hotspots due
longer water residence time, which would enhance the sul- to the potential significant sulfide generation in the septic
fide production.29 Recently, an empirical equation was devel- tank. H2S concentration was positively correlated with sulfide
oped to describe the long-term effect of sulfates and COD concentration, COD and conductivity and negatively corre-
on the maximum sulfide production activity.30 Based on this lated with water flow. The effect of temperature on H2S emis-
equation, the maximum sulfide production activity values in sion was also associated with variations in the sulfide

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production rate and flow turbulence at different locations in 10 Z. Liang, L. Zhang, D. Wu and G. Chen, Systematic
the local sewer system. A significant decrease in the sulfide evaluation of a dynamic sewer process model for
concentration was observed with rainfall-derived high water prediction of odor formation and mitigation in large-scale
flow. This study will be useful in understanding H2S produc- pressurized sewers in Hong Kong, Water Res., 2019, 154,
tion and emission in sewer systems in China. Further work is 94–103.
needed to develop technologies for sulfide control and car- 11 F. Jiang, D. Leung, S. Li, G. Chen, S. Okabe and M. van
bon maintenance in sewer systems. Loosdrecht, A biofilm model for prediction of pollutant
transformation in sewers, Water Res., 2009, 43(13),
Conflicts of interest 3187–3198.
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12 C. Yongsiri, J. Vollertsen, M. Rasmussen and T. Hvitved-


The authors declare no conflict of interest. Jacobsen, Air-water transfer of hydrogen sulfide: an
approach for application in sewer networks, Water Environ.
Acknowledgements Res., 2000, 76, 81–88.
This research was supported by the National Natural Science 13 S. Liang, L. Zhang and F. Jiang, Indirect sulfur reduction
Foundation of China (No. 51678337) and Major Science and via polysulfide contributes to serious odor problem in a
Technology Program for Water Pollution Control and Treat- sewer receiving nitrate dosage, Water Res., 2016, 100,
ment of China (No. 2014ZX07305001) and the Tsinghua Univer- 421–428.
sity Initiative Scientific Research Program (No. 2017z21028). 14 X. Hao, J. Zhao and J. Li, Feasibility analysis of centralized
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