A Comprehensive Carbon Footprint Analysis of Different Wastewater Treatment Plant Configurationspdf

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Environmental Research 214 (2022) 113818

Contents lists available at ScienceDirect

Environmental Research
journal homepage: www.elsevier.com/locate/envres

A comprehensive carbon footprint analysis of different wastewater


treatment plant configurations
Ziping Wu a, Haoran Duan a, b, *, Kaili Li a, Liu Ye a, **
a
School of Chemical Engineering, The University of Queensland, St Lucia, QLD, Australia
b
Australian Centre for Water and Environmental Biotechnology (ACWEB, Formerly AWMC), The University of Queensland, St. Lucia, QLD, 4072, Australia

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

Keywords: With the growing concern of global warming, many water utilities are pioneering in mitigating greenhouse gas
Wastewater treatment process (GHG) emissions, with some water utilities aiming to achieve net-zero emissions operation in the next decade.
Carbon footprint However, for wastewater treatment plants (WWTPs), the carbon footprint of different treatment technologies and
Greenhouse gas emissions
its contribution among various units within each treatment configuration is still unclear. This study evaluates the
Sludge management
Carbon neutrality
impacts of process design on the carbon footprint of WWTPs through the analysis of scope 1 (direct emission),
scope 2 (indirect emission), and scope 3 (value chain emission) emissions. The comprehensive configuration
design in this work considered three nutrient removal processes including typical aerobic and anaerobic
wastewater treatment technologies. Emissions from the sludge management processes are also calculated,
including aerobic and anaerobic sludge stabilization processes, short-term and long-term sludge storage, and
three sludge disposal options. In total, 45 processes were analysed and the results were compared. The results
showed the carbon footprints are highly dependent on the treatment configurations of WWTPs. Analysis sug­
gested scope 2 & 3 emissions can be reduced by selecting suitable processes. In general, anaerobic wastewater
and sludge stabilization technologies are more suitable than aerobic technologies to reduce scope 2 & 3 emis­
sions, leading to a lower overall carbon footprint. In comparison, configuration design offers limited opportu­
nities to reduce scope 1 emissions, which may be the future challenge for WWTP to achieve carbon neutrality.

anaerobic conditions occur such as anaerobic wastewater and sludge


1. Introduction treatment (Daelman et al., 2012). The N2O and CH4 have a global
warming potential (GWP) of 265 and 28 CO2-eq, respectively (IPCC,
The main driver of climate change is the increased greenhouse gas 2013). Even a small amount of N2O and CH4 emissions still contribute
(GHG) in the atmosphere (IPCC, 2022). With the growing concern of significantly to the carbon footprint of a WWTP. De Haas and Hartley
global warming, many countries are committed to achieving carbon (2004) estimated that 1% of nitrogen loading converted to N2O could
neutrality by 2050. Wastewater treatment plant (WWTP) is one of the increase the total carbon footprint of WWTP by 30%. Scope 2 emissions
largest GHG emitters (Pan et al., 2016b; Zhao et al., 2019). Many water are the indirect GHG emissions from energy consumption, e.g., mixing,
utilities are pioneering in mitigating GHG emissions, with some aiming aerating, pumping, dewatering, and transporting of wastewater and
to achieve net-zero emissions operation in the next decades. The carbon sludge (Sotos, 2015). Scope 3 emissions are the GHG emissions from the
footprint of WWTP can be categorized into three components: scope 1 assets not owned or controlled by the reporting organization, e.g., GHG
emissions (direct emissions), scope 2 emissions (indirect emissions), and emissions from off-site sludge disposal (Bhatia et al., 2011).
scope 3 emissions (value chain emissions). Scope 1 emissions refer to The wastewater treatment process mainly involves biological
direct GHG emissions from wastewater treatment-related activities. nutrient removal from wastewater and the by-product sludge treatment.
Specifically, it is N2O and CH4 produced during wastewater and sludge The biological nutrient removal can be achieved by anaerobic or aerobic
treatment. N2O is mainly emitted from biological nitrogen removal treatment technologies. Typical aerobic technologies including Modi­
(BNR) processes during wastewater treatment. Unlike N2O, CH4 is fied Ludzak-Ettinger (MLE), Anoxic/Aerobic (A/O) and membrane
usually formed in the sewer system and parts of the WWTP where bioreactor (MBR) can remove carbon and nitrogen from wastewater

* Corresponding author. School of Chemical Engineering, The University of Queensland, St Lucia, QLD, Australia.
** Corresponding author.
E-mail addresses: h.duan@uq.edu.au (H. Duan), l.ye@uq.edu.au (L. Ye).

https://doi.org/10.1016/j.envres.2022.113818
Received 26 January 2022; Received in revised form 30 May 2022; Accepted 30 June 2022
Available online 14 July 2022
0013-9351/Crown Copyright © 2022 Published by Elsevier Inc. All rights reserved.
Z. Wu et al. Environmental Research 214 (2022) 113818

carbon footprint of different wastewater treatment configurations.


Nomenclature Firstly, many potentially important sources of GHG emissions, particu­
larly in sludge handling processes, were not considered in previous an­
GHG Greenhouse gas alyses. For examples, in sludge stabilization, most analyses only
WWTPs Wastewater treatment plants considered anaerobic stabilization, while the GHG emissions from aer­
BNR Biological nitrogen removal obic stabilization have been largely ignored (Daelman et al., 2012; Piao
GWP Global warming potential et al., 2016; Rodriguez-Garcia et al., 2014). However, experiments
A2/O Anaerobic/Anoxic/Aerobic suggested AeD could be a significant source of GHG emissions in WWTPs
MLE Modified Ludzak-Ettinger (Duan et al., 2019; Pan et al., 2016c). Similarly, sludge storage pro­
UASB Upflow anaerobic sludge blanket cesses, including sludge drying and short-term storage (STS) were not
AD Anaerobic digestion included in previous carbon footprint analyses, while both were shown
AeD Aerobic digestion with significant potential for CH4 emissions (Daelman et al., 2012; Pan
LTD Long-term drying et al., 2016a). Despite suggested by experiments with significant GHG
STS Short-term storage emission potentials, their emission contributions and importance to
DM Dry matter overall WWTP carbon footprint remain unclear. Secondly, Piao et al.
A/O Anoxic/Aerobic (2016) showed that when AD is applied for sludge treatment, GHG
MBR Membrane bioreactor emissions from sludge treatment process increase with the increase of
EGSB Expanded granular sludge blanket sludge quantity. A 59% increase in sludge production from wastewater
EBPR Enhanced biological phosphorus removal treatment could increase the direct GHG emissions from sludge treat­
ment processes by 30%. Various wastewater treatment technologies
could lead to different amounts of sludge production (e.g., aerobic
technologies produce 3–4 times of sludge than anaerobic counterpart)
(Metcalf and Eddy, 2013). Anaerobic treatment technologies such as (McCarty et al., 2011), which may significantly impact the GHG emis­
upflow anaerobic sludge blanket (UASB) and expanded granular sludge sions from the downstream sludge treatment processes. These un­
blanket (EGSB) remove carbon, and can be coupled with post aerobic certainties underpin the importance of analysing the carbon footprint of
treatment to achieve carbon and nitrogen removal (Chernicharo, 2006). wastewater treatment configurations as a whole.
The phosphate removal for these above technologies requires additional This study systematically evaluates the impacts of different WWTP
chemical dosing, such as ferric iron, ferrous iron, aluminium, and cal­ configurations, including various technologies/units used in wastewater
cium (Metcalf and Eddy, 2013). Alternatively, Bardenpho, enhanced treatment, sludge handling and sludge disposal, on the total and specific
biological phosphorus removal (EBPR), etc. Could be applied for the carbon footprint of WWTPs. It aims to fill the knowledge gap in un­
biological phosphate and nitrogen removal in WWTP (Metcalf and Eddy, derstanding the carbon footprint of different WWTP configurations and
2013). Wastewater treatment generates a large amount of sludge. Sludge the contributions from specific processes. The carbon footprint of
management at WWTP includes sludge thickening, stabilization, dew­ different wastewater treatment configurations was analysed via a sta­
atering, drying, and disposal. Sludge stabilization is practiced in most tistical model with a comprehensive scenario design based on the
WWTP to reduce pathogens and unpleasant odours as well as inhibit, literature values and reasonable assumptions. The design involves a
reduce, or eliminate the potential for putrefaction. Anaerobic digestion total combination of 45 processes, comprising 3 different processes on
(AD) and aerobic digestion (AeD) are commonly applied stabilization wastewater treatment, 2 on sludge stabilization, 2 on sludge drying, and
technologies (Duan et al., 2019; Metcalf and Eddy, 2013; Shammas and 3 on sludge proposal. The importance and sources of scope 1, 2, and 3
Wang, 2007). AD reduces sludge volume, provides stabilization, and emissions in overall carbon footprint were also analysed.
generates methane for energy recovery. It has been widely adopted in
large WWTPs. In comparison, AeD is more applied in small WWTPs due 2. Methodology
to its low capital cost, suitability for small amounts of less degradable
sludge, and simple operation (Duan et al., 2019). Stabilized sludge will 2.1. System boundary
be stored in WWTPs before final disposal. Depending on the size of
WWTPs, the storage period is normally between 1 and 5 days (Daelman In this work, the system boundary for GHG emissions calculation is
et al., 2012). In some WWTPs, long-term sludge drying (LTD) is used for illustrated in Fig. 1. Direct GHG emissions (scope 1) including the dis­
further drying (by solar and wind) and digestion before final disposal solved methane in raw wastewater, generation from the wastewater
(Pan et al., 2016c). Sludge disposal is commonly achieved by com­ treatment, and on-side sludge treatment (e.g., stabilization, drying, and
posting, landfills, agriculture/land reuse, incineration, and other pro­ storage) was indicated in boxes with red line. Indirect GHG emissions by
cesses (e.g., ponds, industrial reuse) (Metcalf and Eddy, 2013). energy consumption (e.g., chemical dosing, pumping, aeration system)
Studies have been conducted to analyse the GHG emissions from and energy production by generated biogas from the anaerobic treat­
different wastewater/sludge treatment technologies with various focus ment system to offset energy consumption, were also within the
on part of the wastewater treatment configurations whereas not on the boundary (indicated in boxes with blue line). Scope 3 GHG emissions (in
whole configurations (Ab Hamid et al., 2020; Liao et al., 2020; Lopes green boxes), including off-site sludge disposal processes (Landfill,
et al., 2020; Paulu et al., 2021). Previous studies have suggested that incineration, composting and agriculture usage) were considered as
different wastewater treatment technologies could result in different well. In addition, it was assumed that all the electricity was generated
levels of direct GHG emissions and various extent of energy consumption with coal, with the GHG intensity of 843–1171 g CO2-eq/kWh-el (Lenzen,
and sludge production (Cakir and Stenstrom, 2005; Foley et al., 2010; 2008).
Piao et al., 2016; Rahman et al., 2016; Vidal et al., 2002; Yoshida et al., All the other sources of GHG emissions (e.g. GHG emissions from
2014). For example, Piao et al. (2016) reported that the carbon footprint receiving water body and sewer collection, biogenic CO2 emissions) and
of wastewater treatment processes would increase by 20% by adopted energy consumption or generation (e.g. energy production from sludge
MLE, compared to the WWTP with A2/O. Moreover, the direct GHG disposal, energy consumption for sludge transportation) were out of
emissions could increase 105% by adopting aerobic wastewater treat­ scope (illustrated in blocks in dash line in Fig. 1).
ment, compared to anaerobic wastewater treatment (Cakir and Sten­
strom, 2005).
However, there are still uncertainties for WWTPs to understand the

2
Z. Wu et al. Environmental Research 214 (2022) 113818

Fig. 1. Analytical system boundary for GHG emissions from WWTPs.

2.2. Scenario design investigate the GHG emissions from different wastewater and sludge
treatment configurations (Fig. 2). Three different nutrient removal
A comprehensive process design was performed in this study to wastewater treatment configurations were selected for wastewater

Fig. 2. Illustration of designed wastewater treatment system configurations. *Some configurations were designed for comparison and sludge treatment processes
after thickening were skipped.

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Z. Wu et al. Environmental Research 214 (2022) 113818

treatment. Primary treatment, followed by MLE was selected as the (


typical aerobic wastewater treatment configuration for this study. Note CH4 ww1 = CH4 ​ dis, ​ in ​ ∗ ​ 1 − rox ) (2)
that ferric chloride dosing was required for chemical phosphorus
where: CH4ww1 is the methane emissions from wastewater treatment
removal from the MLE system. 5-stage bardenpho was also included in
processes by active stripping of dissolved methane in the influent
this study. Bardenpho is a commonly used wastewater treatment tech­
wastewater. Note that the dissolved methane is assumed to consist of 1%
nology for biological phosphorus and nitrogen removal. Another
of the total chemical oxygen demand (COD) loading in the influent [kg
wastewater treatment configuration option adopted was UASB + MLE.
CH4] (Daelman et al., 2012); CH4dis,in is the dissolved CH4 in the influent
Recently study shows the UASB system has remarkable potential to treat
wastewater [kg CH4]; rox is the percentage of the amount of CH4
domestic wastewater at ambient temperature (Crone et al., 2016; Daud
oxidized in post-aerobic wastewater treatment. The default oxidation
et al., 2018). The following MLE process aims to achieve nitrogen
percentage in this study is assumed to be 80% (Daelman et al., 2012).
removal from UASB effluent.
(
The sludge treatment in this study included the whole process of CH4 ww2 = CH4 ​ dis, anaerobic ​ ∗ ​ 1 − rox ) (3)
thickening, stabilization, dewatering and STS/LTD (Fig. 2). The gener­
ated sludge after the thickening unit will be transported into the sludge where: CH4ww2 is the methane emissions from the anaerobic wastewater
stabilization configuration. Two commonly used sludge stabilization treatment processes [kg CH4]; CH4dis, anaerobic is the dissolved CH4 in the
configurations, AeD or AD were designed to stabilize sludge. The effluent of anaerobic wastewater treatment [kg CH4]; rox is the per­
digested sludge will then be transported for dewatering. After dew­ centage of the amount of CH4 oxidized in post-aerobic wastewater
atering, two options were designed for sludge storage. The dewatered treatment. The default oxidation percentage in this study is assumed to
sludge can be stored in an LTD or STS configuration, before being be 80% (Daelman et al., 2012).
transported out for sludge disposal. The sludge disposal in this study The sludge production from the wastewater treatment is calculated
included the most common sludge disposal methods, namely, com­ by Eqs. (4)–(6) below:
posting + agriculture, landfills and incineration (Grobelak et al., 2019).
Q ​ ∗ ​ YH ​ ∗ ​ (SCODin − SCOD )
Each configuration was composed of one of the three wastewater XHB = (4)
treatment processes (MLE, Bardenpho, or UASB + MLE), one of the two 1 + bH ​ ∗ ​ SRT
sludge stabilization units (AeD or AD), one of the two sludge storage
where: XHB is the heterotrophs biomass generated per day [kg COD/d];
methods (LTD or STS), and one of the three sludge disposal ways
Q is the flow rate of the influent wastewater [L/d]; YH is the yield rate of
(composting + agriculture, landfills or incineration). A total of 36 sce­
the heterotrophs [kg COD formed cells/kg COD consumed]; SCODin is the
narios were studied.
concentration of the COD in the influent [kg COD/l]; SCOD is the con­
To investigate the impacts of sludge stabilization on the WWTP
centration of the COD in the bioreactor [kg COD/L]; bH is the decay rate
carbon footprint, additional scenarios were studied. Namely, the sludge
of heterotrophs [d− 1]; SRT is the solid retention time of the bioreactor
generated from the wastewater treatment processes was sent to disposal
[d].
without digestion and drying. These scenarios will enable direct com­
( )
parison with the scenarios with sludge treatment. Specifically, these Q ​ ∗ ​ YA ​ ∗ ​ SNH3 in − SNH3
XA = (5)
configuration was composed of one of the three wastewater treatment 1 + bA ​ ∗ ​ SRT
processes (MLE, Bardenpho, or UASB + MLE) and one of the three sludge
disposal options (composting + agriculture, landfills or incineration). A where: XA is the autotrophs biomass generated per day [kg COD/d]; YA
total of 9 scenarios were studied. is the yield rate of the autotrophs [kg COD formed cells/kg NH3–N
consumed]; SNH3in is the concentration of the NH3–N in the influent [kg-
N/L]; SNH3 is the concentration of the NH3–N in the bioreactor [kg-N/L];
2.3. GHG emissions calculation bA is the decay rate of autotrophs [d− 1].
Xinert = SRT ​ ∗ ​ (bA ​ ∗ ​ XA + bH ​ ∗ ​ XH ) ​ ∗ ​ f p (6)
A statistic model was built to calculate the GHG emissions from the
overall WWTPs within the boundary of this study. The designed raw
where: Xinert is the inert solids generated in the bioreactor [kg COD/d];
wastewater characteristics are listed in SI Table S1. The design param­
fp is the fraction of the bio-inactive solids.
eters for different configurations of the WWTPs are mainly based on the
The GHG emissions from sludge treatment are described in Eqs. (7)–
literature values and reasonable assumptions (SI Table S2). The esti­
(10) below:
mation of GHG emissions for different WWTPs is based on the emission
factor (EF) from the literature (SI Table S2). Given that the values of the N2 O ​ AeD = EFAeD ​ ∗ ​ TNloading,sludge ​ ∗ ​
44
(7)
parameters vary between different studies and assumptions, the uncer­ 28
tainty analysis for scope 1, scope 2, and scope 3 emissions from different
where: N2OAeD is the N2O emissions from aerobic sludge digester [kg
designed scenarios was conducted through Monte Carlo analysis in MS
N2O]; EFAeD is N2O emissions factor from AeD [kg N2O–N/kg-N];
Excel. For example, the N2O EF (wastewater treatment processes, aer­
TNloading, sludge is the total nitrogen loading in raw sludge [kg-N].
obic digestion, and sludge disposal options), the COD and nutrients
loading in raw wastewater and the performance of treatment efficiency CH4 ​ AD = CH4 ​ dis, AD + EFAD,i ​ ∗ ​ biogas ​ produced (8)
were used to conduct the Monte Carlo analysis. The summary of design
parameters for uncertainty analysis are listed in SI Table S3. where: CH4AD is the methane emissions from anaerobic sludge digester
For wastewater treatment, the emitted mass of N2O and CH4 were [kg CH4]; biogasproduced is the total generated biogas from the anaerobic
calculated based on Eqs. (1)–(3) below: digester [m3]; EFAD,i is the CH4 emissions factor of the anaerobic
digester, such as methane emissions from the pressure relief valve,
44
N2 O ​ ww = EFi ​ ∗ ​ TNloading ​ ∗ ​ (1) methane emission through gas bubbles entrained in digested sludge, etc
28
[m3 CH4/m3 ].
where: N2Oww is the N2O emissions from wastewater treatment pro­
CH4 ​ LTD = CODAnaerobic ​ ∗ ​ CODBiodegradable (9)
cesses [kg N2O]; EFi is the N2O emissions factor from treatment
configuration i [kg N2O–N/kg-N]; TNloading is the total nitrogen loading where: CH4LTD is the methane emissions from LTD configuration [kg
in influent wastewater [kg-N]; 44/28 is used to convert [kg N2O–N] to CH4]; CODAnaerobic is the ratio of the COD consumed for CH4 generation
[kg N2O].

4
Z. Wu et al. Environmental Research 214 (2022) 113818

(Pan et al., 2016c); CODBiodegradble is the biodegradable COD loading of based on the Eqs. (17) and (18) (Li et al., 2022):
the raw sludge [kg COD]. ∑
Energy ​ recovery− eq,i
Carbon ​ Neutrality = ∑ ∑
CH4 ​ STS = EFSTS ​ ∗ ​ CH4produced (10) Direct ​ emissions− eq,i + Indirect ​ emissions− eq,i

(17)
where: CH4STS is the methane emissions from STS configuration [kg
CH4]; EFSTS is the methane emissions factor of the STS [m3CH4/m3

Energy ​ recovery− eq,i
generated CH4]; CH4produced is the methane generated from the anaer­ Energy ​ Neutrality = ∑ (18)
Indirect ​ emissions− eq,i
obic digester [m3 CH4].

The GHG emissions from sludge disposal are determined by the IPCC where: Direct emissions_eq,i is sum of the direct emissions equivalent

method, as indicated by Eq. (11) to (15) to CO2 from WWTP [kgCO2-eq]; Indirect emissions_eq,i is sum of the

( ) energy consumption equivalent to CO2 of WWTP [kgCO2-eq]; Energy
CH4incineration ​ = IWi ​ ∗ ​ EFIncineration CH4 ∗ ​ 10− 6 (11) recovery_eq,i is sum of the energy recovery equivalent to CO2 from
WWTP [kgCO2-eq].
where: CH4incineration is the methane emissions from incineration [Gg
CH4/yr]; IWi is the amount of solids waste incinerated [Gg/yr]; EFInci­ 3. Results and discussion
neration_CH4 is the aggregate CH4 emissions factor [kg CH4/Gg waste].
( ) 3.1. Carbon footprints of WWTPs with different configurations
N2 Oincineration = IWi ​ ∗ ​ EFIncineration N2 O ∗ ​ 10− 6 (12)
The carbon footprints of WWTPs with different configurations are
where: N2Oincineration is the methane emissions from incineration [Gg calculated and presented by the type of emissions source (scope 1, scope
N2O/yr]; EFIncineration_N2O is the aggregate N2O emissions factor [kg 2, scope 3 emissions) in Fig. 3. It can be seen clearly that the carbon
N2O/Gg of waste]. footprints are highly dependent on the treatment configurations of
( ) WWTPs. The total GHG emissions of different scenarios vary greatly,
N2 Ocomposting = Mi ​ ∗ ​ EFComposting N2 O ∗ ​ 10− 3 (13)
from 411 to 1775 kg CO2-eq/ML-ww/d, with the highest GHG emissions
approximately 4 times higher than that of the lowest GHG emissions.
where: N2Ocompsoting is the methane emissions from composting [Gg The top three high emissions (1649–1775 kgCO2-eq/ML-ww/d) configu­
N2O]; Mi is the mass of organic waste treated by composting [Gg]; rations are dominated by the combination of aerobic nutrient removal
EFCompsoting_N2O is the N2O emissions factor for composting [g N2O/kg (MLE wastewater treatment), AeD and LTD. The sludge disposal in
waste treated]. WWTP only played a minor role in the total carbon footprint profile. In
( )
fact, the top 3 configurations with the highest GHG emissions all
CH4composting = Mi ​ ∗ ​ EFComposting CH4 ∗ ​ 10− 3 − R (14)
adopted aerobic wastewater treatment, aerobic sludge stabilization, and
LTD. The 3 lowest GHG emissions configurations are the combinations
where: N2Ocompsoting is the methane emissions from composting [Gg
employing anaerobic wastewater treatment (UASB), AD and STS, with
CH4]; EFComposting_CH4 is the CH4 emissions factor for composting [g
total GHG emissions of 411–520 kgCO2-eq/ML-ww/d. The large variation
CH4/kg waste]; R is the total amount of CH4 recovered (0 for this study)
of the overall carbon footprint suggests that there are opportunities to
[Gg CH4].
reduce carbon footprint by choosing different configurations or pro­
[( )
16 cesses at the design stage of a WWTP or during the plant upgrading.
CH4Landfill = MSWT ​ ∗ ​ MSWF ​ ∗ ​ MCF ​ ∗ ​ DOC ​ ∗ ​ DOCF ​ ∗ ​ F ​ ∗ ​
12
]
( ) 3.2. Scope 1 emissions
− R ∗ 1 − rox, ​ Landfill

(15) The amount of scope 1 emissions and its contribution to the overall
GHG emissions is undoubtedly significant (as shown in Fig. 3). The scope
where: CH4Landfill is the CH4 emissions from landfill [kg CH4/yr]; MSWT 1 emissions account for 23–83% of the total carbon footprint under
is the total municipal solids waste generated [Gg/yr]; MSWF is the different configuration scenarios. Scope 1 emission could be the major
faction of municipal solids wastes disposed at the Landfill; MCF is the contributor to carbon footprint for configurations with anaerobic pro­
methane correction factor; DOC is the degradable organic carbon [Gg/ cesses. This is because anaerobic treatment technologies could signifi­
Gg municipal solids waste]; DOCF is the fraction of the degradable cantly reduce scope 2 and scope 3 emissions due to energy recovery and
organic carbon; F is the fraction by volume of CH4 in landfills gas; R is less sludge production. For example, in the configuration where the
recovered CH4 [Gg/yr]; rox, Landfill is the oxidation factor of methane. wastewater is treated by UASB + MLE and sludge is stabilized by AD, the
In this study, the N2O emissions from agriculture only considered the scope 1 emissions could contribute to 63%–83% of total GHG emissions
synthetic fertilizer N applied to the managed soils. The N2O emission from WWTP. Scope 1 emissions become less significant in configurations
from agriculture is described by the Eq. (16): with aerobic technologies. For example, when the wastewater is treated
( ) ( ) by MLE or Bardenpho, sludge is stabilized by AeD and the LTD is avoi­
N2 O − Ninput = FSN ​ ∗ ​ EFAgriculture + FSN ​ ∗ ​ EFAgricultureFR (16)
ded, the scope 1 emissions only account for 23%–30% of the overall
carbon footprint of WWTP.
where: N2O-Ninput is the annual direct N2O–N emissions from N inputs to
For comparison, the sources of scope 1 emissions from the waste­
managed soils [kg N2O–N/yr]; FSN is the annual amount of synthetic
water treatment processes and the sludge treatment processes were
fertilizer N applied to soils [kg N/yr]; EFAgriculture is the emissions factor
plotted respectively as shown in Fig. 4. In Fig. 4a, the scope 1 emissions
for N2O emissions from N inputs [kg N2O–N/kg N input]; EFAgriculture_FR
from wastewater treatment processes varied from 218 to 354 kgCO2-eq/
is the emissions factor for N2O emissions from N inputs to flooded rice
ML-ww/d, contributing to 12%–75% of the total GHG emissions in
[kg N2O–N/kg N input].
wastewater treatment processes, both CH4 and N2O emissions
contribute to scope 1 emissions of WWTPs. Compared with Bardenpho
2.4. Carbon and energy neutrality or MLE process, the UASB + MLE process (anaerobic treatment with post
aerobic treatment) produced higher scope 1 emissions than aerobic
The carbon and energy neutrality targets of this study were defined technologies. In the sealed UASB reactor, organics are converted to

5
Z. Wu et al. Environmental Research 214 (2022) 113818

Fig. 3. Carbon footprints of WWTPs with different treatment configurations. The error bar represents the uncertainties (Monte Carlo analysis).

methane-rich biogas and the supersaturated dissolved methane is also


formed normally in the range of 19–29 mg CH4/L (Bandara et al., 2012;
Matsuura et al., 2015; Souza et al., 2012). In the following aerobic
treatment for nitrogen removal, about 20% of the dissolved methane
would be stripped out by aeration (Daelman et al., 2012), which
contributed to 36% more direct GHG than aerobic technology only.
While methane emissions from wastewater treatment processes can be
reduced by choosing aerobic treatment technologies, the N2O is an
inevitable by-product generated in the biological nitrogen removal
process (Duan et al., 2017; Kampschreur et al., 2008). In this study, N2O
is always the dominant GHG when aerobic treatment processes are used,
accounting for up to 96% of the scope 1 emissions. Moreover, the
anaerobic technologies for nutrient removal also produce N2O in the
Fig. 4. Scope 1 emissions from WWTPs with different treatment configurations following nutrients removal process. The N2O emissions from UASB +
(a) scope 1 emissions from carbon and nutrients removal wastewater treatment MLE processes contributed 61.1% of the direct emissions.
processes; (b) scope 1 emissions from sludge treatment. The error bar represents Sludge treatment could also be a significant source of scope 1
the uncertainties (Monte Carlo analysis). emissions (Fig. 4b). The direct GHG emissions from sludge treatment

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Z. Wu et al. Environmental Research 214 (2022) 113818

Table 1
Analyses of carbon neutrality and energy neutrality for different configurations.
Configurations Direct emission, Indirect emission, Energy recovery, Energy neutrality Carbon neutrality
kgCO2-eq/ML-ww/d kg CO2-eq/ML-ww/d kgCO2-eq/ML-ww/d

UASB + MLE + AeD + LTD 579 577 419 73% 36%


UASB + MLE + AeD + STS 399 577 419 73% 43%
UASB + MLE + AD + LTD 508 599 570 95% 51%
UASB + MLE + AD + STS 369 599 570 95% 59%
MLE + AeD + LTD 933 655 0 0% 0%
MLE + AeD + STS 316 655 0 0% 0%
MLE + AD + LTD 793 637 403 63% 28%
MLE + AD + STS 279 637 403 63% 44%
Bardenpho + AeD + LTD 569 620 0 0% 0%
Bardenpho + AeD + STS 265 620 0 0% 0%
Bardenpho + AD + LTD 517 612 176 29% 16%
Bardenpho + AD + STS 249 612 176 29% 20%

varied greatly, from 27 to 716 kgCO2-eq/ML-ww/d, accounting for 4%– 3.3. Scope 2 emissions
58% of the total GHG emissions from WWTP. Unlike the wastewater
treatment process, CH4 emissions contribute to the majority of the scope Scope 2 emissions in this study include energy consumption for both
1 emissions from sludge treatment. The direct CH4 emissions from wastewater and sludge treatment processes. The scope 2 emissions could
sludge are 16–617 kgCO2-eq/ML-ww/d, while the direct N2O emissions contribute 14–68% of total carbon footprint of WWTP. However, it was
from sludge are only 43.1 to 98.4 kgCO2-eq/ML-ww/d. When the LTD was observed that most configurations with relatively low GHG emissions
adopted in WWTP, the overall scope 1 emissions could increase signif­ involve energy recovery, which offsets the scope 2 emissions. Scope 2
icantly by 26%–46%. This is because a significant portion of the stabi­ emissions could be minimized by reducing the energy consumption, as
lized sludge is still biodegradable. A long-term sludge drying lagoon well as by enhancing the energy recovery (scope 2 offset). Effectively,
study showed that 43% of COD was biodegradable (Pan et al., 2016c). the scope 2 emissions from WWTP could be minimized by choosing
The biodegradable portion of the sludge will be slowly digested during configurations with high energy efficiency and energy recovery.
the drying stage under the anaerobic condition to generate CH4. The Anaerobic treatment technologies represent a promising solution to
long-term sludge drying facility is often an open system. Therefore, minimize scope 2 emissions due to their low energy consumption and
methane generated is emitted into the atmosphere. potential for energy recovery via methane-rich biogas capture. UASB
Moreover, the scope 1 emissions from sludge treatment are also enables energy recovery from produced biogas leading to offset GHG
highly dependent on the amount of the waste sludge to be treated. For emissions. During anaerobic wastewater treatment, most of the COD
example, the amount of waste sludge generated from MLE, Bardenpho, would be converted to biogas. Roughly 60–70% of loading COD can be
and the UASB + MLE processes are 24,208 kg dry matter (DM)/d, converted to methane, and approximately 80% of generated methane
10,614 kgDM/d, and 11,412 kgDM/d, respectively (Table 2). The scope could be used for energy recovery (Bandara et al., 2011, 2012; Matsuura
1 emission from sludge treatment after the MLE process are the highest et al., 2015; Souza et al., 2012). For example, when the UASB is adopted
(716 kgCO2-eq/ML-ww/d) and the WWTP with UASB + MLE process has in WWTPs, the carbon footprint of WWTPs could be significantly
the lowest scope 1 emissions from its following sludge treatment pro­ reduced compared to the MLE and Bardenpho. The carbon footprint of
cesses (16–225 kgCO2-eq/ML-ww/d). WWTPs with UASB are 411–816 kgCO2-eq/ML-ww/d. In comparison,
Clearly, scope 1 emissions from sludge treatment can be feasibly total GHG emissions from WWTPs with aerobic wastewater treatment
minimized by avoiding LTD and by adopting the wastewater treatment processes such as MLE and Bardenpho are 599–1773 kgCO2-eq/ML-ww/d
process with less sludge production. However, reducing scope 1 emis­ and 635–1221 kgCO2-eq/ML-ww/d, respectively.
sions from wastewater treatment is still challenging since all the The direct GHG emissions, indirect GHG emissions, and offset GHG
wastewater treatment processes with nutrient removal inevitably led to emissions of all investigated configurations are summarised in Table 1.
N2O emissions (Kampschreur et al., 2009; Vasilaki et al., 2019). Exten­ The results showed that the complete aerobic wastewater and sludge
sive studies have attempted to mitigate N2O emissions from biological treatment has the highest energy consumption. For example, the energy
nitrogen removal processes (Duan et al., 2021), which could further consumption for MEL + AeD and Bardenpho + AeD are 655 kgCO2-eq/
reduce the carbon footprint of WWTPs in the future. ML-ww/d and 622 kgCO2-eq/ML-ww/d, respectively. When UASB and AeD
were adopted in WWTP, the energy consumption was 577 kgCO2-eq/ML-
ww/d as the anaerobic treatment has the potential for energy recovery.

Table 2
Summary of sludge production, sludge for disposal, biogas production, and energy generation.
Configurations Sludge production, kg DM/d Sludge for disposal, kg DM/d biogas production, m3/d Energy generation, kg CO2-eq/d

UASB + MLE + AeD + LTD 11412a 5225 5582 20972


UASB + MLE + AeD + STS 11412a 9078 5582 20972
UASB + MLE + AD + LTD 11412a 5077 6709 28513
UASB + MLE + AD + STS 11412a 8604 6709 28513
MLE + AeD + LTD 24208a 7329 0 0
MLE + AeD + STS 24208a 16150 0 0
MLE + AD + LTD 24208a 7027 3504 20181
MLE + AD + STS 24208a 15174 3504 20181
Bardenpho + AeD + LTD 10614 2687 0 0
Bardenpho + AeD + STS 10614 4679 0 0
Bardenpho + AD + LTD 10614 2603 1534 8841
Bardenpho + AD + STS 10614 6374 1534 8841
a
The generated sludge contained 3647 kg inorganic solid (nonnitrogen content) due to chemical dosing.

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Z. Wu et al. Environmental Research 214 (2022) 113818

Therefore, the highest energy recovery option is the complete anaerobic emissions. Air-stripping is a commonly applied technology to enhance
wastewater and sludge treatment which could recover 570 kgCO2-eq/ the liquid to gas transfer efficiency. It has been applied to remove the
ML-ww/d of energy. Overall, in terms of the scope 2 emissions, the ammonia and methane from landfill leachate (Ferraz et al., 2013).
optimal configurations for minimizing scope 2 emissions are the UASB However, applying air-stripping has the issue with dilution of the
+ AD with only 29 kgCO2-eq/ML-ww/d of scope 2 emissions. methane in the biogas and prohibits the beneficial use of biogas. Another
Lastly, the calculation shows that achieving energy neutrality is still technology is membrane-based technology which uses the non-porous or
far from achieving carbon neutrality (Table 1). Scope 1 and scope 2 microporous membrane to recover the methane for subsequent reuse
emissions were considered in carbon neutrality calculation, and both (Bandara et al., 2011). The microporous membrane can be used for the
electrical and heat energy were considered for the scope 2 emissions and high substrate concentration liquid, such as AnMBR, and the non-porous
energy recovery calculations. In this analysis, energy neutrality could membrane is more suitable for the less solid content effluent like UASB.
achieve 35–95%, while carbon neutrality could achieve 17–59%. When However, the use of membrane technology required sweeping gas to
the UASB and AD were adopted in WWTP, the energy neutrality could create a methane gradient between the outside and inside of the mem­
achieve 73–95%, and the carbon neutrality could reach 36–59%. When brane to increase the mass transfer efficiency, which could reduce the
MLE and Bardenpho were used for wastewater treatment and AD was purity of methane in the biogas (Cookney et al., 2012).
used for sludge stabilization, the energy and carbon neutrality could The effective removal or recovery of the dissolved methane from
increase by 29–63% and 16–44%, respectively. anaerobic treatment technology could reduce GHG emissions. However,
the feasibility of the currently developed post-treatment technologies
3.4. Scope 3 emissions has not yet been fully evaluated by the economic viability and practi­
cability. In addition, while applied anaerobic technology has the above
The contributions of scope 3 emissions to overall emissions are benefits compared to aerobic technology, the benefits of using anaerobic
shown in Fig. 3. It should be noted that in this study scope 3 refers technology may be less significant in the future. With the ongoing
specifically to the GHG emissions from sludge disposal configurations. adoption of renewable energy, the scope 2 emissions may no longer be
Compared to scope 1 and scope 2 emissions, scope 3 emissions play a an issue for WWTP. Thus, the benefits of using the CH4 generated from
minor role in overall GHG emissions in most WWTP configurations, anaerobic technology to offset scope 2 will reduce accordingly.
contributing only 1–13% to the overall carbon footprint. However, when
the landfill is applied for sludge disposal, the scope 3 emissions could 3.6. Sludge stabilization: source or sink?
contribute to 21%–41% of the total GHG emissions. Landfill generates
significantly higher GHG than those from composting, agriculture, and AD and AeD are commonly applied in WWTP for sludge stabilization.
incineration. In addition, the amount of scope 3 emissions highly relies Similar to anaerobic wastewater treatment processes, sludge stabiliza­
on the amount of sludge for disposal. Table 2 presents the amount of tion processes could result in higher scope 1 emissions in WWTP while at
sludge production and sludge disposal. For example, the wasted sludge the same time may reduce scope 2 and/or scope 3 emissions. To answer
for disposal was 5225–9078 kg of dry matter per day when UASB was whether sludge stabilization may lead to a higher or lower carbon
adopted. The scope 3 emission from WWTP with UASB was 8–138 footprint, the scenarios without sludge stabilization were analysed to
kgCO2-eq/ML-ww/d (Fig. 3). As discussed in Section 3.2, the UASB pro­ compare with the same configurations that equip with sludge treatment
duces less sludge compared to the Bardenpho and MLE, thus resulting in (Fig. 5).
less scope 3 emissions from sludge disposal. When the MLE was applied Fugitive GHG will be directly emitted into the atmosphere during the
in WWTP, the generated sludge for disposal was 7329–16150 kg dry sludge stabilization. Compared to the scenario without sludge treat­
matter/d, and the scope 3 emissions were 18–389 kgCO2-eq/ML ML-ww/ ment, the GHG emissions from sludge stabilization processes could in­
d. crease the scope 1 emissions to different extents. AD slightly increases
the scope 1 emissions by 4–16 kgCO2-eq/ML-ww/d, representing 1.2%–
3.5. Role of anaerobic wastewater treatment processes 7% higher emission than configurations without sludge stabilization
(Fig. 4a and b). Methane leakage often occurs due to poor maintenance
The role of the anaerobic wastewater treatment process is seemingly of anaerobic digesters which contributes to the direct GHG emissions
contradictory in terms of GHG emissions. On the one hand, anaerobic (Daelman et al., 2012; Reinelt et al., 2016; Schaum et al., 2015, 2016;
technologies have higher energy efficiency and enable energy recovery Tauber et al., 2019). In an anaerobic digester, the gasholder prevents gas
(scope 2 emissions). On the other hand, it leads to higher scope 1 leakage and stores generated biogas. However, the gasholder and valves
emissions than aerobic technologies due to CH4 emissions. Nevertheless, could result in leakage if poorly maintained. Tauber et al. (2019) re­
this study shows that despite higher scope 1 emissions, anaerobic ported that methane leakage from AD maintenance holes contributed to
technologies lead to an overall small carbon footprint due to much lower 0.4% of the total generated methane due to poor maintenance. The
scope 2 and scope 3 emissions. For example, when comparing the UASB methane loss from pressure-relief valves reportedly contributes to
+ MLE + AD + STS + Landfill with MLE + AD + STS + Landfill for scope 0.06–1.7% of the total methane generated in AD (Reinelt et al., 2016).
1 emissions, the former process was 369 kgCO2-eq/ML_ww/d, which was In comparison, AeD results in significantly higher scope 1 emissions,
higher than the latter MLE only process (279 kgCO2-eq/ML_ww/d). mainly due to N2O emissions. Scope 1 emissions of WWTPs could be
However, for scope 2 and scope 3 emissions, the UASB + MLE process increased by 14%–45% due to the adoption of AeD. In AeD, the available
was much lower than that of MLE only process. In comparison, the scope substrates in feeding sludge are limited so that the microorganisms
2 and scope 3 emissions for the UASB + MLE process were 29 and 122 consume their protoplasm, which the ammonia could be released, to
kgCO2-eq/ML_ww/d respectively, while the MLE process had an emission generate energy for cell reaction maintenance (Metcalf and Eddy, 2013).
of 122 and 355 kgCO2-eq/ML_ww/d for scope 2 and scope 3 emissions. In Then nitrification and denitrification can happen in the aerobic digester
terms of the overall carbon footprint, the wastewater treated by anaer­ (Duan et al., 2019; Kim and Novak, 2017). Consequently, N2O will be
obic configuration emitted 520 kgCO2-eq/ML-ww/d, while the WWTP generated from BNR processes within the aerobic digestor, and the
with aerobic wastewater treatment emitted 868 kgCO2-eq/ML-ww/d. aerobic digester usually is not covered. Therefore, the stripped-out N2O
It should be noted that CH4 emission has been regarded as the major could be directly emitted to the atmosphere, thus causing the increase of
obstacle to the application of anaerobic technologies. The dissolved CH4 scope 1 emissions from AeD.
in the anaerobic treatment effluent could be largely released into the When it comes to scope 2 emissions, AD and AeDs have distinct
atmosphere when the proper post-treatment was not applied. Some of consequences. AD could significantly reduce scope 2 emissions. In this
the post-treatment technologies have been developed to mitigate CH4 study, when the AD was used for sludge stabilization, the scope 2

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Z. Wu et al. Environmental Research 214 (2022) 113818

Fig. 5. Overall emissions from WWTPs with different wastewater treatment configurations but without sludge stabilization process. The error bar represents the
uncertainties (Monte Carlo analysis).

emissions could be significantly reduced by 20.6%–73.2% compared to demonstrated that the UASB has the promising potential to minimize
the WWTP without AD. AD can convert the biogenic carbon contained in GHG emissions compared to aerobic wastewater technologies through
the sludge to biogas to generate bioenergy (Calderon et al., 2021; IPCC significantly reduced scope 2 and 3 emissions but increased scope 1
et al., 2019; Metcalf and Eddy, 2013). The generated biogas can be emissions. Where it is feasible, the anaerobic process should be imple­
converted to electrical energy to cover 60% of the overall electricity mented to enhance energy efficiency and enable energy recovery.
consumption (Daelman et al., 2012). Thus, it reduces the use of energy Nevertheless, the anaerobic process would increase scope 1 emissions
generated from fossil fuel sources. Therefore, the AD process is regarded due to the remaining dissolved methane in the effluent, which is a major
as a carbon sink (UNEP, 2017). In contrast, sludge stabilization by AeD challenge for anaerobic processes. Besides, it should be noted that as
increases the scope 2 emissions. Unlike AD, AeD requires oxygen to renewable energy is becoming widely available, the role of anaerobic
achieve organic matter removal and the aeration results in significant technology in reducing GHG emissions (by reducing scope 2 emissions)
electricity consumption. The oxygen requirements of AeD are typically from WWTP may be less significant.
1.6–1.9 kg O2/kg VSS destroyed (Metcalf and Eddy, 2013). The scope 2 For sludge handling, while sludge drying could significantly reduce
emissions from WWTP with aerobic digester could increase by 13%– the volume of the treated sludge and the operating cost, the uncaptured
31% compared to that from WWTP without sludge stabilization. Note CH4 results in significant scope 1 emissions (Pan et al., 2016c),
that AeD results in significantly higher scope 2 emissions than AD as AeD contributing to 22–59% of the total GHG emissions from WWTP. It
produces 30%–82% higher scope 2 emissions than AD. should therefore be avoided to reduce WWTP carbon footprint.
Both AD and AeD reduce scope 3 emissions due to reduced organic Furthermore, when AD is adopted, the GHG emissions could be reduced
matters after sludge stabilization. Usually, AD and AeD can achieve by 12%–38% compared to the WWTP without sludge stabilization. The
30%–40% organic matter destruction of the sludge, while the digestion potential for GHG emissions reduction from AD is significant. In com­
efficiency highly depends on the SRT and temperature (Kim et al., 2010; parison, while aerobic sludge digestion could also reduce scope 3
Li et al., 2013; Metcalf and Eddy, 2013). Composting, agriculture reuse, emissions due to reducing organic matter for sludge disposal, it increases
landfills, and incineration were considered sludge disposal options in both scope 1 and scope 2 emissions, leading to an overall higher carbon
this study. The IPCC guideline identified the majority of the GHG footprint.
emissions from sludge disposal are N2O and CH4 (IPCC et al., 2019). Lastly, landfills should be avoided for sludge disposal. Compared to
With the carbon loading rate reduced for sludge disposal, the CH4 other sludge disposal methods, the scope 3 emissions from landfills ac­
emissions decreased. In this study, when sludge stabilization was count for 10%–43% of the total carbon footprint. However, the scope 3
adopted in WWTP, the scope 3 emissions could be reduced by 40%– emissions from incineration, composting, and agriculture only
47.5% regardless of AD or AeD. contribute 1%–14% of the total GHG emissions.
Taking scope 1, 2 and 3 emissions into consideration, AD and AeD
can play distinct roles in WWTP carbon footprints. While AD could 5. Conclusion and perspectives
slightly increase scope 1 emissions, it significantly reduces scope 2 and 3
emissions, collectively leading to lower carbon footprints of WWTP by This study systematically evaluated the impacts of different WWTP
2–38%. In comparison, compared with WWTPs without sludge stabili­ configurations. The outcome of this study informs WWTP configuration
zation, AeD leads to higher scope 1 and scope 2 emissions while design, demonstrating that the carbon footprint of WWTP is highly
reducing scope 3 emissions. Consequently, the overall GHG emissions dependent on the treatment configurations, with the highest GHG
significantly increased by 2%–29% compared with the scenarios emissions approximately 4 times higher than that with the lowest GHG
without AeD. emissions.
The analysis showed scope 2 & 3 emissions may be reduced by
4. Implications to wastewater treatment design selecting suitable processes. Specifically, applying anaerobic waste­
water treatment technologies can significantly reduce the total WWTP
This study shows that various wastewater treatment plant configu­ carbon footprint due to its high energy efficiency and energy recovery
rations could have vast different carbon footprints and some processes (scope 2 emissions offset), despite the increased scope 1 emissions due to
are better suited than the others to reduce the carbon footprints of dissolved CH4 stripping. Sludge stabilization via AD could also reduce
WWTPs. the scope 2 & 3 emissions while aerobic sludge digestion may increase
For wastewater treatment, many studies have shown the possibility the overall carbon footprint. Sludge disposal via landfill could result in
of using anaerobic wastewater treatment technology with post aerobic high scope 3 emissions and should be avoided.
treatment, especially UASB, to treat municipal wastewater at ambient or Compared with Scope 2 & 3 emissions, there are less opportunities to
low temperatures, in the past decade (Chernicharo, 2006; Kayranli and reduce Scope 1 emissions by configuration design. Long-term sludge
Ugurlu, 2011; Latif et al., 2011; Lew et al., 2011). This study drying should be avoided as it contributes significantly to the carbon

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Z. Wu et al. Environmental Research 214 (2022) 113818

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Ngarize, S., Osako, A., Pyrozhenko, Y., Shermanau, P., Federici, S. (Eds.), 2019
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The authors declare that they have no known competing financial
IPCC, Switzerland.
interests or personal relationships that could have appeared to influence IPCC, 2022. Climate Change 2022: Mitigation of Climate Change.
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