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Comparative life cycle assessment of hydrogen-


fuelled passenger cars

Daniele Candelaresi a, Antonio Valente b,*, Diego Iribarren c,


Javier Dufour c,d, Giuseppe Spazzafumo a
a
Department of Civil and Mechanical Engineering, University of Cassino and Southern Lazio, Cassino, Italy
b
Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering, ETH Zurich, 8093,
Zurich, Switzerland
c
Systems Analysis Unit, IMDEA Energy, 28935, Mostoles, Spain
d
Chemical and Environmental Engineering Group, Rey Juan Carlos University, 28933, Mostoles, Spain

research highlights

 Environmental performance comparison between different hydrogen-powered vehicles.


 Comparison between fuel cell and hydrogen internal combustion engine vehicles.
 Life cycle assessment of hybrid electric vehicles fed with hydrogen.
 Natural gas-hydrogen and gasoline-hydrogen vehicles are assessed.
 Vehicles fuelled with renewable hydrogen are excellent decarbonisation solutions.

article info abstract

Article history: In order to achieve gradual but timely decarbonisation of the transport sector, it is essential
Received 10 October 2020 to evaluate which types of vehicles provide a suitable environmental performance while
Received in revised form allowing the use of hydrogen as a fuel. This work compares the environmental life-cycle
20 November 2020 performance of three different passenger cars fuelled by hydrogen: a fuel cell electric
Accepted 6 January 2021 vehicle, an internal combustion engine car, and a hybrid electric vehicle. Besides, two
Available online 6 February 2021 vehicles that use hydrogen in a mixture with natural gas or gasoline were considered. In all
cases, hydrogen produced by wind power electrolysis was assumed. The resultant life-
Keywords: cycle profiles were benchmarked against those of a compressed natural gas car and a
Wind electrolysis hybrid electric vehicle fed with natural gas. Vehicle infrastructure was identified as the
Sustainable mobility main source of environmental burdens. Nevertheless, the three pure hydrogen vehicles
Fuel cell electric vehicle were all found to be excellent decarbonisation solutions, whereas vehicles that use
Hydrogen engine hydrogen mixed with natural gas or gasoline represent good opportunities to encourage
Hybrid electric vehicle the use of hydrogen in the short term while reducing emissions compared to ordinary
Hythane vehicles.
© 2021 The Authors. Published by Elsevier Ltd on behalf of Hydrogen Energy Publications
LLC. This is an open access article under the CC BY license (http://creativecommons.org/
licenses/by/4.0/).

* Corresponding author.
E-mail address: antonio.valente@chem.ethz.ch (A. Valente).
https://doi.org/10.1016/j.ijhydene.2021.01.034
0360-3199/© 2021 The Authors. Published by Elsevier Ltd on behalf of Hydrogen Energy Publications LLC. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
35962 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 5 9 6 1 e3 5 9 7 3

around 20% or less for the evaluated impact indicators,


Introduction shifting the main contribution from the fuel to the vehicle
infrastructure. Considering this finding as the background,
In recent years, environmental concerns have grown at an this work aims to identify the environmentally-preferred
ever-increasing rate. In the Paris agreement, 195 countries hydrogen-fuelled vehicle among different alternatives.
adopted the first universal and legally binding covenant on the LCA studies on hydrogen vehicles usually consider only
global climate, defining a global action plan to mitigate fuel cell electric vehicles (FCEV). On the other hand, the few
climate change and trying to keep global warming well below WTW analyses on hydrogen vehicles equipped with an in-
þ2  C compared to the pre-industrial era [1]. Regarding ternal combustion engine do not extend the boundaries of the
Europe, the carbon-neutrality goal has been set by 2050 [2]. system to the vehicle itself. Hence, this study aims to compare
The Intergovernmental Panel on Climate Change clearly different hydrogen powertrain technologies by means of a
states that it is urgent to limit global warming to þ1.5  C rather thorough LCA. Technologies for the use of both pure hydrogen
than þ2  C [3]. The leading cause of these environmental is- and hydrogen mixed with fossil-based fuels were considered
sues lies in the widespread use of fossil fuels for energy pur- since the latter could be a short-term solution to reduce
poses. In 2018, world primary energy demand amounted to vehicle emissions when hydrogen production is not large
14,282 million tonnes of oil equivalent (Mtoe), of which 81% enough to fuel many vehicles. The main novelties of this study
was met by fossil fuels [4]. In particular, the transport sector lie thus in (i) comparing the life-cycle environmental perfor-
alone accounted for 2890 Mtoe, equal to 20% of the global mance of different hydrogen-powered vehicles (FCEV,
primary energy demand. To date, this demand is met almost hydrogen vehicles equipped with internal combustion en-
entirely by fossil fuels (96%) and dominated by petroleum- gines, and hydrogen hybrid electric vehicles), and (ii)
derived products (92%). Moreover, there is a continuous providing detailed life-cycle inventories and indicators of ve-
growth in fuel consumption for transport and an increase in hicles equipped with internal combustion engines fed with
the number of vehicles, especially in non-OECD countries [5]. mixtures of hydrogen and a conventional fuel (natural gas or
For these reasons, the transport sector represents a hard gasoline).
core of the energy transition, being the only sector to have
shown an increase, rather than a reduction, in greenhouse gas
emissions [6]. In particular, light-duty vehicles and passenger Material and methods
cars represent a large part (46%) of the energy demand from
transport, namely 1323 Mtoe in 2018 [5]. Hydrogen is set to The goal of this comparative LCA study is to identify, ac-
play a strategic role in the decarbonisation of the transport cording to the current technology level, which type of vehicle
sector [7]. Due to environmental criteria, its production should provides a suitable environmental performance when using
rely on renewable energy sources [8]. Furthermore, hydrogen hydrogen produced from renewable energy sources. In
does not involve direct carbon emissions in its use, which particular, all vehicles were assumed to be powered by
makes it a promising clean fuel for transportation. However, hydrogen produced by WPE [16]. Three car options fuelled only
comprehensive analyses following a life-cycle perspective are by hydrogen were considered: (i) a fuel cell electric vehicle
required to check the environmental suitability of hydrogen (FCEV), (ii) a hydrogen car equipped with an internal com-
and vehicle systems. bustion engine (H2-ICE), and (iii) a hybrid car fuelled with
In this regard, the standardised methodology of Life Cycle hydrogen (HEV H2-ICE). Hybrid electric vehicles (HEV) are
Assessment (LCA) is widely applied to identify potential bot- partially electrified vehicles, consisting mainly of an internal
tlenecks in the environmental life-cycle performance of combustion engine, an electric motor, and a small battery.
product systems [9,10]. Regarding LCA in the automotive The benchmarking of their environmental life-cycle per-
sector, well-to-wheels (WTW) analyses are often conducted, formance against a compressed natural gas (CNG) vehicle and
which usually include subsets known as well-to-tank (WTT) its hybrid version (HEV CNG) was pursued. Another objective
and tank-to-wheels (TTW) according to the definition of the addresses further comparison with two passenger vehicles
system limits [11e13]. WTW analyses consider all phases of fuelled by hydrogen-fossil fuel blends: a hythane vehicle
fuel production and distribution up to the vehicle tank and, in equipped with an internal combustion engine fed with a
addition, the fuel use phase. A vehicle LCA, in addition to the gaseous mixture of 20% (vol.) H2 and 80% (vol.) natural gas
fuel-related stages, should also consider the manufacturing, (Hythane), and a dual-fuel hydrogen-gasoline vehicle equip-
maintenance and end-of-life phases of the vehicle itself, thus ped with an internal combustion engine (H2-Gasoline)
extending the boundaries of the system [14,15]. considering an energy ratio of the mixture equal to that of
Valente et al. [16] explored the role played by hydrogen as hythane (i.e., H2 provides 7.3% of the mixture energy). Fig. 1
the fuel in the life-cycle environmental performance of a fuel shows a simplified diagram of the various vehicle concepts
cell passenger car, addressing three different hydrogen pro- considered.
duction technologies. They showed that the choice of
hydrogen production technology significantly affects the Technical features of the case studies
whole life-cycle performance of vehicles. Renewable-based
hydrogen, especially when produced through wind power An average European gasoline car, sedan, 5-door, belonging to
electrolysis (WPE), was identified as the preferred fuel option. segment C (small family cars/compact cars/medium cars)
When using hydrogen from WPE, the ratio of hydrogen impact [15,17,18] was considered as reference, with a rated vehicle
to the total impact of the whole system dropped to values
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Fig. 1 e Vehicle concepts under comparison.

power of 80 kW [19]. The main technical specifications of the


Table 2 e Main technical characteristics of the hydrogen
considered average vehicle are listed in Table 1.
vehicles considered in the study.
While FCEVs have already been modelled in Ref. [16], the
Parameter (unit) FCEV H2-ICE HEV H2-ICE
remaining vehicles were modelled taking into account com-
mon components such as the glider (body, chassis, glass H2 consumption (kg/100 km) 0.76 1.68 1.27
surfaces, etc.) as well as all major differences between pow- Weight (kg) 1800 1380 1550
Lifespan (km travelled) 190,000a 300,000b 300,000b
ertrains. Only spark ignition ICE was modelled in this work,
Thermal engine power (kW) e 80 58.4
while compression ignition (diesel) ICE was not considered. Electric motor power (kW) 80 e 48.6
All HEVs considered correspond to the full-hybrid, series/ Driving range (km) 600 300 400
parallel type. The vehicles were modelled by breaking down Storage pressure (bar) 700 700 700
the inventory into main subsystems and components (ICE, air Tank volume (l) 120 120 120
intake system, fuel system, exhaust gas system, control unit, Hydrogen (kg) 5 5 5
etc.). Each subsystem was then subdivided into various com- a
Based on [22].
b
ponents (catalytic converter, exhaust gas manifold, muffler, Based on [24,25].
piping, gaskets, lambda sensors, etc.) [20,21]. The main tech-
nical characteristics of the three hydrogen vehicles under
comparison are presented in Table 2. Vehicle weights and (composite material). A full 120-litre tank at 700 bar can store
lifespans differ, mainly due to differences in powertrains. The about 5 kg H2.
lifespan of the FCEV was assumed to be that of the fuel cell
stack, limited by the durability of the membranes. However, Fuel cell electric vehicle (FCEV)
research efforts are currently focused on improving the
durability of fuel cell membranes in order to reach a life target The FCEV, based on a previous work [16], includes the
of 250,000 km travelled [22,23]. For the other vehicles, the following main sub-inventories: fuel cell based on [26e28],
lifespan was considered to be that of the ICE [24,25]. electric motor based on [29], battery (lithium-ion NCM type)
In the three cases, the same type of tank was assumed, based on [30,31], hydrogen tank based on [28,32,33], balance of
with gaseous hydrogen storage at 700 bar in a type IV tank plant (BOP) based on [28,34], and power control unit (PCU)
based on [28,35].

Table 1 e Main technical specifications of an average Hydrogen internal combustion engine (H2-ICE) vehicle
European passenger car.
Parameter Value The H2-ICE vehicle burns hydrogen and air in a spark ignition
Vehicle rated power 80 kW ICE. Thanks to the combustion characteristics, it can count on
Kerb weight 1200e1350 kg very high efficiency and low polluting emissions, also allowing
Lifespan 250,000e300,000 km the use of ultra-lean (air-fuel) mixtures [36,37]. Structurally, its
(20 years) ICE is almost identical to a CNG one [38e40], while there are
Average European driving 12,000e15,000 km year1 minor differences between the two vehicles mainly related to
performance
the storage of hydrogen on board.
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Hydrogen hybrid electric vehicle (HEV H2-ICE) cycle, directly (in the cylinder [56]) or indirectly (in the air
intake manifold [57]), together with the conventional gasoline
The hydrogen-fuelled HEV considered in this study burns injection. Thus, a part of gasoline is replaced with hydrogen.
hydrogen and air within an ICE as in the previous case, but the An engine with these characteristics is defined as dual-fuel
main difference lies in the hybridisation of the propulsion [45]; the ICE burns air-gasoline-hydrogen mixtures, but never
system: the thermal engine (ICE) is paired with an electric only hydrogen or gasoline. In this vehicle, two separate tanks
motor/generator that produces electrical power on board, and and fuel distribution systems are present, one for gasoline and
a small battery to store the electricity generated [41,42]. In this another for hydrogen.
way, the ICE can work more often at its point of maximum
efficiency. The vehicle can travel for a few kilometres in full- LCA framework
electric mode, transferring energy from the battery to the
electric motor. It can also take advantage of regenerative The LCA methodology was applied to each vehicle system.
braking to recharge the battery. The degree of hybridisation According to the standards [9,10], LCA involves four interre-
(mild, full, plug-in, range-extender) also defines the battery lated stages. In “goal and scope definition”, key aspects such
size and the ratio of the power of the electrical system to that as the system's function and boundaries, the impact cate-
of the thermal system. The vehicle considered in this study is gories and the functional unit (FU) are defined. The second
a full-hybrid of the series/parallel type [43,44]. stage, “life cycle inventory analysis”, consists in data collec-
tion for the main net flows (materials, energy, emissions and
Compressed natural gas (CNG) vehicle waste) that enter or leave the system's boundaries. In the third
stage, “life cycle impact assessment” (LCIA), the potential
Regarding the CNG car, a mono-fuel vehicle designed to run environmental impacts are quantified through specific char-
only on natural gas was considered. It should be noted that to acterisation factors that convert an elementary flow into a
date, in some countries, commercial CNG vehicles classified level of impact. In the last stage, “interpretation”, the main
as mono-fuel still involve an additional small gasoline tank conclusions of the study are drawn according to its goals and
with a capacity below 14 L for fuel reserve and vehicle range. scope.
While a bi-fuel vehicle has two independent fuel systems that Fig. 2 shows the boundaries considered for each vehicle
can run alternately [45], better performances could be ach- system, which involve both the fuel life cycle and the vehicle
ieved if engines were optimised for the use of only CNG [46,47]. life cycle [14,24]. The former includes the stages of production,
The engine considered in this study burns only CNG. distribution and use of the fuel as a WTW-type analysis [12].
The latter involves the vehicle life-cycle stages of
CNG HEV manufacturing, operation, and maintenance.
The fuel and vehicle life cycles converge in the vehicle
The CNG HEV is a vehicle with a hybrid electric/thermal pro- operation phase, when the vehicle tank is filled with fuel and
pulsion, whose ICE burns CNG and air [48]. This vehicle rep- this is used to move the vehicle [14]. A conventional WTW
resents the most likely upgrade of the CNG vehicle, as both analysis would consider only the complete fuel life cycle, from
CNG and hybrid electric vehicles are two alternative technol- cradle to grave. A complete LCA would instead include all
ogies significantly widespread today [49,50]. stages of both the vehicle life cycle and the fuel life cycle
[12,15,58]. However, it should be noted that vehicle end-of-life
Hythane ICE vehicle was not included in this study due to the acknowledged need
for robust inventory data on this stage [59,60]. As shown in
Hythane® (also known as HCNG20) is a commercial name for a Fig. 2, the FU of the study was defined as 1 km travelled by
blend of hydrogen at 20% (vol.) and natural gas at 80% (vol.). As each vehicle.
far as the hythane-powered vehicle is concerned, it can be The life-cycle environmental performance of each vehicle
considered almost identical to a CNG vehicle. This vehicle system was characterised in terms of global warming impact
burns hythane and air in a spark ignition ICE [51,52]. One of potential (GWP), acidification impact potential (AP) and cu-
the main advantages of hythane lies in the technical possi- mulative non-renewable energy demand (CED) using IPCC
bility of transporting hydrogen through the natural gas [61], CML [62] and VDI [63] methods, respectively. The selec-
network, without the need to separate the two fuels before tion of these categories was based on their relevance in the
use. It is thus possible to refuel the vehicle directly with specific field of hydrogen energy systems according to the
hythane (already mixed at the refuelling station), which can literature review by Valente et al. [64] on LCA of hydrogen-
be stored in a tank similar to that of CNG vehicles. Current related systems.
CNG cars could be converted into hythane vehicles with minor
modifications. Data acquisition

Dual-fuel H2-Gasoline ICE vehicle In this section, life-cycle inventories are provided for each
vehicle being compared. Concerning fuels, harmonised car-
The hydrogen-gasoline vehicle is similar to a conventional bon [65], acidification [66] and non-renewable energy [67]
gasoline-powered car with the addition of a separate fuel footprints were used for the production of hydrogen via WPE
system dedicated to pure hydrogen [53e55]. Hydrogen is ethus including capital goodse but adapting the system to the
injected in the engine in small quantities at each operating hydrogen pressure of 700 bar [16]. Hydrogen distribution was
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Fig. 2 e System’s boundaries.

considered via road transport (100 km) [68]. Regarding fossil but adapted to the nominal vehicle power (80 kW). The ICE
fuels, background data from the ecoinvent database [69] were was considered as in the H2-ICE vehicle, but with lower
used. In the case of hythane, hydrogen was assumed to be nominal power (58.4 kW). The fuel system and the exhaust
distributed (100 km) together with natural gas via pipeline up system were assumed the same as in H2-ICE. The electric
to the refuelling point [68]. motor inventory was based on [29,35] and assumed the same
The main inventory data for vehicle manufacturing are as the FCEV electric motor, but sized for lower nominal power
presented in Table 3. The main data sources for vehicle (48.6 kW). The Li-ion battery [30,31] and the hydrogen tank
manufacturing, operation and maintenance were well- [28,32,33] inventories were considered the same as in the
established life cycle databases (ecoinvent [69] and GREET FCEV. Hybrid vehicles involve the use of a planetary mecha-
model [70]), industry specifications, manufacturer's state- nism for the gearbox, which allows energy recovery during
ments, reports and scientific literature (as further specified in braking, and the presence of a PCU (AC/DC inverter, DC/DC
each inventory table). For commercially available vehicles, converter, battery charger and management system, and
data were retrieved from technical datasheets released by power distribution unit) [35] as in the FCEV.
manufacturers. On the other hand, for non-commercially Regarding the CNG vehicle, the main blocks are the ICE,
available vehicles, data collection was based on specific the CNG tank, the fuel system, and the exhaust system. A
literature. 100-litre CNG-II tank type was considered, with 200 bar as
The body and the chassis of ICE and HEV vehicles were storage pressure [34,85]. Platinum group metals (PGM) in the
modelled based on GREET [70], in proportion to a kerb weight TWC were modelled by taking into account the emission
of the reference vehicle of 1250 kg (Table S1 in Supplementary characteristics of a CNG engine [71e76]. In the CNG HEV, the
Information for further details). HEV and ICE vehicles were same components of a CNG vehicle were considered, with
considered to involve the same glider; therefore, weight dif- the addition of the electrical system typical of hybrid vehi-
ferences in vehicles are due to differences in powertrain cles. The thermal and electrical systems were sized as for
configurations (additional components such as tanks and HEV H2-ICE.
batteries). Details on inventory data for FCEV body, chassis The inventory of the hythane vehicle slightly differs from
and fluids are provided in Supplementary Information (Tables that of the CNG car. There is a single cylinder in which the
S1eS2). hythane is stored at pressures similar to those of natural gas,
Regarding the H2-ICE vehicle, the main structural modifi- enabling the use of CNG-I (all metal cylinders) or CNG-II (metal
cations ‒with respect to the CNG vehicle‒ for the use of liner hoop-wrapped with glass fibre and epoxy resin) type
hydrogen were taken into account (e.g., hydrogen tank, fuel tanks which can store gases up to 200 bar and 250 bar,
distribution system, and modifications to the catalytic con- respectively [85]. The use of more resistant cylinders (type III
verter in the exhaust system). It should be noted that or IV) could be considered in order to increase the pressure so
embrittlement does not represent a limitation for the use of as to recover the space taken away by the addition of
hydrogen in the combustion chamber since the commonly hydrogen and increase driving range. Additional seals and
used materials already offer good resistance to this phenom- safety systems to avoid possible backfires due to the increased
enon [36,40,77,78]. The inventory for the manufacturing of an flammability range are also present. The engine has no sig-
ICE car was mainly based on Notter [29] and ecoinvent (Golf nificant changes compared to previous cases, except for small
A4) passenger car [79e81]. Tyres were based on [82]. The changes in the gas injectors. The load of noble metals inside
hydrogen tank was considered to be the same as that of the the TWC is similar to that of the CNG vehicle. However,
FCEV. The fuel system (adapted from that of the CNG vehicle considering combustion improvements from the addition of
[34,69]) includes pipes, fittings, gaskets, valves, pressure hydrogen, it is possible to reduce the PGM load in the TWC.
reducer, safety system, etc. The exhaust system was based on Hydrogen addition involves a reduction in unburnt total hy-
[29,32,34] and noble metals loads in the three-way catalytic drocarbons (HC) and CH4, greater CO conversion to CO2, and
converter (TWC) were adjusted with respect to engine emis- greater tolerance to exhaust gas recirculation (EGR) and ultra-
sions [71e76]. lean combustion (decreasing NOx emissions). In the present
Concerning the inventory of HEV H2-ICE, the ICE and the study, the inventory of the hythane vehicle includes a CNG-II
electric engine were based on [83] and other sources [29,35,84], tank (200 bar) with the modifications needed to use hydrogen.
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Table 3 e Main inventory data for vehicle manufacture (values per one vehicle).
Item Unit FCEV H2-ICE HEV H2-ICE CNG HEV CNG Hythane H2- Gasoline Ref. for
inventory
Body and chassis p 1.00 1.00 1.00 1.00 1.00 1.00 1.00 Table S1
Fluids p 1.00 1.00 1.00 1.00 1.00 1.00 1.00 Table S2
ICE kW e 80.00 58.40 80.00 58.40 80.00 80.00 Tables S3e4
Steel, low-alloyed kg e 50.41 36.80 50.41 36.80 50.41 51.86
Aluminium kg e 41.40 30.22 41.40 30.22 41.40 42.85
Polyphenylene kg e 24.68 18.02 24.68 18.02 24.68 27.59
sulphide
Lubricating oil kg e 8.73 6.37 8.73 6.37 8.73 8.73
Fuel system p 1.00 1.00 1.00 1.00 1.00 1.00 Tables S5e7
Copper kg e 3.94 3.94 1.97 1.97 3.94 3.94
Polyvinylchloride kg e 0.92 0.92 0.46 0.46 0.92 0.92
Reinforcing steel kg e e e e e e 1.45
Gasoline tank p e e e e e e 1.00 Table S8
Polyethylene, HDPE kg e e e e e e 17.5
Injection moulding kg e e e e e e 17.5
Tank CNG-II kg e e e 80.00 80.00 80.00 e Tables S9e10
Steel, low-alloyed kg e e e 70.00 70.00 70.00 e
Epoxy resin, liquid kg e e e 6.00 6.00 6.00 e
Glass fibre kg e e e 4.00 4.00 4.00 e
Hydrogen tank (CNG-IV) kg 93.00 93.00 93.00 e e e 18.60 Tables S11e12
Exhaust system p e 1.00 1.00 1.00 1.00 1.00 1.00 Tables S13e20
Reinforcing steel kg e 34.90 34.90 34.90 34.90 34.90 34.90
Synthetic rubber kg e 1.45 1.45 1.45 1.45 1.45 1.45
Talc kg e 1.40 1.40 1.40 1.40 1.40 1.40
Steel, low-alloyed kg e 25.20 25.20 25.20 25.20 25.20 25.20
Platinum g e 1.40 1.40 2.00 2.00 1.40 1.12 [71e76]
Palladium g e 0.70 0.70 1.00 1.00 0.70 0.42 [71e76]
Rhodium g e 0.64 0.64 0.40 0.40 0.64 0.48 [71e76]
Cerium concentrate, kg e 0.04 0.04 0.04 0.04 0.04 0.04
60% cerium oxide
Zirconium oxide kg e 0.14 0.14 0.14 0.14 0.14 0.14
Aluminium oxide kg e 0.02 0.02 0.02 0.02 0.02 0.02
Polyphenylene kg e 0.10 0.10 0.10 0.10 0.10 0.10
sulphide
Li-ion battery kWh 1.80 e 1.80 e 1.80 e e [30,31]
Electric motor kW 80.00 e 48.60 e 48.60 e e Tables S21e22
Power control unit kg 33.30 e 33.30 e 33.30 e e [27,28,30,35]
Balance of plant kg 55.00 e e e e e e Table S23
Gearbox kg 80.00 80.00 80.00 80.00 80.00 80.00 80.00 Table S24
Starting system p e 1.00 1.00 1.00 1.00 1.00 1.00 Tables S25e27
Cooling system ICE kg e 29.10 29.10 29.10 29.10 29.10 29.10 Table S28
Electronics for control kg 1.30 1.30 1.30 1.30 1.30 1.30 1.30 Table S29
units
Tyres p 4.00 4.00 4.00 4.00 4.00 4.00 4.00 Table S30
Natural gas MJ 1933 1933 1933 1933 1933 1933 1933 [29,69]
Electricity kWh 691 691 691 691 691 691 691 [29,69]

Concerning the inventory of the H2-Gasoline vehicle, the vehicle also presents a gasoline fuel system consisting of a
main difference compared to a gasoline vehicle lies in the plastic gasoline tank, fuel pump, tubes, and gasoline injectors.
presence of a composite material cylinder at 700 bar (type-IV Regarding the operational parameters of the vehicles, fuel
tank) and of small volume (1 kg H2, 25-litre tank) for pure economy (i.e., the reciprocal of consumption) and emission
hydrogen storage. This greatly simplifies the hydrogen storage data were collected. Table 4 presents the fuel economy and
issues because of the small amount of hydrogen required. tailpipe emission values for each of the seven vehicles under
Other differences with respect to conventional gasoline ve- analysis. Information about direct emissions was retrieved
hicles refer to minor engine modifications (gaskets, reinforced from commercial vehicles similar to the chosen reference
valve seats, etc.), TWC with lower load of noble metals (linked vehicle, using data declared by the manufacturers, technical
to combustion improvements), and a hydrogen supply system datasheets and the Ecoscore database [68,86,87]. For non-
(filler neck, valves, special pipes, systems to prevent backfire, commercial hydrogen vehicles (H2-ICE and HEV H2-ICE) and
pressure reducer, injectors, gaskets, etc.). In addition to the mixed concepts (Hythane and H2-Gasoline), data were
dedicated hydrogen fuel distribution system, the H2-Gasoline collected from the GREET model or based on specific literature,
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maintenance than FCEV. These amounts were retrieved from


Table 4 e Fuel economy and tailpipe emissions for the
GREET.
vehicles under study.
The life-cycle models presented in Tables 3 and 5 were
Vehicle Fuel CO2 CO HC NOx
implemented in SimaPro using ecoinvent as the data source
economy [g/km] [g/km] [g/km] [g/km]
for background processes. The environmental characterisa-
[km/kg]
tion was carried out by taking into account the selected life-
FCEVa 131.58 e e e e
cycle indicators and impact assessment methods.
H2-ICEb 59.239 e 0.05851 0.0082 0.0205
HEV H2-ICEb 78.985 e 0.05851 0.0082 0.0172
CNG 28.571c 94.000c 0.04825c 0.0294d 0.0168d
HEV CNGe 43.290 66.888 0.03233 0.0201 0.0049 Results and discussion
Hythanef 34.382 75.670 0.02779 0.0194 0.0269
H2-Gasolineg 31.352 87.146 0.10227 0.0258 0.0337 The inventories previously presented constitute a key
a
Based on [26]. outcome of this article. Furthermore, these inventories were
b
Based on [70]. all implemented in SimaPro for the subsequent LCIA compu-
c
Based on [86]. tation. In this regard, Table 6 presents the life-cycle profile
d
Based on [88,89].
e
calculated for each vehicle system (carbon, non-renewable
Calculated from CNG according to hybridisation factor, and
energy and acidification footprints per one kilometre trav-
contrasted with [70].
f
Own calculation with amounts based on [90,91]. elled). Under GWP and CED criteria, the most favourable
g
Own calculation based on [92e96]. environmental performance was found for HEV H2-ICE, H2-
ICE, and FCEV. Hythane and H2-Gasoline show an interme-
diate performance between CNG and HEV CNG. Under the AP
following the principle of similarity to the reference vehicle. indicator, Hythane arose as the best option, followed by CNG
Values for fuel consumption refer to NEDC (New European and HEV CNG, whereas H2-Gasoline and FCEV show the
Driving Cycle) under a combined cycle (urban/extra-urban highest values. HEV H2-ICE and H2-ICE rank in an interme-
route). diate performance. These findings indicate that the identifi-
Regarding H2-ICE and HEV H2-ICE, data about fuel con- cation of the best vehicle option, from an environmental point
sumption and emissions were taken from GREET [70]. It of view, ultimately depends on the impact categories to be
should be noted that these values correspond with a conser- prioritised.
vative approach, especially those of CO emissions. In fact, in a Fig. 3 shows the comparison of the pure-hydrogen alter-
hydrogen engine, the fuel is carbon-free, and the only carbon natives with CNG and HEV CNG, using CNG as the benchmark.
source is the lubricating oil, which can partially burn in small This figure also shows the main sources of potential impact. In
quantities [38,39,97]. While ein H2-ICE and HEV H2-ICE vehi- this regard, tank-to-wheels (TTW) and well-to-tank (WTT)
clese CO, HC and particulate matter emissions are associated contributions refer to vehicle operation (tailpipe emissions)
with the partial combustion of lubricating oil, in the remain- and fuel production and distribution, respectively. Infra-
ing vehicles using CNG or gasoline these emissions are asso- structure contribution refers to vehicle manufacturing, while
ciated with both lubricating oil and fuel combustion. use and maintenance contribution includes the consumption
Concerning the CNG vehicle, fuel consumption, CO2 and of lubricating oil, spare parts and other consumables as well
CO emissions were collected from commercial vehicles. HC as wear emissions. Additional data about each contribution
and NOx values for CNG refer to both commercial vehicles and expressed as absolute impacts are provided in Supplementary
real driving emissions (RDE) tests [88,89]. Emissions and con- Information (Tables S33eS35 and Figs. S1eS3).
sumption for CNG HEV were calculated proportionally to CNG Regarding GWP and CED, all vehicles fuelled only with
by assuming the same proportion as between a gasoline hydrogen show the best performance, while an unfavourable
vehicle and a gasoline HEV. performance was identified for the CNG car. HEV CNG shows
Fuel consumption and emissions values for Hythane and an intermediate performance between CNG and hydrogen
H2-Gasoline vehicles were based on literature about experi- vehicles. The situation was found to be different in terms of
mental tests and measures [92e96], according to the hydrogen AP, for which the fuel cell vehicle arose as the worst option
percentage under examination. The values considered for due to vehicle infrastructure. The major contributors were
these two vehicles correspond to a conservative approach and found to be the steel-based car frame (vehicle body and
therefore present room for improvement through engine chassis), carbon fibre for the hydrogen tank, battery and
optimisation. components of the vehicle's electrical system and, to a lesser
Finally, Table 5 shows the main inventory data for vehicle extent, platinum group metals and other components of the
operation and maintenance. Tailpipe emissions and fuel stack.
consumption were derived from the values in Table 4. The Concerning vehicle infrastructure, the fuel cell vehicle is
particulate emissions generated by the abrasion of tyres, road outperformed in all impact categories (especially AP) by ve-
and brakes were calculated in proportion to the weight of each hicles with an internal combustion engine, which is closely
vehicle. Regarding maintenance, one battery change and linked to the lower construction complexity of the latter. In
three tyres replacements were considered over the vehicle any case, the platinum group metals present in the catalytic
useful life. Periodic lubricating oil and antifreeze re- converters of ICE vehicles, together with steel for vehicle body
placements were also considered. All vehicles equipped with and engine and the electrical system for HEVs, provide a sig-
ICE require a larger amount of lubricating oil for their routine nificant contribution to AP.
35968 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 5 9 6 1 e3 5 9 7 3

Table 5 e Main inventory data for vehicle operation and maintenance (values per total kilometres travelled).
Item Unit FCEV H2-ICE HEV H2-ICE CNG HEV CNG Hythane H2- Gasoline Ref. for
inventory
Operational inputs
Vehicle infrastructure p 1.00 1.00 1.00 1.00 1.00 1.00 1.00 Table 3
Hydrogen fuel t 1.44 5.06 3.80 e e 0.28 0.27 [16]
Natural gas GJ e e e 534.00 353.00 430.00 e [69]
Gasoline (unleaded) t e e e e e e 9.30 [69]
Maintenance inputs
Lubricating oil kg 3.560 34.60 34.60 34.60 34.60 34.60 34.60 [69,70]
Ethylene glycol kg 12.90 12.90 12.90 12.90 12.90 12.90 12.90 [69,70]
Decarbonised water kg 8.58 8.58 8.58 8.58 8.58 8.58 8.58 [69,70]
Tyres p 12.00 12.00 12.00 12.00 12.00 12.00 12.00 [70,82]
Li-ion battery kWh 1.80 e 1.80 e 1.80 e e [30,31]
Emissions
Carbon dioxide t e e 30.10 21.40 24.20 26.10 Table 4
Carbon monoxide kg e 17.60 17.60 15.40 10.30 8.89 30.70 Table 4
Hydrocarbons, unspecified kg e 2.47 2.47 9.41 6.43 6.21 7.73 Table 4
Nitrogen oxides kg e 6.15 5.17 5.38 1.57 8.60 10.10 Table 4
Brake wear emissions g 304.00 368.00 414.00 379.00 422.00 393.00 356.00 [69]
Road wear emissions kg 3.35 4.05 4.55 4.17 4.64 4.32 3.92 [69]
Tyre wear emissions kg 19.60 23.70 26.60 24.40 27.10 25.30 22.9 [69]
Kilometres travelled km 190,000 300,000 300,000 320,000 320,000 320,000 300,000 e

Regarding WTT impacts, the FCEV arose as the best option


Table 6 e Life-cycle profile of each vehicle system (values
under GWP and CED indicators. This is closely related to the
per FU).
excellent fuel economy of this vehicle as well as to the choice
GWP [kg CO2 CED AP [kg SO2
of hydrogen produced through WPE. Under AP, the best value
eq$km1] [MJ$km1] eq$km1]
was found for HEV CNG.
FCEV 5.601$102 9.913$101 5.332$104 As regards TTW impacts, hydrogen vehicles were found to
H2-ICE 4.343$102 7.450$101 3.618$104
be the best option under GWP. No tailpipe greenhouse gas
HEV H2-ICE 4.103$102 7.227$101 3.500$104
CNG 1.317$101 2.367 2.161$104
emissions are associated with FCEV, while H2-ICE and HEV
HEV CNG 1.004$101 1.734 2.229$104 H2-ICE involve negligible values (related to non-CO2 emis-
Hythane 1.106$101 1.996 2.113$104 sions). In the HEV CNG and CNG vehicles, the use of a fossil
H2-Gasoline 1.301$101 2.211 4.019$104 fuel (natural gas) has a great influence on TTW impacts due to

Fig. 3 e Relative environmental impacts of the three pure-hydrogen vehicle systems and the two CNG systems.
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 5 9 6 1 e3 5 9 7 3 35969

CO2 emissions. Under AP, the best TTW option is the FCEV it is consumed in reduced quantities in mixture vehicles but in
(with no impact), followed by HEV CNG, CNG, HEV H2-ICE and high quantities in the FCEV. Gasoline has an intermediate AP
H2-ICE. Nevertheless, it should be noted that ein all vehiclese value and natural gas has the lowest value. On the other hand,
the TTW-related AP (closely related to NOx emissions) is very vehicle fuel consumption must be considered. The balance
low. between these two terms determines the WTT impact. In this
Concerning use and maintenance contribution, in all cases, sense, in the comparison between hythane and FCEV, the
it has a minor influence on the results. Under all categories, reduced fuel consumption of the latter fails to counterbalance
the best option is given by the CNG vehicle, followed by HEV the reduced fuel-related AP value of the former. The situation
CNG, HEV H2-ICE and H2-ICE, while the FCEV shows a rela- is opposite for the H2-Gasoline vehicle.
tively unfavourable performance. This is mainly related to Regarding use and maintenance, Hythane outperforms
differences in the lifespan of the vehicles under study. H2-Gasoline under all the categories. It should be noted that,
In order to closely explore the environmental performance due to the reduction in the formation of carbon particle de-
of vehicles that involve the use of hydrogen (pure or blended), posits in the combustion chamber, natural gas vehicles have
Fig. 4 additionally shows the relative impacts of the Hythane a greater lifespan than gasoline vehicles. The same could be
and H2-Gasoline vehicle systems with respect to the FCEV applied to vehicles with hydrogen engines; however, a con-
values. servative approach was preferred due to lower technological
Under the set of environmental indicators assessed, due to maturity.
the use of natural gas instead of gasoline, the hythane vehicle Overall, the outcomes of the present work expand the
shows a better performance than the H2-Gasoline vehicle. knowledge in the field of hydrogen vehicles by filling the
However, hydrogen-mixture vehicles were found to perform literature gap in LCA of hythane, hydrogen-gasoline and
significantly worse than FCEV under GWP and CED (due to the hydrogen hybrid electric vehicles. Concerning the life-cycle
involvement of a fossil fuel), unlike under AP (due to the lower performance of the other vehicles addressed in this work,
construction complexity). the findings were found to be in agreement with the recent
Hythane and H2-Gasoline show high TTW-related impacts literature. In particular, the LCA of the FCEV option concurs
in terms of GWP, which is linked to fossil-based CO2 emis- with the study of Evangelisti et al. [28] regarding the main
sions. In fact, concerning TTW performance, the FCEV contributions to carbon, acidification and energy footprints, as
advantage of having no harmful emissions was noticeable well as with Benitez et al. [98] and Miotti et al. [99] under the
only under the GWP category, in contrast to a minor effect on carbon footprint indicator. Finally, regarding the remaining
AP. vehicles, a contextualisation of the results with other authors'
Regarding WTT impacts, FCEV is a better option than findings was possible only in terms of carbon footprint.
Hythane and H2-Gasoline under GWP and CED, which is Despite case-specific differences in scope, the life-cycle im-
linked to its low fuel consumption and the consideration of pacts of CNG, HEV CNG, and H2-ICE vehicles were found to be
renewable hydrogen (produced through WPE). Under AP, the generally in line with the studies of Dai et al. [34], Bauer et al.
hythane vehicle shows a better WTT performance than FCEV, [100], and Desantes et al. [101].
while H2-Gasoline involves the worst performance of all ve-
hicles. This is linked to the acidification footprints of the three
fuels. Hydrogen from WPE has a relatively high AP value, and Conclusions

This comparative LCA study on vehicle systems shows that


hydrogen vehicles are excellent decarbonisation solutions
when fuelled using renewable hydrogen. In particular, albeit
hybrid hydrogen cars with an internal combustion engine
(HEV H2-ICE) require a larger amount of hydrogen with
respect to fuel cell electric vehicles (FCEV), they were found to
involve a better life-cycle environmental performance under
the three indicators considered (carbon, energy and acidifi-
cation footprints). A favourable environmental profile was
also found for the option using hydrogen as the sole fuel in an
internal combustion engine (H2-ICE), but the higher hydrogen
consumption than its hybrid version makes its life-cycle
performance slightly worse. This situation is due to the
lower lifespan of the FCEV compared to other vehicles.
Nevertheless, technological advances in fuel cell (membrane)
durability could overturn this situation. Furthermore, in order
to attain a reduction in the infrastructure impact of the FCEV,
actions are needed on technical factors such as reduction in
vehicle weight, use of steel (for the vehicle body) produced
with new environmentally-friendly techniques, alternative
Fig. 4 e Hythane and H2-Gasoline life-cycle impacts storage system solutions (in particular regarding the carbon
relative to FCEV. fibre of the tank) and alternative battery options.
35970 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 5 9 6 1 e3 5 9 7 3

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