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Keywords: Carbon dioxide (CO2) supply is an important consideration for algae production systems, and using high-purity
Algae CO2 eliminates the need for purification processes. This study assessed the challenges and opportunities inherent
High-purity carbon dioxide in using waste high-purity CO2 to produce algae in the United States. The United States’ upper Midwest region is
Life-cycle assessment
rich in high-purity CO2 from corn ethanol production. However, its climate is not as favorable for algae pro
Greenhouse gas emissions
duction as that on the Gulf Coast. This study assessed the tradeoffs between these factors by comparing algae
Water stress
biofuel production with and without high-purity CO2 across these two regions. Monthly algae cultivation was
modeled in open ponds co-located with high-purity CO2 sources in the Midwest and along the Gulf Coast, where
many steam methane reforming and ammonia production facilities are located. This revealed that, by avoiding
the energy-intensive carbon-capture process, an algae site that sources carbon from a high-purity CO2 source
would achieve a 9–39% reduction in life-cycle greenhouse gas (GHG) emissions and a 9–37% reduction in life-
cycle fossil energy use compared to a similar site using dilute CO2 for algae cultivation. The results also suggest
that during warm months an algae pond in the Midwest would achieve results that are comparable to GHG
emissions from a pond on the Gulf Coast. Furthermore, several Midwest algae ponds investigated in this study
create less local water stress than those located along the Gulf Coast. The abundant high-purity CO2 from corn
ethanol plants thus creates a potential opportunity for algae cultivation in the Midwest. This study illustrated the
interplay between algae productivity, CO2 delivery, GHG emissions, and water stress in siting algae ponds.
* Corresponding author. ,
E-mail address: thawkins@anl.gov (T.R. Hawkins).
https://doi.org/10.1016/j.jclepro.2021.128779
Received 9 March 2021; Received in revised form 4 August 2021; Accepted 21 August 2021
Available online 23 August 2021
0959-6526/© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
and 90% of this comes from ethanol fermentation (Edwards and Celia, framework that captures site-specific environmental conditions, pro
2018). The abundance of high-purity CO2 in the Midwest thus provides duction potential, and resource requirements for bioenergy feedstocks
significant opportunities for carbon capture, utilization, and storage by coupling advanced spatial and numerical models. This study used
(CCUS). CO2-enhanced oil recovery (CO2-EOR) is the most prevalent BAT for land suitability-based algae siting and physics-based modeling
CCUS practice in the world today, accounting for 90% of the anthro of biomass production and water consumption at the algae sites. BAT
pogenic CO2 emissions captured and stored each year, and it mainly reported monthly and annual average algae growth rates and water
occurs in the United States (Edwards and Celia, 2018). consumption for each site; these are important inputs for estimating
However, most Midwestern ethanol facilities are located far away lifecycle GHG emissions and water consumption.
from existing CO2 pipelines, major oil fields, and potential saline storage This study used BAT to simulate freshwater algae growth in a 15-cm-
reservoirs. Transporting captured CO2 from the Midwest to regions deep open pond at each site. The growth rates of three strains of
where there is demand for EOR requires the development of a regional microalgae were modeled as a function of light intensity and tempera
pipeline network and significant investment (Edwards and Celia, 2018). ture under nutrient-replete conditions: (1) Chlorella sorokiniana, (2)
A recent survey of commercial ethanol plant survey revealed that only Monoraphidium minutum, and (3) Scenedesmus obliquus. The three algal
14% of respondents currently capture high-purity CO2 for use (Wu, strains were originally selected as a part of the National Alliance for
2019). Algae used for valuable fuel or products would generate revenue Advanced Biofuels and Bioproducts (Olivares et al., 2014) based on their
while reducing the carbon footprint of corn ethanol. performance under varying climatologies. The strains included a
Although Midwest states are not generally considered favorable for warm-season strain (Chlorella sorokiniana [DOE 1412]; 30–40 ◦ C) which
algae production due to their cold winters and the potential for algae is a naturally occurring strain isolated from a natural freshwater source
production to compete with agricultural land uses, algae production in Texas, a cold-season strain (Monoraphidium minutum; 10–30 ◦ C), and
near ethanol facilities on marginal lands or lands that are unsuitable for an all-season strain (Scenedesmus obliquus; 18–40 ◦ C). These strains have
farming provides another option for utilizing the abundant high-purity undergone extensive lab experimentation for parameterization into a
CO2 in the region. Water consumption is another important issue for microalgae growth model. The microalgae growth model results for the
algae cultivation (Xu et al., 2019), and some Midwest locations may set of strains have been validated as described in Sun et al. (2020) and
offer favorable hydrological conditions for algae production, unlike the original selection (Huesemann et al., 2013) and growth model
some warmer, dryer sites. testing and validation (Huesemann et al., 2016) are also described in
On the other hand, warmer regions such as the Gulf Coast and previous studies.
northern Florida are generally considered favorable for algae produc BAT adopts a strain rotation strategy for each site to select and retain
tion. Algae facilities along the Gulf Coast could potentially use high- the most productive strain in each month (Sun et al., 2020). Each pond
purity CO2 from ammonia and SMR facilities. However, they are likely site yielded a potentially unique combination of strain by month,
to face strong competition for high-purity CO2 because the CO2-EOR depending largely on local meteorology. The strain rotation strategy
industry is already well-established in this region. Florida has highly reduced seasonal variability in biomass productivity and improved
suitable conditions for algae cultivation (ANL, NREL, and PNNL, 2017), overall annual biomass productivity (Sun et al., 2020). Other aspects of
but it does not have significant industrial sources of high-purity CO2. BAT, including land screening criteria, calculation of water usage, and
Therefore, it is useful to understand the opportunities and challenges CO2 demand, are introduced in the Supporting Information (SI).
for the potential uses of waste high-purity CO2 for algae production in
the United States. This study contributes to this discussion by consid 2.2. High-purity CO2 sources
ering the interplay between algae productivity, CO2 delivery, and water
stress. In particular, it assessed whether the availability of high-purity This study considered three categories of high-purity (>95%) CO2
CO2 in the Midwest compensates for its relatively less favorable algae sources in the United States: natural gas SMR facilities, ethanol facilities,
growth conditions. For this purpose, algal hydrothermal liquefaction and ammonia-production facilities (Langholtz et al., 2016). The location
(HTL) biorefineries were modeled in eight states where high-purity CO2 and annual emissions of high-purity CO2 from SMR and
is abundant. HTL was selected as the conversion technology for biofuel ammonia-production facilities were obtained from the Environmental
production because it is suitable for processing high-moisture feedstock Protection Agency 2018 Greenhouse Gas Reporting Program (GHGRP)
like algae (Ou et al., 2015). dataset (U.S. Environmental Protection Agency, 2019). The GHGRP
The study considered three types of abundant high-purity CO2 dataset reports locations and process-level GHG emissions from various
sources in the United States: ethanol plants, natural gas SMR facilities types of industrial sources. Annual emissions of high-purity CO2 from
for hydrogen production, and ammonia production facilities (Somers SMR facilities (indicated by subpart “P” in GHGRP) and ammonia
and Quinn, 2019). To evaluate and compare the potential energy, GHG, manufacturers (indicated by subpart “G” in GHGRP) were obtained as
and water stress implications, the study modeled an algae site using the CO2 emissions from the hydrogen production and ammonia
high-purity CO2 in each state. Annual and monthly life-cycle GHG manufacturing processes, respectively. Locations and capacity of
emissions and water-stress impact were evaluated and compared to ethanol plants were obtained from U.S. Energy Information Adminis
understand whether high-purity CO2 from ethanol facilities outweigh tration (2017). The locations and capacities of the high-purity CO2
lower algae productivity in the Midwest. Finally, the study assessed sources in the United States are summarized in Fig. 1.
potential advantages and drawbacks of each algae site to provide in
sights into the opportunities and challenges of utilizing high-purity CO2 2.3. Site selection
for algae production in the United States in terms of high-purity CO2
availability, the algae farm’s on-stream time, water-stress impacts, and BAT models algae growth and water use on areas screened in the
land availability. United States based on appropriate topography, land use, economically
available CO2 sources, and environmental suitability (ANL, NREL, and
2. Methods PNNL, 2017). Environmentally sensitive lands such as forests, existing
cropland, and national parks are excluded. The SI and previous studies
2.1. Biomass assessment tool document BAT and its land screening criteria in detail. Locations of the
algae ponds modeled by BAT after land screening are shown in Fig. 1.
The Biomass Assessment Tool (BAT) (Coleman et al., 2014), which Note that, to avoid conversion of croplands and other environmentally
was developed at Pacific Northwest National Laboratory (PNNL), is an sensitive lands (e.g., forests and wilderness areas), the land-screening
integrated model, analysis, and data management and development process identified no suitable minimum land area for algae cultivation
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
Fig. 1. Locations of the BAT land suitability for potential algae ponds, high-purity CO2 sources, and selected ponds for case studies. State abbreviations: Minnesota
(MN), Wisconsin (WI), Nebraska (NE), Iowa (IA), Indiana (IN), Texas (TX), Louisiana (LA), Florida (FL).
in Iowa and Illinois even though high-purity CO2 is abundant in these FL, and TX for low-latitude sites), and at least two sites in each latitude
states due to a large number of ethanol plants. range were examined.
Based on the algae ponds BAT modeled after land screening, this One algae site was modeled in each state. Davis et al. (2016) reported
study selected eight locations over two regions where high-purity CO2 is that a production area of 5000 acres (2023 ha) is reasonable for an algae
abundant: the Gulf Coast, which has many SMR and ammonia- facility because it is large enough for downstream biofuel production
production facilities; and the Midwest, where corn ethanol plants are operations to take advantage of economy of scale, but not so large that it
densely located. Louisiana (LA) and Texas (TX) have the highest abun would cause many logistical challenges. Supercritical CO2 can be
dance of high-purity CO2 in the United States. An algae site in each state transported in a pipeline over a long distance (>100 km) (Mohammadi
was examined to evaluate the environmental implications of algae et al., 2019). However, long transportation distances cause the delivered
cultivation and biofuel production. In addition, Florida (FL) was shown CO2 to cost more (Dongjie et al., 2012) because the capital, operating,
to be highly suitable for algae cultivation (ANL, NREL, and PNNL, 2017). and maintenance costs of the pipeline are roughly proportional to its
This study thus considered an algae site in FL as a reference case, even length (McCoy and Rubin, 2008). This study considered a CO2 trans
though FL does not have significant industrial sources of high-purity portation distance of up to 32 km (20 miles). With these two constraints
CO2. (sufficient land availability and proximity to a high-purity CO2 source),
Iowa (IA), Illinois (IL), Nebraska (NE), Minnesota (MN), Indiana (IN) one 5000-acre algae site was selected for each state considered in this
are the top five suppliers of high-purity CO2 in the Midwest (U.S. Energy study. Detailed site selection criteria and information on the selected
Information Administration, 2017). One site was per state in NE, MN, sites are included in the SI. Locations of the selected site are illustrated in
and IN, respectively. Although BAT found no suitable minimum land Fig. 1.
area for algae cultivation in IA under the existing land-screening pa
rameters set forth in Wigmosta et al. (2011) and refined in ANL, NREL, 2.4. System boundary
and PNNL (2017), this study still considered one site in IA because there
are many ethanol facilities in the state. The IA site was selected to ac Fig. 2 illustrates the boundary of the system investigated in this
count for the possibility that suitable land for algae growth may be found study. Two types of CO2 sources are considered: dilute CO2 from the flue
there under loosened land screening constraints (e.g., a fraction of gas of fossil-fuel power plants, and industrial high-purity CO2 emitted by
cropland could be diverted to algae growth if production of algae and its SMR, ammonia, and ethanol plants. An additional carbon capture pro
associated fuel and chemical products could create higher revenues than cess is required to obtain high-purity CO2 when flue gas is used as the
the crops they displace). An algae site in Wisconsin (WI) was considered carbon source. The high-purity CO2, obtained either directly from a
so that the eight sites spanned across various latitudes (MN and WI for high-purity source such as a corn ethanol plant or by carbon capture, is
high-latitude sites; IA, IN, and NE for moderate-latitude sites; and LA, then compressed to a supercritical state and piped to the algae facility.
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
Harvested algae is then sent to a co-located biorefinery where it is mix of the corresponding North American Reliability Corporation
converted to biofuel via HTL and upgrading. Natural gas is consumed to (NERC) region (Argonne National Laboratory, 2020b).
supply hydrogen via steam reforming to hydrotreat the HTL biocrude Intermediate booster compressor stations may be required for
(Jones et al., 2014). The biofuel product from upgrading is then recompression, because the pressure drops when CO2 is transported in a
distributed to gas stations and eventually combusted in vehicles. pipeline. We assumed that booster compressor stations will be needed
every 150 km (da Silva et al., 2018), and the energy requirement for
2.4.1. CO2 capture, compression, transportation, and onsite distribution recompression is 0.01 MJ/kg-CO2 (da Silva et al., 2018). All of the algae
High-purity CO2 is compressed and transported to the algae sites via sites presented here are within 150 km of the CO2 source, so no booster
pipeline in a supercritical state (typically 13 MPa and 40 ◦ C) (Davis compressor stations are needed.
et al., 2016). Previous studies reported energy requirements between Modeling of onsite distribution of the CO2 follows the design of a
0.35 and 0.40 MJ/kg-CO2 were required in order to compress CO2 to a previous study (Somers and Quinn, 2019), where the delivered CO2 is
supercritical state (0.36 MJ/kg-CO2 reported by Supekar et al., 2017; stored as a liquid. The liquid CO2 is slowly heated and evaporated to
0.35–0.40 MJ/kg-CO2 reported by von der Assen et al., 2016; and 0.40 distribute it through the algae ponds (Davis et al., 2016). The energy
MJ/kg-CO2 reported by Zhang et al., 2006). This study assumed an demand for onsite distribution of CO2 is estimated to be 0.14 MJ/kg-CO2
energy consumption of 0.36 MJ/kg-CO2 for CO2 compression (Supekar (Somers and Quinn, 2019). The utilization efficiency of the delivered
et al., 2017). CO2 is 60% (Jonker and Faaij, 2013).
Flue gas from fossil fuel power plants, on the other hand, must be
captured it can be compressed to a supercritical state. Post-combustion 2.4.2. Algae cultivation, harvest, dewatering, and storage
capture using monoethanolamine (MEA) is the most common and Cultivation of microalgae was modeled following previous studies
mature technology for carbon capture from flue gas of fossil-fuel power (ANL, NREL, and PNNL, 2017). Pond circulation consumes a large
plants (Leung et al., 2014). Other carbon capture technologies, including amount of energy and has significant impacts on the lifecycle analysis
membrane separation and direct air capture, have also attracted sig results. This study used the same assumption as the study by ANL, NREL,
nificant attention in recent years. However, they must overcome critical and PNNL (2017), where pond circulation operates 12 h per day and
technical challenges before they can be widely used. For instance, consumes 1.2 kW/ha. Detailed assumptions of material and energy in
membrane separation requires relatively complex operations and has puts of algae cultivation are listed in Table S1. For an algae pond with a
difficulty dealing with flue gas streams due to its low pressure (Al-Ma productivity of 25 g/m2/day, the total energy consumption of algae
moori et al., 2017). Direct air capture is a capital- and energy-intensive cultivation, including pond circulation, onsite water circulation, and
process due to the ultra-low CO2 concentration in the atmosphere make-up water delivery, is estimated to be 0.6 MJ/kg harvested algae on
(House et al., 2011). This study focuses on MEA-based carbon capture. an ash-free dry weight (AFDW) basis.
A wide range of energy requirements for MEA-based carbon capture The biomass was assumed to be harvested when the pond concen
have been reported. Boot-Handford et al. (2014) reported 0.72–1.62 trations reached a density of 500 mg/L (ANL, NREL, and PNNL, 2017).
MJ/kg-CO2 for carbon capture in coal-fired power plants using a variety The harvested algae were dewatered before being sent to biorefineries
of solvents and compression to pipeline pressure (>10 MPa). A review for conversion to biofuels. A three-step harvest and dewatering process
by von der Assen et al. (2016) reported a range between 0.76 and 1.84 consisting of in-ground gravity settlers, hollow fiber membranes, and
MJ/kg-CO2 for MEA-based carbon capture in coal-fired power plants. centrifugation was completed to obtain a concentrated biomass of 200
More recent studies have noted a decreasing trend in carbon capture g/L (Davis et al., 2016), which is suitable for downstream HTL conver
energy requirements (Rochedo and Szklo, 2013). This study thus sion (Guo et al., 2015). The overall separation efficiency of harvest and
considered three values for the energy requirement of MEA-based car drying was estimated to be 87%, where over 99% of algal losses are
bon capture in a coal-fired power plant: 1.5 MJ/kg-CO2, reflecting older recycled back to ponds, and only a small fraction of the growth media is
technologies (Rubin et al., 2015); 1.0 MJ/kg-CO2, for current technol removed to mitigate buildup of salts and other inorganics (ANL, NREL,
ogies (Strube and Manfrida, 2011); and 0.63 MJ/kg-CO2, representing and PNNL, 2017). The concentrated algae biomass is routed to
future technologies (ANL, NREL, and PNNL, 2017). The energy con short-term storage (surge capacity up to 24 h), where 1% AFDW is lost
sumption of carbon capture is assumed to be electricity from the grid (Davis et al., 2016).
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
Algae cultivation, harvest, and dewatering consume a considerable 2.5. Life-cycle assessment
amount of electric energy. In order to account for differences in the
regional electricity mix, this study calculated the carbon intensities of The mass and energy balance results were used to perform LCA for
local electricity using the electricity mix of the corresponding NERC the co-located algae sites and HTL biorefinery. LCA was performed with
region (Argonne National Laboratory, 2020b). Local electricity carbon GREET (Argonne National Laboratory, 2020b). GREET is a publicly
intensities of the selected algae sites are listed in Table S2 (Argonne available LCA tool for analyzing the energy and environmental impacts
National Laboratory, 2020b). of a wide range of technologies in transportation, power, and material
products. It models life-cycle energy and the environmental impacts
2.4.3. Biofuel production, fuel distribution, and fuel combustion effects of bioenergy systems over the entire supply chain based on
Harvested and dewatered algae were sent to a co-located biorefinery process-level energy and material balances, and bioenergy yields. Out
to produce hydrocarbon biofuels via HTL and upgrading (Jiang et al., puts of the life-cycle assessment include life-cycle GHG emissions, fossil
2019). Products of HTL included biocrude, solids, an aqueous phase, and energy use, and water use.
off-gas. HTL biocrude was hydroprocessed to produce diesel and
naphtha-range fuels. The process off-gas was used to generate hydrogen, 2.6. Water-stress impact assessment
heat, and power. External natural gas was purchased for supplemental
hydrogen production. Nutrients (nitrogen and phosphorus) recovered To quantify and compare the water-stress impact of algae production
from the HTL solids were recycled to the algae ponds to reduce the in different locations, this study used the Available Water Remaining for
amount of nutrients such as ammonia (NH3) and diammonium phos the United States (AWARE-US) (Lee et al., 2019), a water-stress impact
phate (DAP) needed for algae growth. HTL yields, hydrocarbon fuel assessment tool (https://greet.es.anl.gov/aware) developed at Argonne
production, and natural gas use were estimated using published data National Laboratory (2020a). AWARE-US quantifies the water-stress
(ANL, NREL, and PNNL, 2017). The overall fuel production was esti impact of new water consumption as a water scarcity footprint (WSF)
mated to be 23.3 MJ fuel product per kg AFDW algae (ANL, NREL, and (Xu et al., 2020), which is the product of monthly water consumption
PNNL, 2017). Natural gas demand for hydrogen production is 0.22 and monthly county-level water-stress characterization factors (CFs)
MJ/MJ fuel product (ANL, NREL, and PNNL, 2017). Other material and (Equation (1)).
energy inputs are listed in Table S1. Consistent with the AWARE global approach (Boulay et al., 2018),
Transportation and distribution of the fuel product are estimated water-stress CFs are calculated by comparing remaining water avail
using default parameters in the Greenhouse gases, Regulated Emissions, ability (i.e., the amount of surface water that is available to new users
and Energy use in Technologies (GREET®) model as shown in Table S1 after satisfying demands of existing users, including ecosystem services)
(Argonne National Laboratory, 2020b). In LCA, it is common practice to in each region to the reference (U.S. average). In AWARE-US, CF ranges
track biogenic carbon in fuel and to omit biogenic carbon dioxide from from 0.1 to 100, with CF = 1 meaning that the remaining water in a
the calculation of global warming potential (Downie et al., 2014). This is given county is equivalent to the U.S. average. Counties with less
because an equivalent amount of carbon dioxide was taken up from the remaining water availability than the U.S. average therefore have higher
atmosphere during biomass growth. In the case of this study, the situ CF values:
ation is a little more complicated as the CO2 used for algae growth is
WSFi = WCi × CFi (1)
sourced from ethanol fermentation CO2 or coal combustion flue gas.
Nonetheless, the CO2 taken up during algae growth would have been WSFi indicates the WSF expressed in liter equivalent per MJ fuel in
emitted to the atmosphere had it not been intercepted for this purpose. month i at the location of interest expressed in terms of U.S. equivalent
Thus, it was assumed that the CO2 released during use of algal biofuel liters. WCi and CFi denote the water consumption in liter per MJ fuel and
was also offset by the CO2 taken up during algal biomass growth. the unitless CF in month i, respectively, at the same location. For water
Therefore, the net GHG emissions from biofuel production and carbon use occurring at the location of the co-located algae and HTL facility (i.
uptake are minimal and result from the small amount of CH4 and N2O e., pond water demand determined by evaporative water loss and
emitted during vehicle operation. incoming precipitation), water use during biofuel production, and water
recycle from biofuel production, local CFs are used in Equation (1). For
2.4.4. Algae farm infrastructure water use associated with upstream processes whose exact location in
Because infrastructure was so important in previous technoeconomic formation is not available, including electricity generation, production
analyses of algae production systems, the life-cycle analysis (LCA) of of chemicals, and infrastructure manufacturing, the average CF in the
algae farm infrastructure is included here (Davis et al., 2016). The United States (i.e., CF = 1) is used. Fig. 3 summarizes the modeling tools,
infrastructure components considered in this study include pipelines for main references, and data flow of this study.
CO2 transport from the source, onsite CO2 delivery infrastructure, open
raceway pond construction, centrifuges for algae dewatering and har 3. Results and discussion
vesting, homogenizer construction, dissolved air floatation construction,
and pipelines to deliver makeup water. Infrastructure requirements are 3.1. High-purity CO2 sources
determined on the basis of the total area of algae cultivation and the
material requirements and usage per unit area. First, the total amount of The annual supply of high-purity CO2 by source type is illustrated in
concrete, high-density polyethylene liner, polypropylene, steel, polyvi Fig. 4. The supply of high-purity CO2 from these sources in 2018
nyl chloride, low-density polyethylene plastic cover, and cast iron were amounts to 107 million metric tons (MMT), with 12 MMT from
determined for algae farm infrastructure based on algae productivity ammonia facilities, 44 MMT from ethanol plants, and 44 MMT from SMR
across different locations. Table S3 provides the material requirements facilities. There exist 198 ethanol plants, 110 SMR plants, and 28
on a per-unit basis for the algae farm infrastructure. Corresponding GHG ammonia manufacturing facilities in the United States. However, 94% of
emissions and carbon intensity were determined based on the net ma the ethanol plants only emit <400 thousand tonne of high-purity CO2
terial use for algae farms. Assuming the design service life of infra per year. Therefore, the average annual emission per plant, which is
structure components is 30 years, the annual average value of the calculated by dividing the total emissions from all the facilities by the
infrastructure environmental impacts was determined for the different number of the facilities, is lowest for ethanol plants.
sites in accordance with the total fuel output for 30 years of operation. There are several large SMR facilities with annual CO2 emissions
higher than 1200 thousand tonne per year while no ethanol plant emits
more than 1200 thousand tonne of high-purity CO2 per year. In
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
Fig. 5. (a) Average life-cycle GHG emissions. (b) Average life-cycle fossil energy use. (c) Average life-cycle water use. (d) Average water-stress impacts. For the flue
gas case, the height of the bar indicates the results for carbon capture energy requirement of 1.0 MJ/kg-CO2, and the error bars indicate the results for carbon capture
energy requirements of 1.5 and 0.63 MJ/kg CO2, respectively.
fossil energy use, and water use for algae cultivation and biofuel pro A recent survey of commercial-scale ethanol plants noted that
duction. The GHG emissions for the states around the Gulf Coast region several corn ethanol plants are generating electricity onsite, and the
are between 35 and 37 g CO2 eq/MJ, while the emissions for the Mid energy sources of onsite electricity generation tend to be renewable
west states range between 38 and 40 g CO2/MJ. rather than fossil-based (Wu, 2019). If the CO2 used for algae cultivation
The life-cycle GHG emissions of algae and biofuel production at the were extracted from an ethanol plant using excess on-site electricity
eight sites selected for this study did not show significant variations generated from renewable sources, the carbon footprint of the
because the annual average algae productivity is comparable across all algae-based biofuels would be further reduced.
the sites, as discussed in Section 3.2. Algae productivity is the main Average infrastructure-based GHG emissions from the Midwest sites
driver for the GHG emissions during algae cultivation because the total are about double those of the Gulf Coast sites, primarily because the use
electricity consumption for pond circulation is constant, and the elec factor is significantly lower in the Midwest where the biorefinery
tricity consumption per kg of AFDW algae increases when algae pro operates between April and September and remains closed during the
ductivity is low. In addition, this study did not consider the impact of other months due to low microalgae productivity. Among the different
algae strains on the downstream fuel production process due to a lack of infrastructure components, the greatest impacts can be attributed to the
data. In other words, fuel yield, energy consumption, and chemicals construction of large open raceways for algae cultivation, followed by
usage during HTL and upgrading were assumed to be the same for all the settling tank and inoculum pond construction. Construction of large
sites. open raceway ponds contributes around 73% of the total infrastructure
The difference in GHG emissions can be attributed to two factors: impacts. Overall, infrastructure accounts for 3–6% of the total life-cycle
regional electricity mix and infrastructure. CO2 sourcing and algae GHG emissions. A detailed breakdown of the impacts of infrastructure
cultivation together contribute to about 50% of the total GHG emissions. on GHG emissions is provided in the SI.
Electricity accounts for 100% of the GHG emissions from CO2 sourcing Also shown in Fig. 5(a) are the life-cycle GHG emissions from an
and delivery and 98% of the GHG emissions from algae cultivation; algae site located in FL but using dilute CO2 sources from the flue gas of a
therefore, variations in local electricity carbon intensities make a dif coal-fired power plant. The dilute CO2 stream is captured using MEA.
ference in the total GHG emissions. Note that carbon uptake during GHG emissions from such an algae site are 22% and 39% higher than a
algae growth is offset by the CO2 emissions from biofuel combustion and similar algae site using high-purity CO2 as the carbon source with old
thus is not included in the emissions from algae cultivation in Fig. 5(a). (1.5 MJ/kg-CO2) and current (1.0 MJ/kg-CO2) carbon capture tech
FL has the lowest electricity carbon intensity (534 g CO2 eq/kWh) nologies, respectively.
among the eight states because 71% of the electricity there is produced Even with more efficient future carbon capture technology (0.63 MJ/
from natural gas (Argonne National Laboratory, 2020b). The clean kg-CO2), the GHG emissions from an algae site using dilute CO2 are still
electricity also contributed to the low life-cycle GHG emissions from the 9% higher than those from a site sourcing CO2 from high-purity sources.
FL site. The main difference derives from the fact that sourcing CO2 from a high-
The carbon intensities of electricity generated in LA (559 g CO2 eq/ purity source avoids the energy-intensive carbon capture process. The
kWh), TX (570 g CO2 eq/kWh) and IN (610 g CO2 eq/kWh) are mod carbon capture process causes an additional GHG emission of 3–14 g
erate. The other states have the highest electricity carbon intensity (638 CO2 eq/MJ, depending on the energy consumption of the carbon capture
g CO2 eq/kWh) among the eight states due to the high share of coal- technology used.
derived electricity (54%) in their regional electricity mix. The large When comparing a Midwest site using high-purity CO2 from corn
impacts of local electricity carbon intensity on the life-cycle GHG ethanol plants for algae cultivation to a FL site using dilute CO2, the
emissions suggest that using low-carbon electricity for CO2 sourcing and Midwest site achieves 9–24% lower GHG emissions than the FL site
algae cultivation can help achieve lower life-cycle GHG emissions. capturing CO2 with old or current carbon capture process. Even if the
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carbon capture process becomes more efficient in the future, the Mid 3.3.2. Monthly results
west algae sites still achieve comparable GHG emissions to a FL algae Algae productivity is subject to seasonal variation in climatic con
site using dilute CO2 for algae cultivation. ditions such as temperature and light intensity. As a result, life-cycle
Fossil energy usage shows a different trend from that of GHG emis GHG emissions also presents seasonal variations, as shown in Fig. 6
sions (Fig. 5(b)). The Midwest sites consume less fossil energy than the (a). The monthly variation in life-cycle GHG emissions is mainly driven
Gulf Coast sites. Fossil energy usage is comparable across all the sites by the monthly fluctuation in the algae growth rate. The GHG emissions
because they have similar annual average algae productivity. The dif of all the sites fall into a range of 34–42 g CO2 eq/MJ, with the lowest
ference is again driven by the regional electricity mix. Coal-derived emissions observed in the summer months (June to August). The Mid
electricity causes higher carbon intensities but lower fossil energy west sites generate slightly higher (~2 g CO2 eq/MJ) GHG emissions
usage than natural gas–derived electricity. The main reason is that than the Gulf Coast sites. This is mainly because of the carbon intensity
natural gas extraction consumes more fossil energy than coal mining of the regional electricity mix is higher, and the equipment utilization
(Argonne National Laboratory, 2020b). The high share of coal-derived factor is lower, in the Midwest. Life-cycle fossil energy use shows a
electricity in the Midwest thus helps algae sites to achieve lower similar trend to GHG emissions (Fig. 6(b)). The lowest fossil energy use
life-cycle fossil energy usage. The algae sites that source carbon from is observed in summer because the algae growth rate is highest then. The
high-purity CO2 achieve a 9–37% reduction in fossil energy use variation among different months is small.
compared to the FL site using a dilute CO2 source due to avoidance of Distinct monthly fluctuations in water usage are observed among
carbon capture. Fossil energy consumption for infrastructure is minor in different algae sites, as shown in Fig. 6(c). The FL and LA sites use the
comparison to the energy use for the other processes. For the different most water in spring (March to May), while all the other sites see peak
sites, infrastructure fossil energy usage contributes to only 4–8% of the water consumption in summer (June to August). The peak monthly
total fossil energy use. water requirement of the FL (6.0 L/MJ), TX (6.4 L/MJ) and NE (5.6 L/
A marked spatial variation is observed in life-cycle water usage, as MJ) sites are high, while the LA (2.2 L/MJ) and IA (3.5 L/MJ) sites use
shown in Fig. 5(c). This is because water use is mainly driven by the moderate water in the months with the highest water demand. The IN
evaporative loss from the open ponds during algae cultivation, which is (1.5 L/MJ) and WI (1.3 L/MJ) sites have the lowest peak monthly water
determined by evaporation rates and incoming precipitation and de demand.
pends on local climatic conditions. Infrastructure only contributes to a Monthly life-cycle water-stress impact results are illustrated in Fig. 6
small portion (less than 0.5%) of total well-to-wheel water usage. (d), taking into account local water availability. For most sites, water-
Among the sites in the Gulf Coast region, the LA site has the lowest stress impacts show a consistent trend with net water usage. LA has
annual average water usage of 1.1 L/MJ. The FL site has medium annual the lowest water-stress impact among the Gulf Coast sites, owing to its
average water usage of 2.1 L/MJ, and the TX site has high annual low water usage and minimal local water stress (monthly CFs between
average water usage of 4.5 L/MJ, with evaporative loss accounting for 0.15 and 0.74). The highest seasonal WSF in LA occurs in October (1.2 L
4.1 L/MJ. On the other hand, the algae sites in WI and IN use the least eq/MJ). The WSF of the FL site shows considerable seasonal variation,
amount of water in the Midwest, with annual average net water usage of with the lowest WSF in September (0.1 L eq/MJ), and the highest in May
less than 1 L/MJ. The water consumptions of the algae sites in MN and (11.2 L eq/MJ). This is consistent with the net water usage at this site.
IA are medium, at 1.5 and 2.3 L/MJ, respectively. The NE site uses the The TX site has substantially higher water-stress impacts than the FL
largest amount of water among the Midwestern sites (4.2 L/MJ), the site, mainly due to high local water stress (CFs between 1.04 and 6.25).
same level as the TX site. The impacts of CO2 purity on life-cycle water High CF means that the water consumption for operating a new algae
use are minimal. site can incur high water-stress impacts in the area. All the Midwest sites
The annual average water-stress impacts are shown in Fig. 5(d). have higher WSFs between July and September than in other months.
Evaporative loss is the dominant contributor to the water impacts, The IN and WI sites have low WSFs, and the IA and MN sites have me
especially for the locations facing high local water stress, such as NE and dium WSFs. However, the WSF of the NE site is prohibitively high in all
TX. The NE site has high water consumption partly due to its high net months because its local CFs are extremely high (28.86–100).
evaporative loss (Fig. 5(c)). More importantly, it also has extremely high
CFs (28.86–100, see Table S2) because it has low remaining water 4. Implications
availability after satisfying demands of existing users (i.e., high local
water stress). In consequence, the NE site has high water scarcity foot High-purity CO2 sources offer reduced GHG emissions, as well as
print according to Equation (1). The TX site also has high water-stress reduced fossil energy use, for algae farms and algae-based biorefineries
impacts (15.4 L eq/MJ). The MN and FL sites have moderate water- because it eliminates the need for the energy-intensive carbon capture
stress impacts (~2 L eq/MJ). The water-stress impacts of the LA, IN, process. A Midwest algae site using high-purity CO2 emitted from a corn
and WI sites are the lowest among all the sites (<1 L eq/MJ). ethanol plants can achieve lower GHG emissions and fossil energy use
Since manufacturing ammonia and diammonium phosphate con than a site on the Gulf Coast that uses dilute CO2 from the flue gas of a
sumes energy and water, recycled nutrient from HTL help to lower the fossil-fuel power plant. This shows that the potential exists to produce
life-cycle GHG emissions, water consumption and waster stress impact algae in the Midwest, because the availability of high-purity CO2 for
by reducing the demand for these external nutrients. However, the algae growth on the Gulf Coast is uncertain due to the competition from
amount of the recycled nutrients is small (equivalent to ~0.7 g NH3/MJ the CO2-EOR industry. Moreover, most Midwest sites have lower water
biofuel and ~0.3 g DAP/MJ biofuel), their impacts on the life-cycle GHG stress than the Florida site.
emissions and water consumption are quite small. For instance, the However, the low algae productivity in the cold seasons must be
recycled nutrients reduce the life-cycle water consumption by ~0.008 addressed. Otherwise, the algae site is likely to shut down, and the HTL
L/MJ, which is less than 1% of the life-cycle water consumption. It can biorefinery needs to use other feedstocks such as woody biomass, sludge,
also be seen from Fig. 5(c) and (d) that evaporative loss is the main and animal manure in the winter months (Cai et al., 2020). Algae pro
contributor to the life-cycle water consumption and life-cycle water ductivity in cold seasons could be improved by methods such as using a
stress impact. Nonetheless, the impacts of recycled nutrients on the GHG greenhouse covering in combination with waste heat recovery from a
emissions, water consumption, and water stress impacts are accounted co-located ethanol plant (Rosenberg et al., 2011), or using closed
for in “fuel production” in Fig. 5(b) and “conversion water usage” in tubular photobioreactor systems. However, the estimated costs of these
Fig. 5(c) and (d), respectively. systems were prohibitively high for biofuel production (Davis et al.,
2011).
Productivity, water stress, and availability of a suitable CO2 source
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
Fig. 6. Monthly results for the algae sites: (a) life-cycle GHG emissions; (b) life-cycle fossil energy usage; (c) life-cycle water usage; and (d) life-cycle WSF.
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
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L. Ou et al. Journal of Cleaner Production 321 (2021) 128779
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