Cleaner Environmental Systems 2 (2021) 100026

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Cleaner Environmental Systems

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Life cycle assessment of electrodialysis for sidestream nitrogen recovery in

municipal wastewater treatment
Donald Vineyard a, Andrea Hicks a, K.G. Karthikeyan b, Christy Davidson c, Phillip Barak c, *
a
University of Wisconsin-Madison, Department of Civil and Environmental Engineering, 1415 Engineering Drive, Madison, WI, 53706, USA
b
University of Wisconsin-Madison, Department of Biological Systems Engineering, 228 Agricultural Engineering Building, 460 Henry Mall, Madison, WI, 53706, USA
c
University of Wisconsin-Madison, Department of Soil Science, 1525 Observatory Drive, Madison, WI, 53706, USA

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

Keywords: Nitrogen is removed during municipal wastewater treatment to reduce eutrophication of waterways and preserve
Ammonium drinking water quality. Nitrification-denitrification and sidestream partial nitrification-anammox are state-of-the-
Anaerobic digest art municipal N removal technologies, but they require energy for aeration and can release nitrous oxide as a
Modeling
fugitive greenhouse gas. An emerging sidestream electrodialysis technology is intended to both remove and
Anammox
Nitrification
recover N as ammonium-based fertilizer. This midpoint life cycle assessment compiles literature values to
Denitrification compare the state-of-the-art technologies of municipal wastewater nitrogen removal to the new electrodialysis
nitrogen removal and recovery technology, accounting for the offset of Haber-Bosch-derived ammonia. Electro-
dialysis is projected to be environmentally favorable compared to the state-of-the-art, predicting electricity sav-
ings similar to anammox and, with the offset of industrial ammonia manufacture, net negative emissions in five of
ten midpoint environmental impact categories, including global warming potential.

1. Introduction
The United States consumes approximately 12 million tons of nitro-
gen (N) fertilizer each year (USDA, 2018), which leads to a significant
load of nutrient pollution to surface waters through surface runoff and
wastewater discharge. Environmental policy is shifting in order to
discourage nutrient pollution of waterways (USEPA, 2009) as the nation
becomes more conscious of the deleterious effects of eutrophication and
mitigating technologies mature. Point sources such as municipal waste-
water utilities are easy and effective targets for regulation and control.
Partial removal of N as part of municipal wastewater treatment is
currently a common practice to reduce nutrient load to surface water
(USEPA, 2007). Existing targeted N removal methods primarily facilitate
the decomposition by microbial consortia of complex nitrogenous com-
pounds into ammonium (NHþ 4 ) and then oxidation to atmospheric ni-
trogen gas (N2) (Clark et al., 2010); nitrification-denitrification is the
most common example while sidestream partial nitrification-anammox is
an emerging technology (van Dongen et al., 2001, Fux et al., 2002,
Kampschreur et al., 2009; Clark et al., 2010, Eini 2012). The
nitrification-denitrification and anammox processes require energy in
the form of electricity for aeration and secondary processes like mixing.
Nitrification-denitrification also requires a carbon (C) source for energy
and biomass; this C is typically derived from extant organic molecules
and thus serves to decrease biological oxygen demand (USEPA, 1973).
Some reactors add an external organic substrate, such as methanol, to
improve N removal (USEPA, 1973; Purtschert et al., 1996; Theis and
Hicks, 2012).
Stoichiometrically, anammox requires only 50% of NHþ 4 to be
oxidized to nitrite (NO2 ) but 57% is considered ideal (Magri et al., 2012).
Anammox requires roughly one-third of the oxygen as
nitrification-denitrification and no C amendment for the same NHþ 4
removal, but is incapable of processing nitrate (NO 3 ) (Eini, 2012).
Anammox reactors are well-suited for side stream processing (USEPA,
2007) of anaerobic digester effluent liquids and can achieve high N
removal rates (Lu et al., 2011; Nifong et al., 2013). Both technologies run
the risk of releasing powerful greenhouse gases in the form of methane
(CH4) and nitrous oxide (N2O), depending on reactor conditions
(Kampschreur et al., 2009; Law et al., 2011).
Electrodialysis with monovalent-selective membranes is a newly
patented technology (Barak, 2018) to recover NHþ 4 directly from waste-
water and concentrate it for reuse as fertilizer. Electrodialysis is a mature
desalination technology that uses an electric field to transport ions
through ion-permeable membranes (Pruyn et al., 1969). The electrodi-
alysis stack typically consists of alternating cation- and anion-exchange

* Corresponding author.
E-mail address: phillip.barak@wisc.edu (P. Barak).

https://doi.org/10.1016/j.cesys.2021.100026
Received 30 November 2020; Received in revised form 15 March 2021; Accepted 19 March 2021
2666-7894/© 2021 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
D. Vineyard et al.
membranes (CEM, AEM) separated with spacers, with inert electrodes on
each end by which an electrical field is applied to the stack. As aqueous
solution flows between these specialized membranes, ions of the influent
stream are separated into an enriched concentrate stream and a partially
desalinated diluate stream. Electrodialysis can be an energy-efficient
method of concentrating ions but solutions with high electrical resis-
tance or large desalting goals can affect stack performance.
Electrodialysis has been previously explored as a method of removing
NHþ 4 ions from municipal wastewater (Eisenmann and Smith, 1967; Ali
et al., 2004; Ippersiel et al., 2012; Gurreri, 2020; Vineyard et al., 2020),
but the process was hampered by accumulation of calcium (Ca2þ) and
magnesium (Mg2þ) scale on membranes that blocked ion flow. To
minimize energy costs, this sidestream electrodialysis technology is
intended to be applied to high-NHþ 4 , low-C feeds such as filtered liquids
from biosolids after anaerobic digestion. In contrast to other N removal
technologies, electrodialysis recovers an aqueous NHþ 4 product that has
potential use as an N fertilizer.
Typical N fertilizers are derived from the Haber-Bosch process, a re-
action that converts atmospheric N2 gas and hydrogen gas into ammonia
(NH3) using a metal catalyst and high temperatures. This reaction re-
quires use of fossil fuel in the form of methane, a large industrial facility,
and a broad scale transportation network. By recapturing NHþ 4 at treat-
ment plants for use in local agriculture, an electrodialysis stack can
theoretically offset the costs and environmental impacts of producing an
equivalent amount of industrial NH3. Electrodialysis will also recover
other monovalent ions such as potassium (Kþ), sodium (Naþ), and
chloride (Cl) in amounts that will vary depending on the composition of
the feed and selectivity of the ion exchange membranes. Of note, these
membranes will also exclude polyvalent heavy metal ions, previously
identified as a key risk in municipal nutrient recovery technologies (Fang
et al., 2016; Lam et al., 2019).
Life cycle assessment (LCA) has been used previously to evaluate the
environmental impacts associated with wastewater treatment (Guest
et al., 2009; Byrne et al., 2017). The wastewater treatment sector is
exploring the benefits of resource recovery as part of the global shift
towards sustainability and circular economies (Guest et al., 2009). While
some studies focus on water (Fang et al., 2016) or energy recovery (Hao
et al., 2019), the myriad of emerging nutrient recovery technologies are
an ongoing area of research (Lebuf et al., 2012; de Faria et al., 2015;
Malila et al., 2019; Sena and Hicks, 2018; Lam et al., 2019).
Nitrogen-specific recovery technologies (Lin et al., 2016) receive less
focus in the literature as most technologies recover a combined N and P
product (Lam et al., 2019). While other N recovery technologies exist in
various stages of implementation, we are aware of none that are wide-
spread or industry standard. A literature review found no previous LCA
studies of electrodialysis for nitrogen recovery.
2. Methods
2.1. Goal and scope definition
The goal of this study was to evaluate an emerging wastewater N
recovery technology and compare the life cycle impacts to existing N
removal methods. We evaluate four different municipal N management
strategies: (1) Do nothing; (2) Nitrification-denitrification; (3) Anam-
mox; and (4) Electrodialysis for NHþ 4 recovery. We built life cycle in-
ventories for the purpose of profiling their environmental impacts using
LCA.
This study is an expansion of Vineyard et al. (2020), which focused on
comparative economic and energy performance of electrodialysis for
these same technologies. Though cost is typically the major deciding
factor for municipalities mandated to implement nutrient removal, such
mandates are ultimately written with the goal of improving environ-
mental quality, which can be evaluated using LCA with standard prac-
tices outlined in ISO 14040 (ISO, 2006) and 14044 (ISO, 2006). This
study is intended for wastewater engineers and policymakers to consider
2
Cleaner Environmental Systems 2 (2021) 100026
environmental impacts of new and existing technologies to achieve
increased N removal goals; while technologies have immediate practical
considerations on-site, their environmental benefits ripple out.
We used the OpenLCA 1.8 software package (GreenDelta, Berlin,
Germany) and the ecoinvent 3.5 database (Wernet et al., 2016) to build
the life cycle inventory and apply impact assessment methods. OpenLCA
was chosen for flexibility and ease of use. Where possible, U.S.-specific
processes were chosen. To interpret the inventory, we used the
midpoint categories of the USEPA's Tool for the Reduction and Assess-
ment of Chemicals and other environmental Impacts (TRACI) version 2.1
(Bare, 2011) packaged with OpenLCA. TRACI was chosen for its high
regard and ubiquity in LCA literature and for its comprehensive range of
midpoint environmental impacts for comparison, but it should be noted
that the characterizations were also U.S.-specific.
When wastewater specifics were necessary, data were taken from the
Nine Springs Wastewater Treatment Plant in Madison, Wisconsin, a mid-
size treatment plant that serves a population of 360,000 over a 180 sq.
mile (466 km2) service area, with a design capacity of 50 million gallons
per day (50 MGD; 189,000 m3/day) (AECOM, 2015). This plant contains
a mesophilic anaerobic digester and dewaters its anaerobic digestor
sludge to produce biosolids using a gravity belt thickener (GBT). The
liquid stream separated out by GBT for recycling to the headworks is high
in nutrients and well-suited for side-stream treatment processes such as
anammox or electrodialysis, but can also be returned to headwaters or
fed directly to nutrient removal reactors. Our technologies are assumed
to be fed the high nutrient liquid stream from this stream. The total GBT
filtrate flow is 0.25 MGD, or 946 m3/day, and averages 1437 mg/L
NHþ þ þ
4 -N, 214 mg/L K , and 256 mg/L Na for 103 meq/L, 5.47 meq/L,
and 11.1 meq/L, respectively. Electricity is assumed to be of low voltage
from the U.S. characterized by data from the Midwest Reliability Orga-
nization (MRO), one of the eight regional electric reliability councils
under the North American Electric Reliability Corporation (NERC).
In the literature search, publications were mined for reactor perfor-
mance data to be incorporated into a master list. If a single publication
reported data from multiple reactors, those reactors were given equal
weight in the list. When publications did not directly report the values
needed, values were instead calculated from available data within the
same publication; missing data were filled with the aggregate average of
publications that reported the needed upstream data. In condensing this
distribution to singular unit processes for an OpenLCA input, the geo-
metric mean of values was used for the process inventory. Full values are
contained within the SI for further exploration. The intention of this
method was to create a process representative of the real world by taking
surveyed data from multiple publications. This assumes that studied and
surveyed plants are representative of plants as a whole and that the data
collection methods have comparable results.
We performed an uncertainty analysis for discussion characterizing
the potential impacts of the variability in literature values and addressing
possible alternative assumptions. High and low values from literature are
used to put boundaries on emissions and energy and material con-
sumptions for traditional technologies. Electrodialysis alternatives
address varied operating conditions and necessary material inputs as
suggested by Vineyard et al. (2020) from electrochemical modeling and
literature review. We use these values to create new inventories and
reassess them for the same environmental impacts. Differences between
scenarios are highlighted with comment to potential causes, effects, and
probabilities.
2.2. Functional unit
Our work assumed that new technology would be implemented with
the intention of meeting a nutrient removal goal and as such uses a mass
basis for N removed; this allows decision-makers to directly compare the
estimated impacts incurred by meeting their goals and then size their
reactors appropriately. The functional unit for comparison in this study
was a single kilogram (kg) of NHþ4 -N removed, a metric with precedent in
D. Vineyard et al. Cleaner Environmental Systems 2 (2021) 100026

nutrient recovery LCA (Byrne et al., 2017; Lin et al., 2016). Comparisons
were performed based on total supply chain environmental impacts, with
highlights on the local energy consumption and fugitive emissions due to
their high impacts.

2.3. System Boundaries

All three technologies embody high energy consumption, material

consumption, and/or fugitive emissions, have relatively simple con-
struction and disposal, and are expected to have useful lifetimes in excess Fig. 2. Intervention point.
of 20 years. Construction and disposal impacts are expected to be
negligible compared to 20 years of operation impacts (see Supplemental
water supplies, fisheries, and recreation usability, a targeted IPCC report
Information). As such, this was a gate-to-gate study beginning with the
estimated that 0.01 kg N2O-N is emitted to the atmosphere for every kg of
entry of wastewater N into the reactor and ending with the N leaving that
N released to rivers (IPCC, 2000); as TRACI does not include a global
reactor to the environment (Fig. 1). The intervention point for the side
warming characterization factor for NHþ 4 to surface water, we supple-
stream technologies is the high-nutrient liquid effluent from an anaerobic
mented the IPCC value. One kg of NHþ 4 -N, for our purposes equated to
digester (Fig. 2). We assumed that removal of N from a small side stream
1.29 kg of NHþ4 ions and 0.0157 kg of N2O gas.
is equivalent to removal from a large stream, effectively disregarding
scalability and total nutrient removal potential in favor of marginal
2.4.2. Nitrification-denitrification
impact of nutrient removal. This assessment allocated all impacts of the
The second scenario, nitrification-denitrification, is a traditional N
process to nutrient removal, disregarding the effects of any secondary
removal technology that uses large cisterns and pumps to move and
benefits and externalities within other plant processes, such as
aerate process water through a series of aerated (oxic) and anoxic zones.
decreasing biochemical oxygen demand (USEPA, 1973) or reduced
We used a value of 3.20 kWh per kg of N removed for electricity to run
digester inhibition by ammonium (Hansen et al., 2004; Calli et al., 2005).
pumps and aerators (SI, Table 1A). For methanol, we used the stoichio-
While there are no existing nitrogen recovery technologies in place to
metric ratio for heterotrophic digestion of 2.44 kg methanol per 1 kg of
compare, comparing removal to recovery processes is made possible by
NO 3 -N, which is metabolized to 2.40 kg of CO2 (Rittmann and McCarty,
the inclusion of the fertilizer offset (ISO, 2006). The production of
2001; Theis and Hicks, 2012). These values are similar to the 3.5 kWh
fertilizer-quality N is accounted as an offset of its nearest industrial
and 3.1 kg of methanol per kg N calculated by the Chesapeake Bay Pro-
analog, ammonia.
gram for marginal reduction of the effluent from 8 to 5 ppm N (2002).
In accounting for fugitive N2O emissions, the nitrification-
2.4. Scenario description
denitrification model considered values from a number of studies and
metastudies (SI, Table 2A). Many publications reported fugitive emis-
2.4.1. Do nothing
sions per N influent in various units, requiring conversion. Two publi-
The default scenario is a simple release of treated wastewater N to
cations (Wicht and Beier, 1995; Foley et al., 2010) contained a combined
surface water through effluent discharge, the bar against which other
70 data points, but were treated as a single data point due to inaccessi-
scenarios are compared. In this scenario, the N leaves the sidestream
bility of associated data. The uncertainty distribution removed two out-
untreated and re-enters the main treatment train where it will eventually
liers from both the top and bottom of the emissions profile. Despite being
be discharged from the plant. This N will then be utilized by plants and
an anoxic, metabolically active, and C-containing environment, we did
microbiota in natural waters. No energy consumption is required in this
not expect methane (CH4) emissions from the denitrification process
scenario. In addition to eutrophic effects of excess nutrients on drinking

Fig. 1. System boundaries.

3
D. Vineyard et al. Cleaner Environmental Systems 2 (2021) 100026

(Westermann and Ahring, 1987; Islas-Lima et al., 2004; Ettwig Katharina
et al., 2008).
2.4.3. Anammox
Energy consumption data were obtained from Maurer et al. (2003),
WSHD (2012), and Lackner et al. (2014), through Hauck et al. (2016),
where the geometric mean was 1.44 kWh/kg N (SI, Table 3A). The N2O
emission data for anammox reactors were taken from literature values
(SI, Table 4A) and averaged 0.0209 kg N2O/kg N; anammox was not
expected to yield fugitive CH4 emissions. It should be noted that the
relationship between reactor conditions and fugitive emissions is not yet
well understood and might be improved by alternative reactor schemas
and aeration regimes (Domingo-F
elez et al., 2014).
2.4.4. Electrodialysis
An electrodialysis stack is a relatively simple machine composed of a
pump, electrodes, and hydrocarbon-based membranes. The electrodial-
ysis membranes are predicted to have a lifetime of 10 years (Vineyard
et al., 2020; AECOM, 2015). Other components are not expected to
require unusual maintenance or replacement. The impacts of this stan-
dard upkeep are expected to be negligible compared to the high elec-
tricity consumption and fertilizer offset. The manufacture and disposal of
the unit is expected to be similarly negligible. In an electrodialysis stack,
the total energy consumption is the product of the voltage and the
electric current. The relationship between these stack conditions and
resultant voltage is a complicated one. Vineyard et al. (2020), a com-
panion article to this study, predicted that an economically optimal stack
of in our assumed conditions would consume 2.36 kWh/kg N. This value
represented an optimal profit method of current selection and was pre-
dicted to remove roughly 41.6% of NHþ 4 from the stream in a single stage
of treatment.
As electrodialysis is also a N recovery technology that produces
fertilizer-quality NHþ 4 , this process contained an offset of 1 kg of N in
NHþ 4 for each kg of N removed, manifested here as an input of negative
production. Ammonia was chosen as the offset fertilizer because it is the
direct chemical analogue to the NHþ 4 salts produced. No weight, positive
or negative, was given to K, Na, bicarbonate or chloride byproducts. The
ecoinvent library's market option for NH3 was chosen for the inventory
flow. No N2O or CH4 emissions from the electrodialysis process were
expected.
3. Inventories and impacts
The life cycle inventories of the four scenarios (1) Do nothing; (2)
Nitrification-denitrification; (3) Anammox; and (4) Electrodialysis for
NHþ 4 recovery are shown in Table 1. Looking at the inputs, electrodialysis
used 74% of the electricity of an equivalent capacity nitrification-
denitrification reactor; an anammox reactor used 40%. Only
nitrification-denitrification required a chemical methanol input and its
conjugate respiration to CO2 as an output. Only electrodialysis generated
a fertilizer offset, shown here as a negative ammonia liquid input.
Considering the outputs, electrodialysis generated no fugitive N2O
emissions; emissions were three times higher for an anammox reactor
than a denitrification reactor and twice as high for the do nothing sce-
nario, which also was the only scenario with an ammonium ion output.
Electrodialysis is the most environmentally favorable technology in
six of ten environmental impact categories considered (Table 2), with
anammox having a narrow advantage in the other four. The offset of
industrial NHþ 4 production in the electrodialysis model led to a net
negative impact, i.e., an environmental benefit, in five of the impact
categories, while the combination of high electricity usage with meth-
anol consumption in the nitrification-denitrification model led to the
largest impact in every TRACI category tested except for eutrophication.
All N removal strategies generated lower eutrophication than the Do-
Nothing scenario by two orders of magnitude. While allowing the N to
discharge freely into the environment did generate global warming po-
tential through the generation of N2O, both nitrification-denitrification
and anammox generated higher total global warming impacts from the
combination of fugitive emissions and energy consumption due to aera-
tion. Fossil fuel depletion, acidification, and smog production were
strongly impacted by methanol production and the fertilizer offset. The
toxicity emission categories of carcinogens, non-carcinogens, ecotoxicity,
and respiratory effects were electricity-dominated effects.
The four scenarios had significant differences in their greenhouse gas
(GHG) profiles (Fig. 3). NHþ 4 discharge to surface water bodies in the do-
nothing scenario was predicted to result in significant N2O generation.
The nitrification-denitrification process had double the electricity-
related emissions of anammox, as well as additional methanol produc-
tion and respiration emissions, but it emitted a third of the N2O of
anammox and less than half the N2O of a surface water discharge.
Fugitive N2O generation dominated the global warming profile of the
anammox process. Despite requiring no C substrate and less oxygenation
than nitrification-denitrification, anammox showed only an 11% savings
against nitrification-denitrification. By contrast, electrodialysis was not
projected to generate N2O and the offset of NHþ 4 production eliminated
methane-related emissions from the supply chain. Greenhouse gas
emissions from its moderate energy consumption were outweighed by
offsets in NHþ4 production.
4. Discussion
4.1. Uncertainty analysis
Each of the four scenarios had uncertainty in at least one input or
output due to the range of literature reported values. In order to address
this uncertainty, we selected literature values as alternative LCA inputs
and outputs (Table 3) to assess the effects on predicted environmental
impacts (Tale 4). These alternative models were intended to help
conceptualize the ranges of possible emissions profiles from real world
implementation. The SI contains tables with a more detailed accounting
of the data sources and uncertainty (Tables 1A–4A) and modeling of
additional scenarios (Tables 5A–12A).

Table 1
Flows of the models of scenarios removing 1 kg of N.
I/O Flow Do Nitrification- Anammox Electro- Provider/Category
Nothing Denitrification dialysis

Inputs Ammonia, liquid (kg) – – – 1.21 market for ammonia, liquid j ammonia, liquid j APOS, U - RER
Electricity, low voltage – 3.20 1.44 2.36 market for electricity, low voltage j electricity, low voltage j APOS,
(kWh) U - MRO, US only
Methanol (kg) – 2.44 – – market for methanol j methanol j APOS, U - GLO
Outputs Ammonium, ion (kg) 1.29 – – – Emission to water/unspecified
Dinitrogen monoxide 0.0157 0.00647 0.0209 – Emission to air/unspecified
(kg)
Carbon dioxide, fossil – 2.40 – – Emission to air/unspecified
(kg)

4
D. Vineyard et al. Cleaner Environmental Systems 2 (2021) 100026

Table 2
Environmental impact results per kg NH4-N removed.
Impact category Unit Do nothing Nitrification-denitrification Partial nitrification-anammox Electro-dialysis
-3
Acidification kg SO2 Eq (10 ) – 12.2 3.02 2.63
Carcinogenics CTUh (109) – 250 91.7 107
Ecotoxicity CTUe – 52.8 19.7 23.7
Eutrophication kg N Eq (10-3) 1002 20.9 8.27 11.2
Fossil Fuel Depletion MJ surplus – 14.1 0.715 6.05
Global Warming kg CO2 Eq 4.68 8.10 7.23 0.810
Non-Carcinogenics CTUh (109) – 1100 335 218
Ozone Depletion kg CFC-11 Eq (10-9) – 775 83.6 440
Respiratory Effects kg PM2.5-Eq (103) – 7.38 3.04 3.85
Smog kg O3 Eq (10-3) – 133 27.0 23.6

Fig. 3. Comparison of global warming potential by energy consumption and fugitive emissions between the three N removal technologies for the removal of 1 kg of
NH4-N.

appropriately included in the impacts. This alternative accounting would

A recent metastudy (Hu et al., 2013) strongly suggested that the IPCC
(2000) estimate of fugitive N2O from surface water discharged NHþ 4 is an
overestimate and that a more representative emission factor might be as
low as 0.0016 kg. If the Hu et al., 2013 data were correct, then the
Do-Nothing scenario might have a much smaller global warming impact
of 0.75 kg CO2-Eq/kg N, an 84% reduction. This would reduce the
Do-Nothing scenario to the lowest global warming impact among the
options, with the exception of the electrodialysis stack that recycles the N
to fertilizer to offset NHþ4 production. The oxidation reaction of NH4 to
þ
NO 3 in a natural waterway stoichiometrically results in a net two
hydrogen ions produced per NHþ 4 ion oxidized. Literature estimated that
half of this NO 3 will undergo plant uptake with an equivalent amount of
alkalinity production upon assimilation (Havlin et al., 2014), leading to a
potential net of 1 mol of Hþ per mole of NHþ 4 ; as the acidification impact
category includes effects on natural waterways, this pH change might be
make doing nothing a greater acidifier than any other option by multiple
orders of magnitude.
Nitrification-denitrification had a range of alternative energy con-
sumptions and fugitive emissions reported in literature. Both high and
low reported values were tested alongside a nitrification-denitrification
basin that did not require methanol as a C substrate. In a standard
nitrification-denitrification reactor, methanol was found to account for
over half of the global warming impacts and two-thirds of acidification,
fossil depletion, and non-carcinogenic human health impacts due to both
the industrial production itself and the eventual oxidation to CO2;
reducing the usage of methanol equivalently reduced these emissions.
Methanol sourced from a non-fossil C substrate such as food waste or
sludge cycled from another plant stream might also lower the global
warming impacts as the eventual decomposition would not result in a net
GHG increase; an alternative C source might even be allocated an offset of
the disposal costs for such a substrate. Fugitive N2O emissions ranged
from insignificant (<0.5 kg CO2-Eq/kg N) to completely dominant over
the GHG profile (>28 kg CO2-Eq/kg N). Variability in reported electricity
usage did not dramatically affect results; the difference between the
lowest (2.5 kWh/kg N) and highest (4.17 kWh/kg N) reported energy
consumptions was about 1 kg CO2-Eq/kg N.
Anammox had a distribution of literature values similar to
nitrification-denitrification. The lowest N2O emitting reactors showed
fugitive emissions as only 20% of the total GHG profile (0.26 kg CO2-Eq),
while the highest emitting reactors showed fugitive GHG emissions forty
times higher than energy based GHG emissions (41 kg CO2-Eq). The

5
D. Vineyard et al. Cleaner Environmental Systems 2 (2021) 100026

highest estimate for an anammox reactor (41.8 kg CO2-Eq/kg N) pre-

Recovery
dicted more greenhouse gases than the highest estimate for nitrification-
denitrification (34.6 kg CO2-Eq/kg N). The highest electricity consump-

2.36
No
tion in an anammox reactor (4.17 kWh/kg N) was equivalent to the

–
–

–
highest electricity consumption in a nitrification-denitrification reactor.
Govern This suggested that reactor performance was of particular importance to

1.21

2.04t
Mc-

anammox reactors as poor function leading to fugitive emissions can

–
–

–
eliminate expected technological gains from energy savings. It was also
possible that the mesophilic bacteria require additional energy for heat
Limiting
Current

pumping in some reactors where prior digestion does not create warm
1.21

3.67
enough conditions, though data of this level of detail were not provided
Electrodialysis

–
–

–
in-source.
Default

Electrodialysis with the economically optimal current as predicted by

1.21

2.36

Tanaka (2015) (2.36 kWh/kg N) (Vineyard et al., 2020) was the scenario
–
–

–
considered, but four alternative energy consumption values were tested:
0.00088

energy consumption at the limiting current density model (3.67 kWh/kg

N) (Vineyard et al., 2020); energy consumption at maximum hourly
1.44
N2O
Low

–
–

profitability (3.09 kWh/kg N); energy consumption at optimal cost as

predicted by an alternative model (2.04 kWh/kg N) (McGovern et al.,
0.137
High

1.44
N2 O

2014); and energy consumption for a chloride targeting analogue

–

–
–

considered in a vendor proposal (2.42 kWh/kg N) (AECOM, 2015),

0.0209
Energy

covered in the SI. The vendor proposal included acid usage to remove
Low

0.8

mineral scale.
–

–
–

Each of these scenarios showed changes in impacts proportionate to

0.0209
Energy

the change in electricity usage; acid addition played a qualitatively

High

4.17

insignificant role in the vendor scenario. Three alternative energy mixes

–

–
–

were also tested in the SI: the Midwest Reliability Organization, the
Anammox

Default

0.0209

Western Electric Coordinating Council, and the Northeast Power Coor-

1.44

dinating Council. The Midwestern mix was found to be the greatest GHG
–

–
–

emitter (0.577 kg CO2-Eq/kg N after methanol offset), likely owing to

Methanol

the disproportionate use of coal in the Midwest region.

0.00647

The offset of industrial ammonia production is a large contributor to

3.2
No

the emissions profile of electrodialysis. Photochemical oxidation, acidi-

–

–
–

fication, and global warming impacts are the most sensitive to the offset.
0.00023

If captured ammonia is not used to offset industrial fertilizer, modeled in

2.44
N2 O
Low

3.2

2.4

the No-Recovery scenario, global warming impacts would be positive and

–

more than double the reported magnitude; acidification and oxidation

would be four and six times their reported magnitudes, respectively. In
0.0953
High

2.44
N2 O

the ozone depletion, eutrophication, and non-carcinogenic human health

3.2

2.4
–

categories, the impacts of energy consumption are negligible compared

to the offset, while in the respiratory effects and ecotoxicity categories
0.00647
Energy

the offsets are of a lower magnitude compared to the impacts of energy

2.44
Low

2.5

2.4

consumption. Without the ammonia recovery offset, N removal by elec-

Nitrification-Denitrification

trodialysis would have a larger impact than anammox in every category

except global warming. As a final test, ammonia fertilizer was replaced
0.00647
Energy
High

4.17

2.44

with the common fertilizer urea (SI), which resulted in higher offsets in
2.4
–

each category and net negative emissions of greater magnitude in the

cumulative results.
0.00647
Default

2.44
3.2

2.4

4.2. Additional considerations

–

0.00251

Electrodialysis run at optimal cost efficiency was projected to

Lower
Alternative flows of N management processes.

1.29
N2O

consume more electricity per kg of N than an anammox reactor, but the

–

–
Do Nothing

increased energy consumption was offset in the supply chain by the

avoided industrial ammonia production; though a utility will not expe-
Default

0.0157
1.29

rience these energy savings itself, it may be able to pursue a grant or

–

subsidy for benefits to the local market.

An electrodialysis stack can theoretically concentrate NHþ 4 with
Ammonia, liquid

Ammonium, ion

Carbon dioxide,
Electricity, low

equimolar chloride and bicarbonate up to the saturation point of about

monoxide (kg)
voltage (kWh)
Methanol (kg)

4 M, 6% N by mass, before precipitation and scaling begin at 20  C

Dinitrogen

fossil (kg)

(Barak, 2018; unpublished data). The product would be a dilute liquid

Flow

fertilizer composed of NHþ

(kg)

(kg)

4 with chlorides and bicarbonates. Though this

product would avoid typical waste-derived fertilizer concerns about the
over application of phosphorus, there will be concerns regarding excess
Outputs
Table 3

Inputs

chloride application. Compared to anhydrous ammonia (82%), urea

I/O

(46%), or even aqua ammonia (20%), a 6% solution would incur greater

6
D. Vineyard et al.
transportation, storage, and application costs as a fertilizer. These costs
might be offset by a much shorter transportation distance between pro-
duction and application. Comparing a 6% solution to a 46% urea load
suggests 7.8 times the transportation costs both environmentally and
economically. With a rough, ecoinvent-based estimate of 0.22 kg CO2-Eq
per 1000 kg-kilometers transported, the kg of electrodialyzed N incurs
3.19 extra kg of CO2-Eq per 1000 km compared to urea. It would take an
average facility-to-farm transport distance of over 750 km by truck to
invalidate the industrial ammonia offset in the comparison. Volatilizing
and condensing recovered N as ammonia or ammonium bicarbonate
would increase electricity costs but reduce transportation costs. Though
construction-phase impacts were expected to be negligible, other studies
of different scopes and methods (Lin et al., 2016; Hao et al., 2019) have
suggested the high concrete, steel, and fuel consumption in construction
may be significant. Accounting for these impacts would likely widen the
gap between electrodialysis and traditional technologies.
Short and long term effects of membrane scale and fouling remain an
unresolved issue here. Eisenmann and Smith (1967) also found that
membranes rapidly scaled with Ca and Mg under operating conditions.
Electrodialysis also faces potential membrane fouling from trace organic
material. Wastewater, even post-treatment, contains high levels of
complex biologically-derived C molecules. These molecules tend to
behave as if they were strongly negatively charged and so interact with
an electrodialysis current, forming a layer of sorbed organic molecules on
the membranes that will impede ion flow (Oztekin and Altin, 2016).
Scale, whether organic or inorganic, may dramatically increase energy
costs by increasing electrical resistance. Prevention and remediation of
scale within the electrodialysis chamber might require pretreatment of
the solution either to remove solutes before precipitation or prevent their
detrimental effects on the electrodialysis process. Pretreatment could
have impacts to both the reactor's environmental life cycle inventory and
to the function of the whole treatment plant. Monovalent-selective
membranes are expected to vigorously exclude the large, highly
charged organic molecules in a fashion that should prevent fouling and
reject the Ca and Mg ions that cause mineral scaling. Future work should
investigate the performance of reactors in broader operating conditions,
particularly with respect to scale formation and membrane fouling.
Given the complex interrelations of wastewater treatment processes,
there may be unforeseen externalities to implementation of these tech-
nologies not captured in this study. Some wastewater treatment systems
may not have suitable influent for processing, may have side stream
processes incompatible with new nutrient removal, or may have existing
products degraded or reactors impeded by nutrient removal. It is also
possible that N removal in-plant can reduce the occurrence of ammonia-
toxicity in municipal sludge digesters (Desloover et al., 2012; Desloover
et al., 2015); improved digester performance can decrease end waste
mass and cost, while yielding higher biogas recovery for on-site energy
generation (Karim et al., 2005; Gungor and Karthikeyan, 2008; Holly
et al., 2017). Current allocation methods disregard any costs or benefits
of pathogen reduction or C removal in the reaction. Future analysis
would benefit greatly from a characterization of the interaction between
N removal processes and overall treatment plant performance, particu-
larly in the emission of fugitive GHGs and aeration energy requirements
of main stages. An expanded scope would be within the recommenda-
tions of Corominas et al. (2013).
5. Conclusions
Based on these theoretical LCA results, N removal and recovery by
unimpeded electrodialysis appear to be far and away the preferable
environmental choice of N removal technologies, projecting net negative
impacts in key categories including GHG emissions and fossil fuel
depletion. Electrodialysis is predicted to consume 64% more electricity
than an equivalent capacity anammox reactor but 26% less than a
nitrification-denitrification reactor. Models of aeration-based N removal
technologies, particularly anammox, were found to be extremely
7
Cleaner Environmental Systems 2 (2021) 100026
sensitive to fugitive N2O emissions, suggesting that proper reactor
function should be a top priority for operators seeking to reduce global
warming impacts.
Declaration of competing interest
The authors declare the following financial interests/personal re-
lationships which may be considered as potential competing interests:
One of the authors, Phillip Barak, is a co-owner of Nutrient Recovery and
Upcycling, LLC, which is rights holder to US Patent 10,125,428 (issued
Nov. 13, 2018) for the removal of nitrogen from wastewater using
monovalent-selective electrodialysis, with international patent applica-
tions pending. This work was funded by the United States Department of
Agriculture/National Institute of Food and Agriculture through Hatch
Project No. WIS01920 and INFEWS/T3 (Project No. 2017-67003-26055).
We thank the Nine Springs Wastewater Treatment Plant and the Madison
Metropolitan Sewerage District for providing plant and reject water
specifications.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.cesys.2021.100026.
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