Applied Energy 279 (2020) 115884

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

BECCS based on bioethanol from wood residues: Potential towards a

carbon-negative transport and side-effects
Sara Bello a, b, *, Ángel Galán-Martín a, Gumersindo Feijoo b, Maria Teresa Moreira b,
Gonzalo Guillén-Gosálbez a
a
Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093 Zürich, Switzerland
b
Department of Chemical Engineering, CRETUS Institute, Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• BECCS systems have the potential to

deliver carbon-negative wood-based
biofuels.
• A carbon footprint of − 2.7 kg CO2 eq./
100 km was the best result obtained in
an E85.
• Net removal depends on the carbon in­
tensity of electricity and heating
consumed.
• Risk of burden-shifting is a reality and
should be considered for biofuel
policies.

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

Keywords: Bioenergy with carbon capture and storage (BECCS) is gaining broad interest as an effective strategy to go
Negative emission technologies beyond carbon neutrality. So far, most of the work on BECCS focused on power systems, while its application to
Bioenergy with carbon capture and storage the transport sector has received much less attention. To contribute to filling this gap, this work investigates the
(BECCS)
potential of BECCS as a carbon-negative strategy in the transport sector by applying process modelling and life
Lignocellulosic bioethanol
Life cycle assessment
cycle assessment (LCA) to bioethanol production from lignocellulosic waste. The process was analyzed following
Cradle-to-wheel a cradle-to-wheel approach, i.e., from biomass growth to the combustion of biofuel in the cars, assuming that the
Carbon-negative biofuel CO2 emitted in the fermentation and cogeneration units is captured, compressed and transported to be stored
permanently in geological sites. Several scenarios differing in the bioethanol-gasoline blends (10–85% bio­
ethanol) were considered for a functional unit of 1 km of distance travelled, comparing with fossil-based gas­
oline. Our results show that blends above 85% (ethanol/gasoline) could have the potential to deliver a net-
negative emissions balance of − 2.74 kg CO2 eq per 100 km travelled and up to − 5.05 kg CO2 eq per 100 km
using a low carbon electricity source. The final amount of net CO2 removal is highly dependent on the carbon
intensity of the electricity and the heating utilities. Biofuels blends could, however, lead to burden-shifting in
eutrophication, ozone depletion and formation, toxicity, land use, and water consumption. This work highlights
the potential of BECCS in the transport sector, and the need to analyze impacts beyond climate change in future
studies to avoid shifting burdens to other categories.

* Corresponding author at: Department of Chemical Engineering, CRETUS Institute, Universidade de Santiago de Compostela, 15782 Santiago de Compostela,
Spain.
E-mail address: sara.bello.ould-amer@usc.es (S. Bello).

https://doi.org/10.1016/j.apenergy.2020.115884
Received 29 May 2020; Received in revised form 7 September 2020; Accepted 12 September 2020
Available online 29 September 2020
0306-2619/© 2020 Elsevier Ltd. All rights reserved.
S. Bello et al. Applied Energy 279 (2020) 115884

1. Introduction emissions at a safe level even under conditions hard to predict [20]. In
this context, Möllersten et al. addressed the potential CO2 reductions
The European Union member states have set targets to achieve a 40% and associated costs in the chemical pulp and paper mill industry [21]
reduction in greenhouse gas (GHG) emissions by 2030 (and proposed an and in sucrose fermentation to produce ethanol [22]. In 2003, the term
even more ambitious goal of at least 55%) aiming at reaching climate BECCS was first introduced as a technological solution to convert the
neutrality by 2050. In this context, the European Green Deal is based on energy system into a CO2 remover [23]. However, the kick-off for BECCS
a series of strategic goals mainly sustained on three pillars, i.e., was the special report on CCS published in 2005 by the Intergovern­
encouraging energy efficiency, promoting cleaner energy through the mental Panel on Climate Change (IPCC), which highlighted BECCS as a
deployment of renewable sources and incorporating clean mobility feasible large-scale option to provide net negative emissions [24]. Since
systems (e.g., use of second or third-generation biofuels) [1]. then, due to the continued use of fossil fuels and the steady increase in
Very likely, these actions will have to be accompanied by carbon the associated carbon emissions, BECCS has attracted increasing atten­
dioxide removal (CDR) strategies, which seem vital to meet the goals tion as a key option to meet the climate targets sought [5,25].
stated in the Paris Agreement [2]. The draft of the upcoming EU Climate Despite their expected pivotal role in climate change mitigation, the
Law explicitly mentions the necessity of CDR to achieve the EU 2050 deployment of BECCS technologies would, however, face some obsta­
climate-neutrality goal [3], which could be delivered through carbon cles. These challenges include constraints given by land availability and
capture and storage (CCS). The portfolio of CDR options available in­ CO2 storage capacity, socio-economic barriers, policy adequacy issues,
cludes afforestation and reforestation (AR), ocean alkalinity enhance­ logistical implementation difficulties, as well as other sustainability
ment, biochar sequestration, mineralization of carbon dioxide, direct air concerns [26,27], all of them linked to the specific BECCS technology
capture and storage (DACCS) and bioenergy with carbon capture and selected. There are a handful of BECCS technologies implementing
storage (BECCS). Notably, CCS could be applied to a wide range of fossil- several conversion routes and spanning different sectors. These include
based industries. High emission sources include the cement industry, the (among others) biomass feedstocks burned at power or heating plants
iron and steel industry, and fossil refineries [4]. CCS in the fossil-based with CCS [28], gas or liquid biofuels production at biorefineries with
industry is deemed necessary to reach the decarbonization goals, yet it CCS [29–31], and pulp and paper mills equipped with CCS [32].
cannot lead to a net negative carbon balance. On the other hand, BECCS Several studies have delved into the BECCS technologies analyzing
and DACCS, regarded as promising CDR options, have the potential of its cost-effectiveness, potentials and side-effects [8,25,33–35]. Other
achieving net negative emissions. authors studied the negative emission potential of biomass co-fired with
According to estimates, the CO2 removal capacity for CDR options in coal in a power plant coupled with CCS from a life cycle assessment
2050 will range from 0.5 to 3.6 GtCO2⋅yr− 1 for afforestation and refor­ perspective [36]. On the other hand, others focused on the BECCS supply
estation, 2.0 to 4.0 GtCO2⋅yr− 1 for enhanced weathering, 0.5 to 2.0 chain optimization to deliver carbon-negative electricity [37–39].
GtCO2⋅yr− 1 for biochar, and reach 5.0 GtCO2⋅yr− 1 for soil carbon Despite extensive research and the growing interest in BECCS at the
sequestration. DACCS is assumed to be only limited by the geological industrial level [40], most of the efforts on BECCS have focused on
storage capacity and the availability of energy resources. At the same biomass conversion to heat and power. In contrast, the BECCS concept
time, the potential of BECCS varies significantly, between 0.5 and 5.0 applied to biorefineries that produce biofuels [14,39] remains mostly
GtCO2⋅yr− 1, depending on the technical assumptions and land avail­ unexplored [7].
ability (i.e., degraded and marginal land and/or abandoned and unused Carbon-negative biofuels could, however, become an appealing
agricultural land) [5–10]. alternative to replace conventional fossil-based fuels in the transport
Among all these CDR options, BECCS is receiving significant atten­ sector. By 2050, a 60% reduction in GHG emissions from transport is
tion and already emerges as predominant in most of the climate change expected compared to 1990 in order to comply with the recommenda­
mitigation scenarios aligned with the 1.5 ◦ C target. BECCS allows tions [41]. Accordingly, the use of alternative fuels in transport will need
removing CO2 while providing the clean and reliable energy needed to to grow by about 20% to meet the 2 ◦ C scenario of decarbonization [42].
underpin economic growth and development, which makes it particu­ In this context, the use of carbon-negative biofuels could provide sig­
larly appealing [5,11]. Indeed, BECCS is already considered in some nificant environmental benefits by reducing the dependence on fossil
Integrated Assessment Models (IAMs), in which other CDR engineered fuels and curbing the associated GHG emissions. Furthermore, they
options are rarely contemplated mainly due to lack of maturity could also help to accomplish the more ambitious goal of achieving a
[8,12,13]. Hence, alongside with AR, the broad deployment of BECCS carbon–neutral or even carbon-negative road transportation sector.
technologies will very likely play a pivotal role in meeting the climate Previous works on carbon-negative biofuels focused only on quan­
goals as they represent a good compromise between the carbon removal tifying the savings in global warming potential (GW) while disregarding
potential and the associated removal costs [8,14]. the potential collateral damage on other environmental categories such
Primarily, the BECCS concept refers to technologies converting as land use, acidification or toxicity. Some authors estimated the cradle-
biomass resources into valuable products in tandem with CO2 capture to-wheel GHG emissions of bioethanol [43–46], while only a few
systems. The latter prevents the release of the CO2 absorbed via considered CO2 capture coupled with the biofuel production pathway
photosynthesis during biomass growth to the atmosphere. Then, the [29,47–50]. To the best of our knowledge, no single study carried out a
captured CO2 is transported and injected into underground geological full life cycle assessment (LCA) of a bioethanol production system with
sites ensuring its long-term storage [15]. Compared with other CDR CCS adopting a “cradle-to-wheel” scope and embracing impacts on
options, BECCS has the value-added of potentially providing a net human health, ecosystems and resources. This research gap is particu­
negative balance of CO2 with the atmosphere while delivering renew­ larly critical, given the trade-offs between climate change and other
able energy-based products. The latter can, in turn, displace the use of environmental impacts inherent to some carbon mitigation strategies
their fossil-based counterparts, thereby avoiding their associated im­ [51–55]. These trade-offs are exemplified in the case of first-generation
pacts [8,16]. biofuels, where carbon emissions are reduced at the expense of exac­
The BECCS concept emerged in the last decade of the 20th century erbating impacts on land use and water consumption while posing the
through conceptual studies addressing the production of biomass-based issue of competition for land with food crops [12,56]. Overlooking these
biofuels combined with CCS (as applied to the hydrogen fuel [17]) and trade-offs could lead to unwanted collateral damages, thereby poten­
other bio-energy applications that could potentially deliver negative tially hampering sustainable development.
emissions [18,19]. The beginning of the 21st century brought formally To contribute to filling this research gap, in this study, we investigate
the concept of BECCS (initially called biomass-energy with carbon the production of bioethanol from residual woodchips covering a range
removal and disposal) as a risk management strategy to maintain GHG of environmental categories beyond climate change. Our analysis

2
S. Bello et al. Applied Energy 279 (2020) 115884

considers direct and indirect emissions throughout the whole supply were considered and compared with the fossil-based counterpart, i.e.,
chain, including biomass residues procurement, transportation, con­ conventional gasoline. In short, our results show that achieving a net
version, and the end-use of the biofuel in vehicles. Hence, acknowl­ negative emissions balance requires a bioethanol-gasoline blend above
edging the potential role of BECCS as an effective strategy to go beyond 85% and that the sources of electricity and heat consumed by the pri­
carbon neutrality, we apply LCA to the production of wood-based bio­ mary production process play a vital role in the final carbon balance
ethanol coupled with CCS as a potential negative emission biofuel for achieved. However, biofuels from lignocellulosic residues could worsen
transport decarbonization. LCA is a well-established holistic methodol­ other environmental impacts, including eutrophication, ozone depletion
ogy that allows conducting a negative emissions assessment by consid­ and formation, toxicity, land use and water consumption. Our results
ering all the carbon emissions in the entire life cycle of the fuel while could help in the development of future policies aimed at promoting
simultaneously evaluating other environmental categories. Hence, LCA negative emissions technologies and practices, where holistic assess­
allows us to determine whether technologies can deliver a net negative ments are critical to ensure sustainable development.
carbon balance and whether this may happen at the expense of wors­
ening other categories. This holistic analysis is particularly relevant for 2. Methods
BECCS technologies, as they have not yet been extensively deployed at
large scale. Moreover, LCA also allows us to pinpoint environmental A holistic evaluation of the value chain for bioethanol production
hotspots within complex value chains, thereby assisting in the prioriti­ was performed through the implementation of the LCA approach, as
zation of efforts to improve the environmental performance [57]. described in the ISO 14040 and 14044 standards [58,59]. The goal and
Eight scenarios differing in the bioethanol-gasoline blending ratios scope definition, life cycle inventory (LCI), life cycle impact assessment

Fig. 1. Cradle-to-wheel system boundaries for the use of bioethanol produced in a biorefinery with CCS (functional unit: 1 km travelled with bioethanol and/or a
bioethanol blend with a gasoline-fueled vehicle).

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S. Bello et al. Applied Energy 279 (2020) 115884

(LCIA), and the interpretation of the results stages were all completed, as requirements of the system. Notably, the CO2 flue gas and the off-gas
discussed in detail in the ensuing sections. from cellulase production are directed through a blower towards an
absorption–desorption system with an aqueous monoethanolamine
2.1. Goal and scope definition (MEA) solution [63]. MEA absorption was selected as CO2 capture
method due to its suitability for post-combustion capture. MEA is highly
The goal of the study is to analyze the carbon footprint (CF), together reactive in contact with CO2 and is particularly recommended to treat
with other environmental impacts, of the complete lignocellulosic bio­ gas streams with low concentrations of CO2 (such as the one leaving the
ethanol production and utilization value chain. To this end, our study cogeneration system) [64,65]. In the stripping section, the MEA is des­
follows a cradle-to-wheel scope that considers all the impacts from the orbed from the CO2, resulting in a purified CO2 stream that exits the top
growth and exploitation of lignocellulosic biomass to the end-use of the of the column at a purity of 13.9% wt., containing 86.1% wt. of residual
biofuel in a passenger vehicle. This scope, therefore, covers direct and water; this gaseous stream will later undergo a compression stage. The
indirect CO2 emissions over the whole life cycle while avoiding double bottoms stream of the distillation column is recirculated to reuse the
counting . The functional unit that best describes the main operational lean solvent back in the capture process. Before compression, the target
objectives of the system is 1 km travelled by the bio-fueled vehicle. CO2 stream is directed through a flash unit, in which a fraction of the
water is removed. The overall compression ratio of 110 requires four
2.2. System boundaries stages, with a constant inter-stage compression ratio of 3.2. Inter-stage
cooling between compressors is applied to keep the temperature
This section describes the system under study (Fig. 1) based on a within the desired range [66]. The flash cooling allows delivering a
cradle-to-wheel scope. Five main subsystems (SS) have been defined: purified CO2 stream free of water, reaching the required quality speci­
SS1 Feedstock; SS2 Biorefinery; SS3 CO2 Capture and compression; SS4 fications. The conditions of the stream leaving the compression stage
CO2 transport and injection; and SS5 Biofuel utilization. should be fixed based on the pressure, temperature and purity condi­
tions required for the transport and injection of CO2.
2.2.1. SS1. Feedstock
The biomass feedstock consists of hardwood residues, specifically 2.2.4. SS4. CO2 transport and injection
beechwood chips from a sawmill. This subsystem includes the silvicul­ CO2 exits the previous system at a pressure of 110 bar and 50 ◦ C, that
ture activities, comprising the uptake of CO2 associated with forest is, at a supercritical state that facilitates its transport, geological injec­
growth, soil preparation, and wood extraction activities. The extracted tion and long-term storage (e.g., in saline aquifers). Purity specifications
round wood is then further processed in sawmill facilities to obtain the are relevant to avoid pipeline corrosion, i.e., water limit of 400 ppm, and
three main products: bark, sawn timber, and wood residues. The latter, a concentration below 4% vol. of N2 and H2, the main compounds pre­
corresponding to the waste fraction, is the target feedstock in this pro­ sent in the treated streams. A concentration of CO2 above 95.5% wt. is
cess and enters the biorefinery in the form of woodchips [60,61]. also recommended (in our case, 99.8% wt. in SS3) [67]. SS4 includes the
pipeline for CO2 transport, considering a distance of 200 km. Based on
2.2.2. SS2. Biorefinery the physical conditions of the stream and the transport distance, we
The biorefinery includes all the process units required for the assume that no further recompression is needed. The LCA covers the
transformation of the woodchips, which are transported from a sawmill. drilling of the well and the CO2 losses during pipeline transport,
We assume a transportation distance of 100 km by lorry. Woodchips are considering 0.026% of losses per 1,000 km [68].
first digested in an Organosolv reactor, using ethanol and sulfuric acid as
the catalyst at 180 ◦ C. Pulp and liquor fractions are recovered in this first 2.2.5. SS5. Biofuel utilization
unit. The pulp stream is rich in hydrolyzable celluloses and hemi­ The bioethanol produced in the biorefinery is used in internal com­
celluloses. These compounds are transformed into fermentable sugars in bustion engine vehicles fueled with bioethanol-gasoline blends. Direct
an enzymatic hydrolysis unit using cellulases. Lignin is precipitated from emissions in a vehicle travelling a distance of 1 km (functional unit)
the liquor stream, which enters a distillation unit for the recovery of were considered. Eight scenarios were studied differing in the biofuel-
ethanol. A furfural stream is recovered via distillation as well. The sugars gasoline blend percentages. Scenarios were also defined according to
fraction is processed in an evaporator that removes water and acids. A the heating source employed in the capture and compression system
liquid–liquid extraction unit separates then the acetic acid from a re­ (SS3), i.e., either natural gas or sugar cane bagasse (Table 1) to provide a
sidual water flow. All lignocellulosic sugars are fed to the fermentation set of results ranging from fossil- to bio-based resources. The latter
unit, where steep corn liquor and other micro-nutrients are added to resource is only available in specific geographic regions, yet including it
produce bioethanol. Products other than ethanol are retrieved from the in the analysis sheds further light on the extent to which biofuels can
wood fractioning steps (furfural, lignin, acetic acid), yet our study fo­ deliver negative emissions. Moreover, bio-based heating from sugar
cuses on bioethanol as the primary fermentation product. Process resi­ cane bagasse was selected following a conservative assumption, as it
dues and natural gas are both combusted in the cogeneration unit in shows a poor GW performance among all the heating alternatives from
order to cover the energy requirements of the system [62]. biomass available in the Ecoinvent v3.5 [69] database (Figure S2). The
fossil-based alternative is based on conventional gasoline since gasoline-
2.2.3. SS3. CO2 capture and compression fueled vehicles represent the largest share of today’s fleet. Our analysis
The CO2 flue emissions from the biorefinery are captured, purified excludes the vehicle infrastructure (i.e., manufacture, assembly, and
and compressed in this subsystem. Three main emission streams are the end-of-life) since all the scenarios consider the same internal combustion
target of this subsystem (see Figure S1 and Table S1 in Supplementary engine vehicles.
Material). In the biorefinery (SS2), heating needs are supplied by com­
busting both process residues and fossil fuels. Therefore, the stream 2.3. Assumptions and limitations
leaving the cogeneration unit contains a mix of biogenic and fossil CO2,
both of which are captured. On the other hand, the CO2 emissions from The following assumptions apply to the LCA study. The transport of
the ethanol fermentation unit and the production of cellulases are bioethanol to fueling stations was omitted. In contrast, we considered
entirely biogenic. The CO2 streams from the cogeneration unit and the the transportation of woodchips from the sawmill to the biorefinery,
enzyme production process are fed to the capture system. In contrast, the assuming a distance of 100 km with 5% losses in a lorry freight. Elec­
biorefinery off-gas is fed just before the compression stage (due to its tricity and chemical processes are based on a European average, when
higher degree of purity), which reduces the energy and chemicals available, or a global average otherwise. The role of the carbon intensity

4
S. Bello et al. Applied Energy 279 (2020) 115884

Table 1
Scenarios considered based on the biofuel-gasoline blend percentages.
Scenario acronym Heating source in the ethanol plant Fuel blend Vehicle

Bioethanol(%) Gasoline(%)

Gasoline – 0 100 Gasoline compression ignition, internal combustion engine vehicle (GCI ICEV)
E10 SC Sugar cane 10 90 Spark ignition, internal combustion engine vehicle (SI ICEV)
E10 NG Natural gas
E25 SC Sugar cane 25 75 Spark ignition, internal combustion engine vehicle, high octane fuel (SI ICEV HOF)
E25 NG Natural gas
E40 SC Sugar cane 40 60 Spark ignition, internal combustion engine vehicle, high octane fuel (SI ICEV HOF)
E40 NG Natural gas
E85 SC Sugar cane 85 15 Spark ignition, internal combustion engine vehicle (SI ICEV dedicated)
E85 NG Natural gas

(CI) of the electricity mix was analyzed by considering a wide range of eutrophication in kg P eq, marine eutrophication in kg N eq, freshwater
mixes differing in their CFs (below and above the European average). ecotoxicity in kg 1,4-DCB eq, marine ecotoxicity in kg 1,4-DCB eq,
Regarding the heat requirements of the CO2 capture and compression human toxicity in kg 1,4-DCB eq, land use in m2a crop eq, fossil re­
system, we assumed that the cooling needs are covered using cooling sources scarcity in kg oil eq and water consumption in m3.
water pumped in a closed circuit. Infrastructure was omitted (installa­
tion, construction, and decommissioning), as it can be considered 2.5.1. Carbon accounting within LCA: Carbon footprint
negligible over a typical lifetime of industrial installations of over 30 Standard LCAs of systems involving biogenic inputs with a CO2 up­
years [70]. take from the atmosphere, such as those involving forests, assume that
In SS1 -biomass feedstock acquisition- economic allocation was this CO2 uptake is released at the end of the product’s life cycle.
applied to split the total impact among the products and co-products. Accordingly, the biogenic CO2 cycle is assumed to be mass balanced over
Notably, impacts from forest activities and sawmill were economically the life cycle [75]. In contrast, fossil CO2 emissions (both direct and
allocated among co-products, while the impacts from chipping were indirect) contribute to GW because they entail a net release of fossil
allocated entirely to woodchips [71]. All the impacts from the bio­ carbon to the biosphere (atmosphere), which contributes to climate
refinery subsystem were allocated to the bioethanol, which represents change. Accordingly, most standard LCA methods, such as ReCiPe or
the most conservative approach. CML, assign a zero characterization factor for GW to the biogenic CO2
In this analysis, the impacts from the production, assembly, and end- emissions [73,76].
of-life stages of the vehicle itself were omitted. Note that all the sce­ In contrast, when assessing the CF in systems that capture CO2 and
narios consider the same conventional gasoline-fueled spark-ignition store it permanently (CCS), it is critical to consider both the fossil and
vehicle (ICEV), so they remain comparable. Direct combustion emissions biogenic carbon flows adequately. A system either capturing fossil CO2
from the use of bioethanol and gasoline were considered from the or consuming biomass resources without CCS can lead, in the best case,
GREET 1.3 vehicle cycle model [72], together with the indirect impacts to a zero-balance, i.e., carbon–neutral system (Fig. 2). On the other
from the production of each fuel. hand, routes consuming biogenic carbon coupled with CCS systems
could potentially achieve a net negative balance, provided the CO2 is
2.4. Life cycle inventory stored underground in the long-term [77,78]. More precisely, a system
can provide a net negative emissions balance if the biogenic CO2 uptake
The LCA analysis relies on a compendium of different data sources, exceeds the fossil and biogenic life cycle emissions (considering the
namely bibliographic-published data, simulation data, as well as data­ capture system) embodied in the biofuel product (Fig. 2). Therefore, to
bases. For the biomass silviculture [60,61] and the biorefinery facility quantify the carbon emissions of CCS systems precisely, the biogenic
[62], bibliographic data was used. Data for transport and injection of CO2 captured via photosynthesis during biomass growth (embodied in
CO2 were retrieved from literature sources [68]. The GREET 1.3 data­ the biomass resource) is assigned a negative value to give credit to the
base was used for estimating the direct emissions of vehicles, including CO2 removed from the atmosphere. The carbon footprint accounting is
CO2, CH4 and NOx emissions, by subtracting the well-to-pump emissions then performed by considering all of the upstream and downstream
from the well-to-wheel emissions, both available in the said database activities and their corresponding direct and indirect (both biogenic and
[72]. fossil) GHG emissions occurring throughout the fuel’s value chain. The
With regards to SS3, data are based on a process simulation of the latter include, as well, the end-of-life direct emissions from burning the
CO2 capture system following the work by Adams II et al. (2014) [63]. biofuel in the engine. Furthermore, to assess the real potential to deliver
Further details regarding the process simulation for the capture and negative emissions (physical net removal of CO2 from the atmosphere),
compression of CO2 are presented in the Supplementary Material file. we consider a cradle-to-wheel approach (also known as cradle-to-grave
The inventory data for each subsystem are displayed in Tables S2-S6 in or well-to-wheel) [77]. Hence, based on this tailored LCA accounting
the Supplementary Material. system, a fuel is deemed carbon-negative if it achieves a negative GHG
emissions balance over its life cycle [14,79]. All data employed in this
2.5. Life cycle impact assessment method study are included in Table S7 in the Supplementary Material.

An attributional approach was followed to quantify a set of midpoint 3. Results and discussion
impact indicators. Characterization factors from the ReCiPe 1.1 Hier­
archist method [73] were applied using the SimaPro 9.0 software. The The results section presented below focus, firstly, on discussing the
Ecoinvent v3.5 database [69] was used for the modelling of the back­ CF results, to then extend the analysis to other environmental indicators,
ground processes. Our analysis covers the CF indicator derived from the investigating the potential occurrence of burden-shifting.
GW category from ReCiPe [74], expressed in kg CO2 eq, as well as a set
of mid-level impact categories provided by the same impact assessment 3.1. Carbon footprint assessment: Negativity potential
method. The latter include ozone depletion in kg CFC11 eq, ozone for­
mation in kg NOx eq, terrestrial acidification in kg SO2 eq, freshwater The CF was analyzed following the methodology explained in

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S. Bello et al. Applied Energy 279 (2020) 115884

Fig. 2. Carbon accounting of direct CO2 emissions in fossil and bio-based systems with and without CCS.

Section 2.5.1. Notably, we cover several fuel blends as well as national holds that increasing the bioethanol content decreases the CF for the
electricity mixes and renewable technologies (i.e., solar photovoltaic whole range of carbon intensities considered. However, in the scenarios
and wind energy), which differ in their CI (i.e., kg CO2eq⋅kWh− 1). The using natural gas as the heating source, some of the lines cross for high
base-case corresponds to the European average electricity mix. Recall carbon intensities. Consequently, higher bioethanol contents can lead to
that the electricity is consumed in the sawmill activities, the biorefinery larger CFs, e.g., E40 NG vs. E25 NG for a CI above 0.70
section, and also in the CO2 capture and compression stage (Fig. 1). kg CO2 eq⋅kWh− 1.
Fig. 3 shows the CF results as a function of the CI of the electricity For the bio-based heating scenarios, all bioethanol blends, except for
consumed by the process. Each scenario is depicted by a line whose slope E10 SC for carbon-intensities above 0.85 kg CO2 eq⋅kWh− 1, perform
depends on the specific composition of the blend. Similarly, the inter­ better than the business as usual (BAU) scenario (i.e., conventional
cept of the line is given by the concentration of bioethanol in the blend gasoline depicted with a horizontal blue line). However, for the sce­
and the heat source in the process. Higher slopes correspond to blends narios based on natural gas as the heating source for SS3, only the E40
with a higher concentration of bioethanol, in which the contribution of NG and the E85 NG scenarios would outperform the conventional
electricity towards the total emissions is higher. For a carbon-free benchmark gasoline for low carbon electricity sources. Notably, the only
electricity source, it holds that a higher bioethanol content results in a blend delivering negative emissions is E85 SC, which does so for CIs
lower CF. Furthermore, the efficiency of the engine increases with the below 0.91 kg CO2eq⋅kWh− 1. For the average electricity mix in Europe,
bioethanol content [80] (e.g., the energy consumed per distance trav­ E85 SC would deliver − 2.74 kg CO2 eq/100 km, while in Switzerland or
elled for the E40 is 2,677.9 J⋅m− 1, while for the E85 is 2,016.7 J⋅m− 1) France, the CF would be further reduced to − 4.62 kg CO2 eq/100 km
[72]. Therefore, increasing the bioethanol content in the blend provides and − 4.87 kg CO2 eq/100 km, respectively. Furthermore, wind power
environmental benefits directly related to the lower fuel requirements. could reduce the CF of E85 SC to − 5.05 kg CO2 eq/100 km. In contrast,
In all the bio-based heating scenarios (depicted in green in Fig. 3), it European countries such as Poland, which plans to maintain coal power

Fig. 3. Cradle-to-wheel carbon footprint (kg CO2

eq km− 1) for eight scenarios as a function of the
CI of the electricity mix (kg CO2 eq kWh− 1).
Green scenarios use sugarcane bagasse as the heat
source in SS3. Red scenarios use natural gas as
the heat source in SS3. The darker the shade of
the color, the higher the bioethanol content in the
blend (E10, E25, E40, E85). Vertical dotted lines
denote the carbon intensities of the electricity
mixes of some EU countries and renewable elec­
tricity technologies. For comparison purposes,
gasoline is depicted with a horizontal blue line.

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S. Bello et al. Applied Energy 279 (2020) 115884

plants to enhance its energy security [81], would be unable to produce capita emissions. Similarly, reductions of 37.51% in per capita emissions
biofuels leading to net negative emissions. (relative to average values) could be achieved in Europe [83].
Considering that a regular passenger car may typically travel an Meeting the environmental goals of the European Commission will
average of 14,000 km⋅yr− 1 [82], the potential for decarbonization of a critically depend on our ability to change the European vehicle fleet.
E85 SC vehicle would be − 382.98 kg CO2 eq⋅(car⋅yr)-1 assuming an According to the IPCC, the global transport sector could reduce its
average European electricity mix. The overall savings, however, should emissions 4.7 GtCO2 eq⋅yr− 1 by 2030 [5]. The implementation of
also consider the avoided emissions by gasoline replacement (3,121 carbon-negative bioethanol fueled vehicles could help to offset emis­
kg CO2 eq⋅(car⋅yr)-1 [72]). Considering, for instance, the average carbon sions from hard-to-abate aviation or shipping transportation [84].
emissions in Spain, i.e., 5,030 kg CO2 per capita for 2017 [83], the Considering the total passenger-car fleet in 2015 in the European Union
implementation of the E85 SC fuel could reduce 52.98% current per [82], replacing gasoline-fueled passenger vehicles by E85 SC vehicles

Fig. 4. Breakdown of contributions of each subsystem to the CF for the E85 SC and E10 NG scenarios expressed per 1 km travelled. Subplot A corresponds to the E85
SC, i.e., the best-case scenario, while subplot B corresponds to E10 NG, i.e., the worse-case scenario. Pie charts show the relative CF contributions per activity for
each subsystem.

7
S. Bello et al. Applied Energy 279 (2020) 115884

could reduce 0.88 GtCO2 eq yr− 1, which represents 18.79% (16.73% CO2 eq⋅km− 1 (i.e., 90% gasoline, 10% bioethanol). The emissions from
from the removal of gasoline cars and 2.06% from the negative emis­ the biomass pretreatment and biorefining activities are quite small
sions in E85 vehicles) of the global transportation sector reduction target (<2% of the total). In contrast, the CO2 capture and compression stage
for 2030 in the 1.5 ◦ C scenario (4.7 Gt CO2 eq⋅yr− 1). Note, however, that accounts for 11% of the total emissions due to the large amount of en­
the final CDR potential required to meet the climate targets remains ergy required to regenerate the amine in the CCS system. Most of the
uncertain as it ultimately depends on the delay of the mitigation actions. positive emissions correspond to the biofuel combustion in the vehicle,
Moreover, other BECCS technologies, such as biomass conversion to around 60% of the total well-to-wheel emissions; meanwhile, the
power and heat, as well as other negative technologies and practices in emissions of the silviculture and sawmill activities and the CO2 trans­
the portfolio of CDR options, could help to reduce the reliance on BECCS portation are, again, negligible (<0.5%).
[13]. Notably, the large scale deployment of BECCS will face many The breakdown of the CO2 emissions per activity of each subsystem
challenges, such as sustainability concerns (e.g., land-system change and (pie charts in Fig. 4) allows identifying environmental hotspots where
loss of biodiversity) [51], governance problems, sociopolitical con­ potential improvement efforts are most needed. The heat consumed to
straints and economic viability barriers [85]. regenerate the MEA is a major source of CO2 emissions in SS3. Hence,
The pathways to avoid overshooting the 1.5 ◦ C target by 2050 the CF performance of biofuels could be improved by using low-carbon
require removing globally around 8 Gt CO2⋅yr− 1 by BECCS [5]. heating sources or taking advantage of waste heat from industrial ac­
Removing this amount of carbon using E85 SC vehicles would require tivities. Identifying new solvents or developing new catalytic processes
producing 3,400 GL per year of lignocellulosic bioethanol (considering to reduce energy consumption in the CCS system (SS3) could also help to
the full displacement of gasoline). The annual world production of reduce this contribution [88,89]. At present, this is the primary hotspot
bioethanol in 2018 was 110 GL, while only<1% of the global bioethanol for this subsystem in both the natural gas scenarios (93% share within
production in Europe was second-generation fuel [86]. Hence, the the subsystem) and the bio-based heating scenarios (65% share within
commercialization of lignocellulosic bioethanol with CCS should be the subsystem). As for the biorefinery plant (SS2), the primary hotspot is
dramatically increased for this fuel to play a significant role in given jointly by the consumption of chemicals and heat, with 32% and
combatting climate change. Note, however, that the CDR that would be 38% shares of the total impact, respectively.
required to reach the climate goals is expected to be provided by BECCS Furthermore, the feedstock (SS1) contributes with 1.03% in scenario
applied also to the power and heating sector. E85 SC and 0.25% in scenario E10 NG. We note that the impact of beech
To provide a full picture of the CF balance, we next analyze the wood (given by the fertilizers, water use, machinery and associated
breakdown of emissions by subsystem for the extreme cases, i.e., the E85 yield) may vary in forestry residues of other species (e.g., birch, euca­
SC and E10 NG scenarios (waterfall plot in Fig. 4, subplot A and subplot lyptus, spruce) [90]. However, these changes might not be that signifi­
B, respectively) in the base case (i.e., European average electricity mix). cant unless second-generation biomass (i.e., wood or residues) is
Due to space limitations, the results for the remaining scenarios are replaced by first-generation biomass (i.e., edible crops). Notably, the
presented in the Supplementary Material (Figures S3-S8). latter shows worse performance in all of the environmental categories
For the E85 SC scenario (Fig. 4, subplot A), the negative emissions (Figure S10) and also competes with food [91]. Furthermore, the process
from the CO2 uptake during biomass growth account for 52% of the total would need to be adjusted to accommodate other feedstocks, e.g., the
absolute value. The direct emissions in the vehicle engine are the most biomass pretreatment method might entail a lower environmental
significant positive contributor to the total CF impact (28%), followed impact when dealing with first-generation feedstocks [92]. Specifically,
by the capture and compression plant (SS3), and then the production Organosolv or other pretreatment methods for delignification, such as
process in the biorefinery (SS2), which account for 9.1% and 8.1% of the steam explosion or liquid hot water, are generally more energy-intensive
total emissions, respectively. In contrast, the contributions of the silvi­ due to the recalcitrance of biomass [93].
culture and sawmill-related activities (SS1) and the CO2 pipeline Regardless of the fuel blend, the capture and compression plant
transportation and injection (SS4) are both marginal (1.03 and 0.26% subsystem causes a significant impact (Figs. 4 and 5). With gasoline
relative contributions, respectively). Overall, the negative emissions percentages above 75% in the blend, however, the hotspot shifts from
exceed the positive ones, thereby resulting in a carbon-negative biofuel the capture plant to the direct emissions from the gasoline combustion
providing − 0.027 kg CO2 eq⋅km− 1. (Figures S3-S8). The development of new sorbents could help to reduce
The sensitivity of the CF results to the CO2 transport distance to the the substantial energy requirements (and costs) of the CO2 separation,
geological site has been studied in the range of 1–400 km, considering thereby decreasing its impact [89]. Accordingly, Figure S11 in the
that after the first 200 km, recompression of the CO2 is needed [68] Supplementary Material provides the results of a sensitivity analysis on
(Figure S9). The CF of the scenarios varies very little with the CO2 the heating demand of the CCS plant for the different scenarios bench­
transportation distance, ranging from 0.11% to 8.40% of increase in CF marked against bibliographic heat demands for MEA absorption pro­
for the E10 NG and the E85 SC scenarios, respectively. Note that the cesses [94–99]. Our CCS system requires 7.5 MJ per kg CO2 captured, an
overall conclusions remain qualitatively the same, as the scenarios still amount slightly above the values reported in the literature (5.5–3.5
lead to a negative balance (although the net carbon efficiency would be MJ⋅kg− 1 CO2 captured). Note that, for lower heating needs, the E85 NG
reduced). The transport distance from the BECCS plant to the geological would be able to achieve carbon-negativity, even when relying on nat­
site, together with the distance to the areas of larger lignocellulosic ural gas as the heating source (Figure S11). These results indicate that
biomass availability, will determine the optimal geographical location the CF of biofuels could be further improved by reducing the heating
of the plant. The low emissions of the CO2 transport through pipelines needs for the solvent regeneration and by exploiting waste-heat recovery
and the low energy density of biomass make locations near the biomass options and other synergies with other industries [28]. Ultimately, the
source more appealing. However, the need of infrastructure for CO2 impact of the heating demand is dependent on its magnitude (MJ⋅kg− 1
transport could hinder a quick deployment of BECCS for biofuels, which CO2 captured) as well as the heating source. As presented in Figure S11
might be essential to meet the decarbonization goals [39,87]. in the Supplementary Material, for bio-based heating, lowering the en­
Regarding E10 NG (Fig. 4, subplot B), its positive emissions exceed ergy consumption would not affect that much the impact, especially for
the negative ones linked to the uptake of CO2 during the biomass values below 35 GJ⋅kg− 1 bioethanol. On the contrary, heating via nat­
growth, thereby making the fuel carbon-positive on a life cycle basis ural gas offers more room for improvement.
(+0.25 kg CO2 eq⋅km− 1). Notably, negative emissions from biomass We note that very pure CO2 streams from fermentation could be
growth represent 13% of the total emissions (− 0.043 kg CO2 eq⋅km− 1), handled via direct dehydration and compression of the gas stream,
and (in absolute value) lie slightly below the positive cradle-to-gate thereby reducing the energy needs substantially [9]. Flue gas with a
emissions embodied in the gasoline contained in the blend, 0.044 kg lower CO2 concentration would increase the energy and solvent

8
S. Bello et al. Applied Energy 279 (2020) 115884

Fig. 5. Comparative evaluation of environmental profiles for the best-case scenario E85 SC, the worst-case scenario E10 NG and the BAU alternative, i.e., con­
ventional gasoline. OD: ozone depletion, OF: ozone formation, TA: terrestrial acidification, FE: freshwater eutrophication, ME: marine eutrophication, FET: fresh­
water ecotoxicity, MET: marine ecotoxicity, HT: human toxicity, LU: land use, FS: fossil resource scarcity and WC: water consumption.

requirements in CCS, and, consequently, the impact of SS3. Thus, the and fossil resource scarcity, where it is inferior due to its higher content
BECCS potential for net CO2 removal would be lower in less concen­ of fossil-based resources (gasoline in the blend and natural gas for
trated streams and higher in more concentrated ones. The CO2 source, heating). Therefore, it becomes clear that the potential collateral dam­
therefore, impacts the net removal efficiency and, thus, needs to be age of biofuels should not be overlooked.
considered in the selection of the capture method [24]. Either way, there Delving into the drivers of burden-shifting, the breakdown of im­
is a clear need to cut down the energy needs, mostly through better pacts in Fig. 5 allows pinpointing the main hotspots in each impact
solvents and, whenever possible, through the use of waste heat (or heat category. The relative burdens and environmental profile change sub­
from waste biomass). stantially attending to the scenario analyzed (Fig. 5), which can be
further observed in Figures S3 through S8 in the Supplementary Material
for the scenarios omitted here. Overall, for blends rich in bioethanol, the
3.2. Other environmental implications and burden-shifting biorefinery (SS2) and the CO2 capture and compression (SS3), are the
main hotspots of the system in most of the impact categories.
We now turn our attention to the potential occurrence of burden- The ozone depletion category for the bioethanol blends worsens with
shifting, that is, the collateral damage to some environmental areas of respect to gasoline, mainly due to the high heating needs in the capture
protection taking place when attempting to mitigate carbon emissions. process (SS3) and the marginal increase in the unburned hydrocarbons
Accordingly, Fig. 5 (and Tables S8 and S9 in the Supplementary Mate­ and nitrogen oxide in the engines [101]. Similarly, in the ozone for­
rial), shows the relative performance (compared to gasoline) of the two mation and terrestrial acidification categories, the E85 SC performs
extreme scenarios (E85 SC and E10 NG) in the midpoint impacts of the worse than the E10 NG and gasoline alternatives due to the large im­
ReCiPe 1.1 pacts of the biorefinery and the capture activities. Note that the impact
Indeed, burden-shifting takes place in the E85 SC fuel, which dis­ of the fuel utilization subsystem (SS5) is negligible in most non-climate
plays a negative CF (Fig. 3) and emerges as the best option in fossil change related impact categories, with the exception of ozone-related
resource scarcity but shows the worst performance in all the other indicators (ozone depletion and ozone formation) where it represents
impact categories [100]. . Similarly, E10 NG performs worse than gas­ around 18% of the total impact in both categories. As seen in Fig. 5, the
oline in all the categories, except for fossil resource scarcity and E10 NG fuel performs slightly better than gasoline due to the reduction
terrestrial acidification. The latter impacts are strongly linked to fossil in the emissions of organic compounds (contributing to the ozone for­
fuel combustion and the atmospheric deposition of acidifying com­ mation burdens), nitrogen oxides and ammonia (main drivers of the
pounds. Note that, due to the use of chemicals in SS2 (e.g., sulfuric acid), acidification category). These emissions are strongly linked to the
increasing the bioethanol content worsens the TA and OF categories. refining and combustion of fossil fuels.
Our results show that burden-shifting is particularly critical in ma­ Freshwater eutrophication and marine eutrophication worsen sub­
rine eutrophication, land use and water consumption, i.e., E85 SC bio­ stantially in the E85 SC and, to a lesser extent, in the E10 NG. The main
fuel with 42.45, 82.91 and 23.59 times higher impact relative to drivers of these impacts are the use of nitrogen fertilizers (soil N2O,
gasoline, respectively (and 1.46, 1.48 and 2.34 times in each category, ammonia and NOx emissions) and phosphorous fertilizers (phosphoric
for the E10 NG benchmarked against gasoline). Furthermore, the E10 acid emissions). Both compounds are linked to the production of
NG outperforms the E85 SC biofuel in all the categories except for CF

9
S. Bello et al. Applied Energy 279 (2020) 115884

dedicated bioenergy crops (i.e., the sugar cane bagasse employed for climate change mitigation may exacerbate impacts on eutrophication,
heating in SS3). In the marine eutrophication category, 97% of the im­ ozone depletion and formation, toxicity, land use, and water consump­
pacts of E85 SC are due to the capture and compression plant. This high tion. Minimizing energy consumption in the CO2 capture and
impact might be linked to the nutrient accumulation in water bodies due compression stages, e.g., via heat integration and the use of biobased
to the loss of nitrogen and phosphorus fertilizers (associated with the residues for heating, could reduce the collateral damage to other envi­
heat source) and the use of monoethanolamine. The latter is an amine- ronmental areas. Nevertheless, trade-offs will arise in the deployment of
compound that can act as a driver of nutrient oversupply in marine biofuels, which should not be overlooked to avoid potential undesirable
environments. side-effects.
Ecotoxicity in the freshwater and marine compartments also worsens Overall, the BECCS concept applied to biorefineries offers excellent
in both biofuels (Fig. 5). Particularly, E85 SC increases the ecotoxicity opportunities to reduce the carbon footprint of the passenger-vehicle
impacts by 74% and 69%, respectively (and 30% and 26%, for the E10 fleet in the transition towards a carbon–neutral (or even carbon-
NG). The trend in human toxicity is quite similar, where the best option negative) mobility system. In this context, the occurrence and severity
is, again, gasoline followed by the E10 NG and, finally, the E85 SC fuel. of burden-shifting should be analyzed in-depth.
For scenarios rich in bioethanol, the main contributors are the CO2
capture and compression (SS3) and biorefinery sub-systems (SS2), while CRediT authorship contribution statement
for the others, the primary hotspot is the gasoline. This might be due to
the pesticides and fertilizers consumed during the biomass growth (e.g., Sara Bello: Formal analysis, Investigation, Methodology, Writing -
sugarcane cultivation), which evaporate and runoff into freshwater and original draft, Writing - review & editing, Visualization. Ángel Galán-
marine water bodies, and also to some compounds involved in the Martín: Conceptualization, Methodology, Writing - review & editing,
pretreatment and fermentation of the wood residues [102]. Visualization. Gumersindo Feijoo: Methodology, Writing - review &
Regarding the land use and water consumption, the E85 SC fuel is by editing. Maria Teresa Moreira: Conceptualization, Methodology,
far the worst option, with the E10 NG alternative lying close to gasoline. Writing - review & editing. Gonzalo Guillén-Gosálbez: Conceptuali­
The negative impact in these categories is mainly due to the contribution zation, Methodology, Writing - review & editing, Supervision.
of the sugar cane burnt to provide heat in the CO2 capture system (SS3).
The land use impact is mostly linked to the transformation and occu­ Declaration of Competing Interest
pation of land to grow the sugarcane feedstock. Furthermore, the in­
crease in water consumption is due to the irrigation needs and the water The authors declare that they have no known competing financial
required for pulp washing and lignin precipitation (SS2). interests or personal relationships that could have appeared to influence
the work reported in this paper.
4. Conclusions
Acknowledgements
In this work, we investigated the concept of BECCS applied to a
biorefinery coupled with CCS that converts wood waste material into This contribution was supported by the European project iFermenter
bioethanol. We showed that blends with higher contents of bioethanol (Grant Agreement 790507). S. Bello, G. Feijoo and M.T. Moreira belong
have the potential to deliver negative emissions. Moreover, in most of to the Galician Competitive Research Group GRC ED431C 2017/29 and
the scenarios, biofuels with CCS reduce the CF of conventional gasoline, to the CRETUS Strategic Partnership (ED431E 2018/01). All these pro­
more so when using low-carbon electricity and/or biomass as the grams are co-funded by FEDER (EU).
heating source in the process. Particularly, with an E85 blend, a net
balance of − 2.74 kg CO2 eq per 100 km travelled could be attained Appendix A. Supplementary data
considering the European average electricity mix and heating for the
capture and compression system supplied by biomass resources. Supplementary data to this article can be found online at https://doi.
Furthermore, electricity mixes with higher shares of renewable en­ org/10.1016/j.apenergy.2020.115884.
ergy (e.g., Switzerland, France or Norway) would double the final net
amount of negative emissions provided (e.g., − 5.01 kg CO2 eq/100 km
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