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Assessing Uncertainties of Well-To-Tank Greenhouse Gas Emissions from

Hydrogen Supply Chains

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DOI: 10.3390/su9071101

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 sustainability

Article
Assessing Uncertainties of Well-To-Tank Greenhouse
Gas Emissions from Hydrogen Supply Chains
Akito Ozawa 1 , Mai Inoue 2 , Naomi Kitagawa 1 , Ryoji Muramatsu 1 , Yurie Anzai 1 ,
Yutaka Genchi 1 and Yuki Kudoh 1, *
1 Research Institute of Science for Safety and Sustainability, National Institute of Advanced Industrial Science
and Technology (AIST), 16-1 Onogawa, Tsukuba, Ibaraki 305-8569, Japan; [email protected] (A.O.);
[email protected] (N.K.); [email protected] (R.M.); [email protected] (Y.A.);
[email protected] (Y.G.)
2 Leave a Nest Co., Ltd., Tokyo Head Office Institute of Innovation & Knowledge (I2K), 4F/5F
Iidabashi-Miyuki Bldg 1-4 Shimomiyabi-cho, Shinjuku-ku, Tokyo 162-0822, Japan; [email protected]
* Correspondence: [email protected]; Tel.: +81-29-861-8032

Received: 31 May 2017; Accepted: 21 June 2017; Published: 23 June 2017

Abstract: Hydrogen is a promising energy carrier in the clean energy systems currently being
developed. However, its effectiveness in mitigating greenhouse gas (GHG) emissions requires
conducting a lifecycle analysis of the process by which hydrogen is produced and supplied. This
study focuses on the hydrogen for the transport sector, in particular renewable hydrogen that is
produced from wind- or solar PV-powered electrolysis. A life cycle inventory analysis is conducted to
evaluate the Well-to-Tank (WtT) GHG emissions from various renewable hydrogen supply chains. The
stages of the supply chains include hydrogen being produced overseas, converted into a transportable
hydrogen carrier (liquid hydrogen or methylcyclohexane), imported to Japan by sea, distributed to
hydrogen filling stations, restored from the hydrogen carrier to hydrogen and filled into fuel cell
vehicles. For comparison, an analysis is also carried out with hydrogen produced by steam reforming
of natural gas. Foreground data related to the hydrogen supply chains are collected by literature
surveys and the Japanese life cycle inventory database is used as the background data. The analysis
results indicate that some of renewable hydrogen supply chains using liquid hydrogen exhibited
significantly lower WtT GHG emissions than those of a supply chain of hydrogen produced by
reforming of natural gas. A significant piece of the work is to consider the impacts of variations in
the energy and material inputs by performing a probabilistic uncertainty analysis. This suggests that
the production of renewable hydrogen, its liquefaction, the dehydrogenation of methylcyclohexane
and the compression of hydrogen at the filling station are the GHG-intensive stages in the target
supply chains.

Keywords: hydrogen; supply chain; hydrogen carrier; life cycle inventory analysis; GHG emissions;
probabilistic uncertainty analysis

1. Introduction
Hydrogen has been attracting attention as a clean energy source in part because of its flexibility as
an energy carrier; it can be produced from a variety of industrial processes and consumed by a variety
of end-users. For example, hydrogen can be produced from hydrocarbon feedstocks via chemical
processes (e.g., steam reforming of natural gas (NG) and coal gasification), and by using electricity to
power the electroylysis of water [1,2]. “Renewable hydrogen” is produced using renewable energy
or electricity sources and can usually be expected to decrease the greenhouse gas (GHG) emissions
associated with its use [3,4]. At the other end of the supply chain, hydrogen can be consumed by
diverse end-use applications as it can be transformed into kinetic, electric and thermal energy [3,4].

Sustainability 2017, 9, 1101; doi:10.3390/su9071101 www.mdpi.com/journal/sustainability

Sustainability 2017, 9, 1101 2 of 26

In the transportation sector, for example, hydrogen fuel cell vehicles (FCVs) have received attention
globally as one of the next-generation clean vehicles that major motor companies are developing
and releasing in the passenger car market [5–7]. Other types of FCVs, such as forklifts [8–10] and
buses [11–13], have also been commercialized. Regarding residential energy applications, micro fuel
cell combined heat and power (FC-CHP) systems could decrease household energy use owing to
their high gross energy efficiencies (the sum of power generation efficiency and heat production
efficiency) [14]. Megawatt-class hydrogen energy systems have also been installed around the world
in data centers, hotels and many other commercial facilities to combine distributed renewable energy
resources—such as solar photovoltaics (PV) and wind turbines—and measures to ensure a stable energy
supply—such as battery storage, and water electrolyzers, storage tanks and fuel cells for hydrogen
production, storage and use, respectively [15–18]. In terms of power generation, a commercially
operated 12 MW hydrogen turbine began operating in Italy in 2009 [19,20].
Given this flexibility, hydrogen is regarded as useful for increasing energy diversity and mitigating
GHG emissions in Japan. To support future increases in its supply and demand, various technologies
related to the production, transport and storage of hydrogen are being developed in Japan [21]. Liquid
hydrogen (LH2 ) and methylcyclohexane (MCH) are promising hydrogen carriers that are suitable for
long-term storage and long-distance transport owing to their relative ease of handling [22]. LH2 and
MCH have therefore been considered for a private-sector-led national demonstration project focusing
on an international hydrogen supply chain that transports hydrogen produced from renewable or
excess energy to Japan [23–25].
In parallel with research and development (R&D) surrounding hydrogen technologies, designing
the future hydrogen economy requires understanding the potential socio-economic and environmental
properties of the hydrogen supply chain. A common approach to help decision makers with the
design and development of products and processes is to evaluate their environmental influences
throughout their life cycle [26]. Many studies have been published that report life cycle approaches
to the hydrogen production process. For example, life cycle inventory (LCI) analyses have been
published that calculate the life cycle GHG emissions for hydrogen produced from steam reforming
of NG [27–32], coal gasification [29,31,32], and renewably powered electrolysis of water [30–33].
Specifically, Kato [34] took an economic approach and estimated the final cost in Japan of hydrogen
produced in South Australia, Norway and the Middle East. Meanwhile, other studies have conducted
life cycle sustainability assessments to simultaneously evaluate the economic, social and environmental
impacts [35–37].
A number of LCI studies have also been published that compare the environmental benefits of
using hydrogen instead of conventional energy sources. Examples of such comparative studies in the
automotive sector using Well-to-Wheel (WtW) and Well-to-Tank (WtT) frameworks to estimate GHG
emissions have been carried out for Japan, the US and Europe [38–42]. Regarding the use of hydrogen
in local energy systems, Usui and Hondo [43] compared the life cycle CO2 emissions from electricity
storage systems for distributed wind power, including hydrogen storage using LH2 and MCH that
was then used in FC-CHP. Mori et al. [44] compared the life cycle environmental emissions from a
renewable hydrogen-powered uninterruptible power system (UPS) and a UPS powered by an internal
combustion engine. However, it should be noted that most of these LCI studies were conducted based
on specific assumptions and the mere use or the combinations of the results in previous studies does
not make sense due to the differences of methodologies, system boundaries and databases used in each
analysis. These Japanese studies were also conducted under the energy supply and demand structure
during the first decade of the 21st century. After the Great East Japan earthquake occurred in 2011, our
energy supply structure has drastically changed so that the LCI results should be different if conducted
under the current energy supply. As far as the authors recognize, the WtW study conducted by Mizuho
Information & Research Institute [45] was the only study that assessed the life cycle GHG profiles of
various hydrogen supply chain under the current energy supply but most of the data used for the
assessment are not provided in their report. In the same manner as the EU’s CertifHy project [46], LCI
Sustainability 2017, 9, 1101 3 of 26

analysis should be conducted to understand the environmental profile of the potential international
hydrogen supply chain and extract the technical issues related to hydrogen carrier to make the supply
chain low-carbon.
Using LCI analysis as a decision-making tool requires considering the range of possible
consequences of a given technological pathway [47]. Once the pathway is identified, remaining
uncertainty in the LCI is usually attributed to the use of inaccurate or unrepresentative data [48,49].
One method of mitigating these uncertainties is to conduct sensitivity analyses. The ISO 14044
guidelines suggest that sensitivity analyses should include a wide range of factors to determine
the influence of variation in assumptions, methods and data [50]. An alternative option, uncertainty
analysis, employs probabilistic simulations based on the Monte Carlo method to evaluate the combined
influence of multiple uncertain factors on the results. Here, probability distributions are assumed
for the system’s input parameters. Repeated calculations with different input values then yield a
probability frequency distribution of total GHG emissions from the whole system [49]. The application
of uncertainty analysis using Monte Carlo simulation and LCI has been demonstrated for WtW
emissions [41].
As awareness of unintended and unwanted side-effects has increased, it has become common
practice during the early stages of new technology development to carry out ex ante assessments of
potential consequences that the widespread implementation of the new technologies may create [51,52].
Most components in the hydrogen supply chain are immature and still developing, which creates
uncertainties regarding their real-world performance and could affect the supply chain’s total GHG
emissions. These uncertainties have not be fully considered in previous Japanese WtW studies [38–40]
and addressing this knowledge gap is a key focus of this study.
Foreground inventory data related to the hydrogen supply chains are collected by literature
surveys, and the Japanese life cycle inventory database is used as the background data of the analysis.
A probabilistic uncertainty analysis of the LCI results is then conducted and the results used to
highlight GHG hotspots in the supply chain to promote a discussion of the technical opportunities
available for reducing GHG emissions across the different supply chains.

2. Methods and Assumptions

2.1. Overview
Figure 1 shows the processes that are within the study’s system boundary. The renewable
hydrogen supply chain comprises domestic and overseas stages. The overseas stages are: the
generation of renewable power; the production of renewable hydrogen by water electrolysis; the
production and storage of the hydrogen carrier (LH2 or MCH); and the ocean transport of the hydrogen
carrier to Japan. The domestic stages comprise: the storage of the hydrogen carrier and its distribution
to hydrogen filling stations by tank truck; the release of hydrogen from the energy carrier (restoration)
followed by its compression; and finally the filling of FCVs with hydrogen. A reference supply chain
of hydrogen produced domestically from the steam reforming of natural gas (NG) was also analyzed.
This supply chain comprises: the overseas extraction and liquefaction of NG; the ocean transport of
liquefied natural gas (LNG) to Japan; the production of hydrogen by steam reforming of NG which is
obtained by LNG regasification; the compression and distribution of hydrogen as compressed gaseous
hydrogen (CGH2 ) to hydrogen filling stations by tank truck; and finally the compression and filling of
FCVs stages.
According to Kato [34], Australia and Norway both have the potential to supply large amounts
of low-cost hydrogen using wind power. In Australia, solar PV is also a potential power source for
hydrogen production and the feasibilities of exporting solar PV-generated hydrogen from Australia to
Japan have been investigated [53,54]. For these reasons, Australia and Norway were chosen as the
renewable hydrogen producing countries in this study. The one-way transport distance to Japan was
set as 10,000 km from Australia and 20,000 km from Norway.
potential to significantly decrease GHG emissions from Australian renewable hydrogen supply
chain.
Inventory data were collected from previous WtW and LCI studies on hydrogen supply chains.
Where more than two process options were found (owing to differences in equipment specifications),
the mean and standard deviation were also calculated. The Japanese Inventory Database
Sustainability 2017, 9, 1101
for
4 of 26
Environmental Analysis (IDEA) ver. 2.0 [55] was used as the background data.

Figure 1. Process flow charts showing stages within

within the
the life
life cycle
cycle inventory
inventory (LCI)
(LCI) system
system boundary.
boundary.

Table
Table 1 shows the case settings 1. The base
configured forand low-carbon
hydrogen cases.
from Australia. It was typically assumed
that the electricity
Case used in overseas processes other than hydrogen
Description production was supplied using the
country’s standard electricity grid (referred to as “base case” hereafter). Electricity from the Australian
Electricity for hydrogen production via water electrolysis was supplied
grid has a high GHG emissions intensity owing to the grid’s strong dependency on coal-fired power
BaseThus,
generation. Case the usewith renewable electricity,
of low-carbon electricity,while the electricity
as investigated used
in the in the othercase” where
“low-carbon
all electricity inputs wereAustralian
from theprocesses was supplied
same low-carbon by Australian
source, grid electricity.
was investigated for its potential to
significantly decrease GHGElectricity used
emissions in
from all the Australian
Australian processes
renewable was
hydrogen supplied
supply with the
chain.
Low-Carbon Case
same renewable electricity as water electrolysis.
Table 1. The base and low-carbon cases.
2.2. GHG Emissions Calculation Using IDEA
Case Description
GHG emissions were defined as the sum of the 100-year CO2-equivalent global warming
Electricity for hydrogen production via water electrolysis was supplied with renewable
potentials of emitted CO 2, CH4, N2O, HFCs, PHCs and SF6 [56].
Base Case electricity, while the electricity used in the other Australian processes was supplied by
The IDEA inventory database
Australian was developed by National Institute of Advanced Industrial
grid electricity.
Science and Technology [55]. Figure 2 illustrates IDEA’s structure, which uses a unit process to relate
Electricity used in all the Australian processes was supplied with the same renewable
Low-Carbon
input Casematerials, energies, and resources) to output flows (products, wastes, emissions to
flows (raw electricity as water electrolysis.
air, water and soil) [57].

Inventory data were collected from previous WtW and LCI studies on hydrogen supply chains.
Where more than two process options were found (owing to differences in equipment specifications),
the mean and standard deviation were also calculated. The Japanese Inventory Database for
Environmental Analysis (IDEA) ver. 2.0 [55] was used as the background data.

2.2. GHG Emissions Calculation Using IDEA

GHG emissions were defined as the sum of the 100-year CO2 -equivalent global warming potentials
of emitted CO2 , CH4 , N2 O, HFCs, PHCs and SF6 [56].
The IDEA inventory database was developed by National Institute of Advanced Industrial Science
and Technology [55]. Figure 2 illustrates IDEA’s structure, which uses a unit process to relate input
flows (raw materials, energies, and resources) to output flows (products, wastes, emissions to air, water
and soil) [57].
Sustainability 2017, 9, 1101 5 of 26
Sustainability 2017, 9, 1101 5 of 24

Figure 2.
Figure 2. Data
Data structure of Inventory
structure of Inventory Database
Database for
for Environmental
Environmental Analysis
Analysis (IDEA)
(IDEA) [57].
[57].

The GHG emissions of a product were calculated using IDEA as follows. First, a matrix (the
The GHG emissions of a product were calculated using IDEA as follows. First, a matrix (the IDEA
IDEA input coefficient table) was configured by tabulating the input flows. Each element of the table
input coefficient table) was configured by tabulating the input flows. Each element of the table (aij )
( ) represented the amount of product required to produce one unit of product . Letting and
represented the amount of product i required to produce one unit of product j. Letting xi and f i be the
be the amount of production and final demand of product , respectively, the supply–demand
amount of production and final demand of product i, respectively, the supply–demand balance for
balance for product could be expressed using Equation (1):
product i could be expressed using Equation (1):
(1)
⋯ Ax + f = x (1)
where  ⋮ ⋱ ⋮ ;  ⋮  ; and ⋮ . 
a11 ⋯· · · a1n
 
x1 f1
 .. .. . ; x =  .. ; and f =  .. .
where A = the
Then,  amount
. . of .. produced
 ( .) was
 obtainedusing . a matrix operation. Here, the inverse
matrix was approximated
an1 · · · ann by the sum of the
xn power series, as
f n shown in Equation (2):
Then, the amount of i produced (xi ) was obtained using a matrix operation. Here, the inverse
⋯ (2)
matrix was approximated by the sum of the power series, as shown in Equation (2):
where denotes the identity matrix.  
By defining as the GHG I − A)−1 f from
x = (emissions = I+ + A2process
theAunit + A3 +for · · ·product
f , the embodied GHG (2)
emissions were then obtained from Equation (3):
where I denotes the n × n identity matrix.
(3)
By defining ei as the GHG emissions from the unit process for product i, the embodied GHG
where
emissions were ⋯ .
then obtained from Equation (3):
IDEA ver. 2.0, released in May 2016, includes inventory data of more than 3800 unit processes.
Because it covers all of the items in the Japan Standard GHG = Ex Commodity Classification, the GHG emissions (3)
of any product produced in Japan in the year 2014 are included in IDEA. However, IDEA’s embodied
where E = (e1 · · data
GHG emissions · en ).are limited to Japanese economic activities and thus require assumptions to
IDEA ver.
approximate the2.0, releasedattributed
emissions in May 2016, includes inventory
to Australian or Norwegian data of more than
economic 3800 unit
activity. processes.
For estimating
Because it covers all of the items in the Japan Standard Commodity Classification,
overseas activity using IDEA, a new matrix ′ was created and used in Equation (2) instead the GHG emissions
of ′
of
wasany product produced
configured from the in Japan
IDEA in the
input year 2014
coefficient are included
table in IDEA.the
by employing However,
following IDEA’s
steps:embodied
GHG emissions data are limited to Japanese economic activities and thus require assumptions to
 All of the elements of ′ were set equal to those in . This assumed that the economic activity
approximate the emissions attributed to Australian or Norwegian economic activity. For estimating
in Australia and Norway was the same as that in Japan. (For example, if the same product is
overseas activity using IDEA, a new matrix A0 was created and used in Equation (2) instead of A A0
produced in Japan and Australia, it requires the same inputs in both countries).
was configured from the IDEA input coefficient table A by employing the following steps:
 The ′ elements for oversea transport of resources were set to zero to ensure that the
• All of the elements
approximated of A0 were
emissions set equal
of a product didto not
those in A. those
include This assumed
generated that
by the economic
overseas activity
transport of
in Australia and
the constituent inputs.Norway was the same as that in Japan. (For example, if the same product is
 produced in Japan and Australia, it requires the same inputs in both countries).
The ′ elements referring to grid electricity in Japan were changed to reflect grid electricity in
• The A0 elements
Australia or Norway. for oversea transport of resources were set to zero to ensure that the
approximated emissions of a product did not include those generated by overseas transport
of the constituent inputs.
Sustainability 2017, 9, 1101 6 of 26

• The A0 elements referring to grid electricity in Japan were changed to reflect grid electricity in
Australia or Norway.

2.3. Renewable Power Generation in Hydrogen-Producing Country

Renewable power plants (wind and solar PV in Australia, and wind in Norway) were assumed to
provide dedicated power to parts of the hydrogen supply chains. This meant that the power plants’ life
cycle GHG emissions (for example, those associated with materials production, construction, transport
and operation) were then used whenever renewable electricity was consumed.
The input data used by Imamura et al. [58,59] were used to calculate life cycle GHG emissions
using IDEA. The assumptions made by Imamura et al. [58,59] were to evaluate the Japanese renewable
power plants. In order to reflect the wind conditions and insolation in hydrogen producing countries,
the Australian and Norwegian load factors for wind and solar PV [34,60] were used in our calculation.
Table 2 shows the specifications of wind and solar PV power plants assumed in this study while Table 3
shows the calculated life cycle GHG emissions of wind and solar PV power generation. The reason for
the large difference in Australian and Norwegian wind power emissions could be attributed to the
GHG emissions intensity divergence in grid electricity of the two countries.

Table 2. Specifications of wind and solar PV power plants used in the model.

Parameter Wind Solar PV

Capacity (MW) 40 10
Load factor (%) 35 18
Auxiliary power ratio (%) 10 3
Amount of electricity generated (MWh/year) 122,640 14,532
Life time (year) 30 30

Table 3. Calculated life cycle GHG emissions for wind and solar PV power generation (g-CO2 eq./kWh).

Hydrogen-Producing Country Wind Solar PV

Australia 15.3 66.4
Norway 10.8 n/a

2.4. Renewable Hydrogen Production by Water Electrolysis

Water electrolysis is a popular method of producing hydrogen which has been known for around
200 years [61]. Hydrogen was assumed to be produced using renewable power via electrolysis using
either polymer electrolyte membranes or alkaline water. The mean electricity input was calculated
as 5.19 kWh/Nm3 -H2 [62–74]. The pure water requirement was set to the theoretical value of 0.804
kg/Nm3 -H2 .

2.5. Hydrogen Energy Carriers

2.5.1. Liquid Hydrogen (LH2 )

Hydrogen liquefaction has long been the preferred method of increasing hydrogen density for
transport as the liquid has approximately one eight-hundredth of the volume of gaseous hydrogen [22].
This preference is despite hydrogen having the second lowest boiling point (−253 ◦ C) after helium
and the large amount of electricity that the process requires. Figure 3 shows the renewable hydrogen
supply chain using LH2 that was modeled in this study. Assumptions for each of the supply chain
components are described below.
Sustainability 2017, 9, 1101 7 of 26
Sustainability 2017, 9, 1101 7 of 24

Figure 3. Renewable hydrogen supply chain using LH2. Only renewable electricity was used for
Figure 3. Renewable hydrogen supply chain using LH2 . Only renewable electricity was used for
hydrogen production (expressed in green font). For electricity inputs for production and storage of
hydrogen production (expressed in green font). For electricity inputs for production and storage of
liquid hydrogen (red font), the base cases assumed the input was equal to grid electricity. However,
liquid hydrogen (red font), the base cases assumed the input was equal to grid electricity. However, for
for
the the Australian
Australian low-carbon
low-carbon cases,
cases, the the same
same renewable
renewable electricity
electricity input
input waswas assumed
assumed as that
as that usedused
for
for hydrogen production.
hydrogen production.

 LH2 production
• LH2 production
LH2 was produced by cooling gaseous hydrogen. The mean electricity input for LH2 production
LH2 was produced
was calculated by cooling
as 0.906 kWh/Nm gaseous
3-H hydrogen. The mean electricity input for LH2 production
2 [65,66,75–78].

was calculated as 0.906 kWh/Nm3 -H2 [65,66,75–78].

 LH2 storage at loading port
• LH22 was
LH storage at loading
stored port insulation tanks at a loading port. It was assumed that the boil-off
in stationary
of hydrogen gas during this stage was subsequently re-liquefied. The electricity input for LH2 storage
LH2 was stored in stationary insulation 3tanks at a loading port. It was assumed that the boil-off
at the loading port was set to 0.055 kWh/Nm -H2 [39].
of hydrogen gas during this stage was subsequently re-liquefied. The electricity input for LH2 storage
at theLH 2 ocean
loading transport
port 0.055 kWh/Nm3 -H2 [39].
was setbytotanker

• A
LHLH 2 tanker (160,000 m tank capacity, 16 knots sailing speed) [66] was assumed for transport
3
2 ocean transport by tanker
of LH2 to Japan. However, because LH2 tankers are still being developed, exact data were not
available.
A LHThus,
2 tanker the(160,000 m3 tank
emissions data capacity,
were estimated
16 knotsusing
sailingdata for LNG
speed) tankers
[66] was in IDEA
assumed under the
for transport of
assumption that the GHG emissions of a LH tanker per transport volume of LH
LH2 to Japan. However, because LH2 tankers are still being developed, exact data were not available.
2 2 expressed in ton-
kilometer
Thus, unit were data
the emissions equalwere
to those for a LNG
estimated usingtanker perLNG
data for ton-kilometer
tankers in of LNG.
IDEA The the
under emissions from
assumption
laden and ballast voyages were both included in the estimation. The mean boil-off
that the GHG emissions of a LH2 tanker per transport volume of LH2 expressed in ton-kilometer unit rate of LH 2 during
the voyage
were equal towas calculated
those as 0.3%/day
for a LNG tanker per [65,66].
ton-kilometer of LNG. The emissions from laden and ballast
voyages
 were both included
LH2 storage at unloading port in the estimation. The mean boil-off rate of LH2 during the voyage was
calculated as 0.3%/day [65,66].
LH2 was assumed to be transferred from the tanker to stationary tanks at an unloading port. It
•
was LH 2 storage
assumed thatat unloading port
the gas resulting from hydrogen boil-off was subsequently re-liquefied. The
electricity input for LH2 storage at the unloading port was set to 0.055 kWh/Nm3-H2 [39].
LH2 was assumed to be transferred from the tanker to stationary tanks at an unloading port.
It was
Domestic
assumed distribution
that the gas of resulting
LH2 by tank fromtruck
hydrogen boil-off was subsequently re-liquefied. The
electricity input for LH storage at the unloading port wasoilsetfuel
to 0.055 kWh/Nm 3 -H [39].
LH2 tank trucks (232 kL tank capacity, 3.5 km/L-diesel economy) [45,79] were
2 assumed to
be responsible for the domestic distribution from the LH2 storage terminal to the hydrogen filling
• Domestic distribution of LH2 by tank truck
stations. The one-way distance was set to 50 km [66], and both the emissions by the laden and empty
journeys were included to the inventory.
LH tank trucks (23 kL tank capacity, 3.5 km/L-diesel oil fuel economy) [45,79] were assumed
2
to beLHresponsible forhydrogen
2 storage at the domestic distribution
filling stations from the LH2 storage terminal to the hydrogen filling
stations. The one-way distance was set to 50 km [66], and both the emissions by the laden and empty
LH2 was assumed to be transferred from tank trucks to stationary tanks at hydrogen filling
journeys were included to the inventory.
stations. The electricity input required for LH2 storage at a filling station was set to 0.055 kWh/Nm3-
H• 2 [39].
LH2 storage at hydrogen filling stations

2.5.2.LH
Methylcyclohexane (MCH)
2 was assumed to be transferred from tank trucks to stationary tanks at hydrogen filling stations.
The electricity input required for LH2 storage at a filling station was set to 0.055 kWh/Nm3 -H2 [39].
MCH (CH3C6H11) is another promising hydrogen carrier. It is produced by the hydrogenation of
toluene (TOL; CH3C6H5) and releases hydrogen via catalytic dehydrogenation:
Sustainability 2017, 9, 1101 8 of 26

2.5.2. Methylcyclohexane (MCH)

MCH (CH3 C6 H11 ) is another promising hydrogen carrier. It is produced by the hydrogenation of
toluene (TOL;
Sustainability 2017,CH 3 C 6 H5 )
9, 1101and releases hydrogen via catalytic dehydrogenation: 8 of 24

CH3 C6 H5 + 3H2
CH3 C6 H11 (4)
CH C H 3H ⇌ CH C H (4)
MCH was wasfirst
firstproposed
proposedasas a hydrogen
a hydrogen storage system
storage systemfor use
for as
usea vehicle fuel infuel
as a vehicle 1980in[80]
1980under
[80]
what
under is now
what known
is now as the
known methylcyclohexane-toluene-hydrogen
as the methylcyclohexane-toluene-hydrogen (MTH)
(MTH)system
system[81,82].
[81,82]. After
hydrogenation
hydrogenation ofofTOL TOL at hydrogen
at the the hydrogen supply
supply site, MCHsite, MCH is by
is transported transported
tanker and by tanker and
dehydrogenated
dehydrogenated
at the demand site at to
theyield
demandH2 andsite the
to yield H2 and
original TOL,the original
which TOL,
is then which istothen
returned returned
the supply toand
site the
supply
reused site
[83].and
Thereused [83]. The dehydrogenation
dehydrogenation of MCH to TOL of MCH to TOL is
is important toimportant
the processto the
owing process
to itsowing
large
to its large endothermic
endothermic heat (205
heat of reaction of reaction (205 kJ/mol-MCH
kJ/mol-MCH = 68.3 kJ/mol-H = 68.32 )kJ/mol-H ) [84]. Aofnumber
[84]. A 2number of
catalysts,
catalysts,
includingincluding
those thatthose that are platinum
are platinum [85–88], [85–88],
palladiumpalladium
[88–90][88–90]
and nickeland nickel
[91,92][91,92]
based,based,
have have
been
been investigated
investigated for their
for their ability
ability to facilitate
to facilitate an efficient
an efficient dehydrogenation
dehydrogenation of MCH.
of MCH. FigureFigure 4 shows
4 shows the
the renewable
renewable hydrogen
hydrogen supply
supply chainchain
usingusing
MCH MCH
thatthat
waswas assumed
assumed in this
in this study.
study.

Figure 4. Renewable
Figure 4. Renewable hydrogen
hydrogen supply
supply chain
chain using
using MCH.
MCH. Only
Only renewable
renewable electricity
electricity was
was used
used for
for
hydrogen
hydrogen production (expressed in green font). For electricity inputs for production and storage of
production (expressed in green font). For electricity inputs for production and storage of
MCH
MCH andand TOL
TOL (red
(redfont),
font),the
thebase
basecases
casesassumed
assumedthetheinput
input
waswas equal
equal to to grid
grid electricity.
electricity. However,
However, for
for
the the Australian
Australian low-carbon
low-carbon cases,
cases, the the same
same renewable
renewable electricity
electricity input
input waswas assumed
assumed as that
as that usedused
for
for hydrogen production.
hydrogen production.

 MCH production
• MCH production
MCH was produced by the chemical reaction between TOL and hydrogen. The reaction yield of
MCH was produced by the chemical reaction between TOL and hydrogen. The reaction
hydrogen addition to TOL and the hydrogen consumption rate were set to 99.8% and 97.9%,
yield of hydrogen addition to TOL and the hydrogen consumption rate were set to 99.8% and
respectively [65]. The mean electricity input for MCH production was calculated as 40.68 kWh/t-
97.9%, respectively [65]. The mean electricity input for MCH production was calculated as
MCH [65,66,93].
40.68 kWh/t-MCH [65,66,93].
 MCH storage at loading port
• MCH storage at loading port
MCH was assumed to be stored in cone roof tanks at an overseas loading port. The mean
MCH was assumed to be stored in cone roof tanks at an overseas loading port. The mean
electricity input for MCH storage at the loading port was calculated as 0.915 kWh/t-MCH [65,66].
electricity input for MCH storage at the loading port was calculated as 0.915 kWh/t-MCH [65,66].
 MCH ocean transport by tanker
• MCH ocean transport by tanker
A chemical tanker was assumed to be used for the ocean transport of MCH to Japan. The
A chemical
associated tanker was
GHG emissions assumed
were to be
calculated usedIDEA’s
using for theemissions
ocean transport
data for aofchemical
MCH totanker.
Japan. The
associated GHG emissions were calculated using IDEA’s emissions data for a chemical tanker.
 MCH storage at unloading port
• MCH storage at unloading port
MCH was assumed to be transferred from the chemical tanker to cone roof tanks at a domestic
MCH port.
unloading was assumed to be transferred
The electricity fromstorage
input for MCH the chemical
at the tanker to cone
unloading portroof
wastanks at a domestic
assumed to be the
unloading port. The electricity input for MCH storage
same as that required for storage at the loading port. at the unloading port was assumed to be the
same as that required for storage at the loading port.
 Domestic distribution of MCH/TOL by tank trucks
Tank trucks (20 kL tank capacity, 2.34 km/L-diesel oil fuel economy) [45,79] were assumed to be
used for the domestic distribution of MCH to and TOL from the hydrogen filling stations. The one-
way distance was set as 50 km [66], and both the emissions associated with the MCH- and TOL-laden
trucks were included in the inventory.
Sustainability 2017, 9, 1101 9 of 26

• Domestic distribution of MCH/TOL by tank trucks

Tank trucks (20 kL tank capacity, 2.34 km/L-diesel oil fuel economy) [45,79] were assumed to be
used for the domestic distribution of MCH to and TOL from the hydrogen filling stations. The one-way
distance was set as 50 km [66], and both the emissions associated with the MCH- and TOL-laden trucks
were included in the inventory.
Sustainability 2017, 9, 1101 9 of 24
• Dehydrogenation of MCH at hydrogen filling stations
 Dehydrogenation of MCH at hydrogen filling stations
At the hydrogen filling stations, MCH was assumed to be converted to hydrogen and TOL by
At the hydrogen filling
the dehydrogenization stations,
reaction. MCH was rate,
The conversion assumed to be converted
selectivity to hydrogen
and hydrogen andreaction
yield of the TOL by
the dehydrogenization
were set to 95.0%, 99.9%reaction. The conversion
and 90.0%, respectivelyrate,
[65].selectivity and hydrogen
It was assumed yield
that heat of the reaction
required by the
dehydrogenization was supplied by combustion of city gas. The mean electricity input for by
were set to 95.0%, 99.9% and 90.0%, respectively [65]. It was assumed that heat required MCHthe
dehydrogenization was supplied by combustion of 3city
dehydrogenization was calculated as 0.310 kWh/Nm -H2 [65,66,93]. gas. The mean electricity input for MCH
dehydrogenization was calculated as 0.310 kWh/Nm3-H2 [65,66,93].
• TOL storage at loading port
 TOL storage at loading port
TOL was assumed to be stored in cone roof tanks at a domestic loading port. The mean electricity
TOL was assumed to be stored in cone roof tanks at a domestic loading port. The mean electricity
input for TOL storage at the loading port was calculated as 0.915 kWh/t-TOL [65,66].
input for TOL storage at the loading port was calculated as 0.915 kWh/t-TOL [65,66].
• TOL ocean transport by tanker
TOL ocean transport by tanker
A
Achemical
chemicaltanker
tankerwas
wasassumed
assumedfor
fortransport
transportof
ofTOL
TOLfrom
fromJapan.
Japan. The
The associated
associated GHG
GHG emissions
emissions
were calculated using IDEA’s emissions data for a chemical tanker.
were calculated using IDEA’s emissions data for a chemical tanker.
• TOL
TOLstorage
storageat
atunloading
unloadingport
port
TOL
TOL was
was assumed
assumed toto be
be transferred
transferred from
from the
the chemical
chemical tanker
tanker to
to cone
cone roof
roof tanks
tanks at
at aadomestic
domestic
unloading
unloading port.
port. The
The electricity
electricity input for
for TOL
TOL storage
storage atat the
the unloading
unloading port
port was
was assumed
assumed to to be
be the
the
same
sameas
asthe
theinput
inputat
atthe
theloading
loadingport.
port.

• TOLreplacement
TOL replacement
Owing to
Owing to unwanted
unwanted sideside chemical
chemical reactions
reactions (including
(including demethylation,
demethylation, isomerization,
isomerization,
cycloreversion and
cycloreversion and dimerization)
dimerization) that
that also
also occur
occur during
during the
the hydrogenation
hydrogenation and
and dehydrogenation
dehydrogenation
stages, a portion of the TOL must be replaced with virgin TOL to maintain the MTH cyclecycle
stages, a portion of the TOL must be replaced with virgin TOL to maintain the MTH efficiency
efficiency [94].
[94]. It was assumed that 3% of the initial TOL-loading was replaced
It was assumed that 3% of the initial TOL-loading was replaced every year. every year.

2.6. Supply
2.6. Supply Chain
Chain for
for Hydrogen
HydrogenProduced
Producedby
byNatural
NaturalGas
Gas(NG)
(NG)Reforming
Reforming
Figure55shows
Figure shows the
the supply
supply chain
chain for hydrogen
hydrogen produced
produced by NG reforming assumed in this study.
IDEA’sGHG
IDEA’s GHGemissions
emissionsassociated
associatedwith
withthe
thecombustion
combustionof ofLNG
LNGwere
wereused
usedto
tocalculate
calculatethe
theemissions
emissions
associatedwith
associated withthe
theproduction
productionof ofNG,
NG,its
its compression
compressiontotoproduce
produceLNG
LNGand
andLNG
LNG transport
transportby
by tanker
tanker
toJapan.
to Japan. Other
Other stages
stages in
in the
the supply
supplychain
chainarearedescribed
describedbelow.
below.

Figure 5.
Figure 5. Supply
Supply chain
chain for
for hydrogen
hydrogen production
productionby
byNG
NGreforming.
reforming.

 Hydrogen production via steam reforming of NG

Gaseous hydrogen was assumed to be produced in Japan by reforming NG derived from
imported LNG. The mean NG and electricity inputs were calculated as 15.04 MJ(LHV)/Nm3-H2 and
0.211 kWh/Nm3-H2, respectively [38,39,95–97]. The process water requirement was set to 1.964 × 10−3
Sustainability 2017, 9, 1101 10 of 26

• Hydrogen production via steam reforming of NG

Gaseous hydrogen was assumed to be produced in Japan by reforming NG derived from

imported LNG. The mean NG and electricity inputs were calculated as 15.04 MJ(LHV)/Nm3 -H2
and 0.211 kWh/Nm3 -H2 , respectively [38,39,95–97]. The process water requirement was set to
1.964 × 10−3 m3 /Nm3 -H2 [68,97].

• Hydrogen compression at production plant

The produced hydrogen was assumed to be compressed to 20 MPa and loaded into gas tank
trucks for distribution. The electricity input for the compression stage at the production plant was set
to 0.272 kWh/Nm3 -H2 [39].

• Domestic distribution of CGH2 by tank trucks

Gas tank trucks were assumed to carry out the domestic distribution of CGH2 . The mean tank
capacity and fuel economy of the trucks were calculated as 2330 Nm3 -H2 and 2.75 km/L-diesel oil,
respectively [40,98]. The one-way distance was set to 50 km [66], and both the emissions associated
with laden and empty trucks were included to the inventory.

2.7. Hydrogen Compression and Filling of FCVs at Hydrogen Filling Stations

At the hydrogen filling stations, hydrogen was assumed to be compressed to a pressure of 70 MPa
before the FCVs were filled. The electricity consumption for the compression and filling activities were
set to 0.282 kWh/Nm3 -H2 and 0.093 kWh/Nm3 -H2 , respectively [39].

2.8. Uncertainty Analysis

A range of parameters (listed in Table A1) were considered as part of the uncertainty analysis
carried out on the WtT GHG emissions resulting from the various hydrogen supply chains.
To determine the probability distribution for each parameter, the WtW analysis methodology adopted
by General Motors et al. [95] was applied. Most parameters were assumed to follow a normal
distribution curve according to the mean and standard deviation values presented in Table A1. Based
on the literature values for inventory data quality, the standard deviation of GHG emissions attributed
to renewable power generation was assumed to be 10% of the mean value [99,100].
As for MCH production, hydrogen production by NG steam reforming and hydrogen compression
at the NG steam reforming plant, electricity input might show negative if a normal distribution was
assumed for the parameters. Hence, in these processes triangle distribution functions using the mean,
minimum and maximum data in the inventory were assumed instead of a normal distribution.
Monte Carlo simulations were performed using Oracle Crystal Ball [101]. A total of 10,000
iterations was used for each simulation to ensure the analysis was reproducible [102].

3. Results and Discussion

3.1. WtT GHG Emissions for Hydrogen Carriers

3.1.1. Liquid Hydrogen (LH2 )

Figure 6 shows the mean WtT GHG emissions from the renewable hydrogen supply chains using
LH2 . The emissions from the NG reforming hydrogen supply chain are also shown for reference.
Except for the Australian solar PV base case, all supply chains that combined LH2 with renewable
power-produced hydrogen showed lower GHG emissions than those from reforming of NG.
further decreasing the carbon-intensity of renewable hydrogen production [106,107]. Meanwhile,
employing domestic renewable energy sources to power the hydrogen compression process at the
filling stations could decrease GHG emissions from this stage.
Regarding
Sustainability 2017, 9,the NG reforming hydrogen supply chain, hydrogen production via steam reforming
1101 11 of 26
of NG was the most GHG-intensive process which account for 60% of the total GHG emissions.

Figure 6. Mean WtT GHG emissions for renewable hydrogen supply chains using LH2 as the
Figure 6. Mean WtT GHG emissions for renewable hydrogen supply chains using LH2 as the
hydrogen carrier.
hydrogen carrier.

3.1.2. Methylcyclohexane (MCH)

In the Australian base cases, cooling hydrogen to produce LH2 was responsible for the largest
Figure
portion 7 shows
of GHG the meanaccounting
emissions, WtT GHG emissions
for 67% and from 56%theof renewable
the totalhydrogen
for the windsupply
andchains
solar that
PV
used MCH as the hydrogen carrier. The associated emissions for hydrogen
supply chains, respectively. This is explained by considering the large electricity consumption of the produced by NG
reformingliquefaction
hydrogen are again also shown
process for to
owing reference.
hydrogen’sAllvery
of thelowWtT GHG
boiling emissions
point (−253 ◦presented
C). Possiblelieoptions
in the
range
for 130–170 electricity
decreasing g-CO2eq./MJ(LHV)-H
consumption which indicates
2 include improving that the GHG
process emissions
efficiency were relatively
by implementing new
insensitive to both where the hydrogen was produced and the renewable
liquefiers [103,104] or combining the liquefaction with a LNG re-gasification process [105]. Alongside power technology
employed. the
decreasing Unlike the large
electricity decreasestheobserved
requirement, associated forGHGhydrogen
emissions supplied
could beusing LH2, the
decreased WtT GHG
by employing
emissions for the low-carbon cases for Australian wind and solar PV power
a low-carbon power source: using wind and solar PV power in Australia rather than grid electricity were only 5% and 4%,
respectively, lower than the emissions in the base
decreased the total GHG emissions by 70% and 55%, respectively. case.
For allGHG
Other cases,hotspots
the dehydrogenation
of the LH2 supply of MCHchainat were
the hydrogen
the originalfilling stationsproduction
hydrogen was responsible
step andfor
the largest portion—approximately half—of the total GHG emissions. Because
hydrogen compression at domestic filling stations. Continued R&D for technologies related to the the dehydrogenation
of MCH is in
components considerably endothermic—and
water electrolysis—such therefore
as electrodes, energy-intensive—the
electrolytes and membranes—is energyimportant
source and in
process decreasing
further efficiency for this
the step have a largeofinfluence
carbon-intensity renewable on hydrogen
the supplyproduction
chain’s overall life cycleMeanwhile,
[106,107]. emissions.
Given that domestic
employing it was assumed
renewable thatenergy
the heat required
sources for the
to power thedehydrogenation
hydrogen compression was obtained
processby the
at the
combustion
filling stations ofcould
city gas, this stage’s
decrease GHG emissions
GHG emissions from this could
stage. be decreased by using waste heat from
nearby plants. For example, if all of this heat could
Regarding the NG reforming hydrogen supply chain, hydrogenbe supplied from waste sources,
production viathe total reforming
steam emissions
of NG was the most GHG-intensive process which account for 60% of the total GHG emissions.lower
for the Australian base cases for wind and solar PV power could be 58 and 48%, respectively,
than when burning city gas. Notably, Cresswell and Metcalfe demonstrated a MCH dehydrogenation
3.1.2.
system Methylcyclohexane
in which the reaction (MCH) heat was supplied by waste heat from a solid oxide fuel cell [108]. R&D
that focuses
Figure 7 shows the meandehydrogenation
on improving the WtT GHG emissions catalystsfrom is also important for
the renewable advancing
hydrogen the process
supply chains
efficiency
that used MCH[109,110]. In this
as the manner,
hydrogen catalysts
carrier. Thethat facilitateemissions
associated the dehydration using low-quality
for hydrogen produced by waste
NG
heat have been reported by Chaouki and Klvana [111] and Hodoshima et al. [112].
reforming are again also shown for reference. All of the WtT GHG emissions presented lie in the range
As with the LH2 process, the GHG emissions attributed to the initial production of renewable
130–170 g-CO2 eq./MJ(LHV)-H2 which indicates that the GHG emissions were relatively insensitive to
hydrogen and the compression of hydrogen at filling stations were also found to have a moderate
both where the hydrogen was produced and the renewable power technology employed. Unlike the
impact on the total. Finally, the two-way long-distance ocean transport (of MTH and TOL) was
large decreases observed for hydrogen supplied using LH2 , the WtT GHG emissions for the low-carbon
cases for Australian wind and solar PV power were only 5% and 4%, respectively, lower than the
emissions in the base case.
Sustainability 2017, 9, 1101 12 of 24

particularly
Sustainability notable
in the Norwegian case where the combined emissions attributed to 12
2017, 9, 1101 ocean
of 26
transport of MTH and TOL accounted for 20% of the total WtT GHG emissions.

Figure 7. Mean WtT GHG emissions from the renewable hydrogen supply chains that use MCH as
Figure 7. Mean WtT GHG emissions from the renewable hydrogen supply chains that use MCH as the
the hydrogen carrier.
hydrogen carrier.

3.2. WtT GHG Emissions Based on Uncertainty Analysis

For all cases, the dehydrogenation of MCH at the hydrogen filling stations was responsible for
Figureportion—approximately
the largest 8 shows the uncertaintyhalf—of
analysisthe
results
total for
GHG theemissions.
WtT GHGBecause
emissionsthefrom renewable and
dehydrogenation of
NG reforming hydrogen supply chains. From the comparison of all
MCH is considerably endothermic—and therefore energy-intensive—the energy source andresults and their variability
process
analyses, for
efficiency it isthis
clear that
step theaGHG
have large emissions
influence on from
the renewable hydrogen
supply chain’s overallusing LH2 emissions.
life cycle as the hydrogen
Given
that it was assumed that the heat required for the dehydrogenation was obtained byfor
carrier are significantly lower than those from hydrogen produced by NG reforming thethe Australia
combustion
low-carbon
of cases
city gas, this and the
stage’s GHG Norway case.could
emissions Conversely, no significant
be decreased decrease
by using waste was
heat observed
from nearby for the
plants.
MCH cases. Nonetheless, with future technical developments, such as those described
For example, if all of this heat could be supplied from waste sources, the total emissions for the in the previous
section, thebase
Australian GHGcases
emissions from
for wind thesolar
and MCHPV process
powerare expected
could be 58to decrease.
and 48%, respectively, lower than
when burning city gas. Notably, Cresswell and Metcalfe demonstrated a MCH dehydrogenation
system in which the reaction heat was supplied by waste heat from a solid oxide fuel cell [108]. R&D
that focuses on improving the dehydrogenation catalysts is also important for advancing the process
efficiency [109,110]. In this manner, catalysts that facilitate the dehydration using low-quality waste
heat have been reported by Chaouki and Klvana [111] and Hodoshima et al. [112].
As with the LH2 process, the GHG emissions attributed to the initial production of renewable
hydrogen and the compression of hydrogen at filling stations were also found to have a moderate
impact on the total. Finally, the two-way long-distance ocean transport (of MTH and TOL) was
particularly notable in the Norwegian case where the combined emissions attributed to ocean transport
of MTH and TOL accounted for 20% of the total WtT GHG emissions.

3.2. WtT GHG Emissions Based on Uncertainty Analysis

Figure 8 shows the uncertainty analysis results for the WtT GHG emissions from renewable
and NG reforming hydrogen supply chains. From the comparison of all results and their variability
analyses, it is clear that the GHG emissions from renewable hydrogen using LH2 as the hydrogen
carrier are significantly lower than those from hydrogen produced by NG reforming for the Australia
low-carbon
Figure 8.cases and theanalysis
Uncertainty Norway case.forConversely,
results no significant
WtT GHG emissions decrease and
from renewable wasNGobserved for the
reforming
MCHhydrogen
cases. Nonetheless, with future technical developments, such as those described in the previous
supply chains. Bar graphs show the mean values; error bars represent the 95% confidence
section, the GHG
interval. emissions
Probability from the
histograms MCH
of the WtTprocess are expected
GHG emissions to decrease.
obtained by Monte Carlo simulation are
shown in Appendix B.
NG reforming hydrogen supply chains. From the comparison of all results and their variability
analyses, it is clear that the GHG emissions from renewable hydrogen using LH2 as the hydrogen
carrier are significantly lower than those from hydrogen produced by NG reforming for the Australia
low-carbon cases and the Norway case. Conversely, no significant decrease was observed for the
MCH cases.
Sustainability Nonetheless,
2017, 9, 1101 with future technical developments, such as those described in the previous
13 of 26
section, the GHG emissions from the MCH process are expected to decrease.

Figure 8. Uncertainty analysis results for WtT GHG emissions from renewable and NG reforming
Figure 8. Uncertainty analysis results for WtT GHG emissions from renewable and NG reforming
hydrogen supply chains. Bar graphs show the mean values; error bars represent the 95% confidence
hydrogen supply chains. Bar graphs show the mean values; error bars represent the 95% confidence
interval. Probability histograms of the WtT GHG emissions obtained by Monte Carlo simulation are
interval. Probability histograms of the WtT GHG emissions obtained by Monte Carlo simulation are
shown in Appendix B.
shown in Appendix B.

4. Conclusions
To better understand the potential role of hydrogen energy in decreasing GHG emissions in Japan,
a WtT LCI analysis was carried out for renewable hydrogen supply chains originating in Australia
and Norway. Wind- or solar PV-powered electrolysis generated hydrogen that was transported to
Japan using a hydrogen carrier (LH2 or MCH), before being distributed to domestic hydrogen filling
stations where the hydrogen was restored and pressurized for FCV applications. Data were drawn
from literature surveys and IDEA, the Japanese life cycle inventory database. A Monte Carlo-based
uncertainty analysis was performed to investigate the impact of variations in the supply chain’s energy
and material inputs. The LCI analyses showed that the initial hydrogen production, its liquefaction to
produce LH2 , the dehydrogenation of MCH and the compression of hydrogen at the filling stations
were particularly GHG-intensive activities in the respective supply chains. A number of technological
options to decrease GHG emissions in these areas were discussed, as summarized in Figure 9. With a
95% confidence interval, renewable hydrogen produced in Australia (low-carbon cases) or Norway and
transported to Japan as LH2 exhibited significantly lower WtT GHG emissions than those calculated
for hydrogen produced by NG reforming. Although the technology options modeled herein suggested
the MCH pathway exhibited similar GHG emissions to those from the NG reforming production
supply chain, the uncertainty analysis results suggested that feasible technical developments could
result in significantly lower emissions from the MCH pathway.
This study mainly focused on the GHG emissions of hydrogen produced from renewable energy
resources. However, other potentially low-carbon supply chains exist, such as hydrogen produced
from gasification of lignite combined with carbon capture and storage (CCS), which shall be evaluated
in future work.
Similarly, we note that extending the LCI analysis to include economic, social and other
environmental impacts as part of multiple criteria analyses will also be increasingly important for the
deliberation of hydrogen’s potential role as an energy medium.
 as summarized in Figure 9. With a 95% confidence interval, renewable hydrogen produced in
Australia (low-carbon cases) or Norway and transported to Japan as LH2 exhibited significantly lower
WtT GHG emissions than those calculated for hydrogen produced by NG reforming. Although the
technology options modeled herein suggested the MCH pathway exhibited similar GHG emissions
to those from the NG reforming production supply chain, the uncertainty analysis results suggested
Sustainability 2017, 9, 1101 14 of 26
that feasible technical developments could result in significantly lower emissions from the MCH
pathway.

Figure 9. GHG hotspots in the hydrogen supply chains, and associated developments that could
Figure 9. GHG hotspots in the hydrogen supply chains, and associated developments that could
decrease GHG emissions.
decrease GHG emissions.

This study mainly focused on the GHG emissions of hydrogen produced from renewable energy
Acknowledgments:
resources. However, Thisother
studypotentially
was supported by “Advancement
low-carbon of Hydrogen
supply chains Technologies
exist, such and Utilization
as hydrogen produced
Project” funded by the New Energy and Industrial Technology Development Organization (NEDO).
from gasification of lignite combined with carbon capture and storage (CCS), which shall be
Author Contributions:
evaluated Akito Ozawa performed the LCI and uncertainty analyses and, together with Mai Inoue,
in future work.
interpreted the results and wrote the manuscript under the supervision of Yuki Kudoh and Yutaka Genchi.
NaomiSimilarly, we note
Kitagawa, Ryoji that extending
Muramatsu the helped
and Yurie Anzai LCI analysis to include
collect inventory data. economic, social and
All authors approved the other
final
environmental
version impacts as part of multiple criteria analyses will also be increasingly important for the
of the manuscript.
deliberation
Conflicts of hydrogen’s
of Interest: potential
The authors role
declare no as an energy
conflicts medium.
of interest.
Acknowledgments: This study was supported by “Advancement of Hydrogen Technologies and Utilization
Abbreviations
Project” funded by the New Energy and Industrial Technology Development Organization (NEDO).
AUS AustraliaAkito Ozawa performed the LCI and uncertainty analyses and, together with Mai Inoue,
Author Contributions:
CGH
interpreted
2 thecompressed
results and gaseous hydrogen
wrote the manuscript under the supervision of Yuki Kudoh and Yutaka Genchi.
FC-CHP
Naomi Kitagawa, fuelRyoji
cell combined heat
Muramatsu and
and power
Yurie unit helped collect inventory data. All authors approved the
Anzai
FCVs
final version of fuel cell vehicles
the manuscript.
GHG greenhouse gas
Conflicts of Interest:
IDEA TheDatabase
Inventory authors declare no conflicts of
for Environmental interest.
Analysis
ISO International Organization for Standardization
LCI life cycle inventory
LHV lower heating value
LH2 liquid hydrogen
LNG liquefied natural gas
MCH methylcyclohexane
MTH methylcyclohexane-toluene-hydrogen
NG natural gas
NOR Norway
PV photovoltaics
R&D research and development
TOL toluene
UPS uninterruptible power system
WtT Well-to-Tank
WtW Well-to-Wheel
Sustainability 2017, 9, 1101 15 of 26

Appendix A

Table A1. The probability distribution function, mean, standard deviation (SD), minimum (min.) and
maximum (max.) values for various uncertainty parameters.

Parameter (Unit) Function Mean SD Min. Max. Reference

GHG emissions for wind power
generation in Australia Normal 15.3 1.53 [34,58–60,99,100]
(g-CO2 eq./kWh)
GHG emissions for solar PV power
generation in Australia Normal 66.4 6.64 [34,58–60,99,100]
(g-CO2 eq./kWh)
GHG emissions for wind power
generation in Norway Normal 10.8 1.08 [34,58–60,99,100]
(g-CO2 eq./kWh)
Electricity input for hydrogen
production via water electrolysis Normal 5.19 0.94 [62–74]
(kWh/Nm3 -H2 )
Electricity input for liquefaction of
gaseous hydrogen to produce LH2 Normal 0.906 0.233 [65,66,75–78]
(kWh/Nm3 -H2 )
LH2 Boil-off rate during ocean transport
Normal 0.3 0.1 [65,66]
(%/day)
Electricity input for MCH production
Triangular 40.68 37.62 7.54 93.30 [65,66,93]
(kWh/t-MCH)
Electricity input for MCH storage at
loading/unloading port Normal 0.915 0.085 [65,66]
(kWh/t-MCH)
Electricity input for MCH
dehydrogenization Normal 0.310 0.047 [65,66,93]
(kWh/Nm3 -H2 )
Electricity input for TOL storage at
Normal 0.915 0.085 [65,66]
loading/unloading port (kWh/t-TOL)
NG input for hydrogen production via
NG steam reforming Normal 15.04 0.24 [95,97]
(MJ(LHV)/Nm3 -H2 )
Electricity input for hydrogen
production via NG steam reforming Triangular 0.211 0.110 0.100 0.323 [95,97]
(kWh/Nm3 -H2 )
Electricity input for hydrogen
compression at NG steam reforming
Triangular 0.272 0.135 0.119 0.440 [39]
hydrogen production plant
(kWh/Nm3 -H2 )
Tank capacity of CGH2 tank trucks
Normal 2,330 130 [40,98]
(Nm3 -H2 )
Fuel economy of CGH2 tank trucks
Normal 2.75 0.25 [40,98]
(km/L-diesel oil)
Sustainability 2017, 9, 1101 16 of 26

Table A2. Electricity input for hydrogen production via water electrolysis; individual values of
inventory data from each literature are shown side by side.

Reference Electricity (kWh/Nm3 -H2 )

Asaoka et al. [62] 4.5 5.1 4.85
Hydrogenics [63,64] 5.4 4.9 6.7
IAE (2010) [65] 6.5 4.3 5.3
IAE (2016) [66] 4.8
Japan Petroleum Energy Center [67] 4.8 5.3 6.5 4.5
Kawasaki Heavy Industries [68] 4.8
Kobelco Eco-Solutions [69] 6.5
4.3 4.6 3.9 4.2 4.6 4.8 4.3
Mitsusima and Matsuzawa [70] 4.3 4.5 4.7 4.4 5.8 6.0 4.5
4.5 3.9 3.7 5.6 5.2
NEDO [71] 4.3 5.3 6.5
NREL [72] 6.3 6.1
Proton On-Site [73,74] 7.3 7.0 6.8 6.2
Mean 5.19
Standard deviation 0.94

Table A3. Electricity input for liquefaction of gaseous hydrogen to produce LH2 ; individual values of
inventory data from each literature are shown side by side.

Reference Electricity (kWh/Nm3 -H2 )

IAE (2010) [65] 1.059 0.958 0.900
IAE (2016) [66] 0.550 0.690
IAE et al. [75] 0.970
JRC [76] 0.900
JHFC [77] 1.259
Kawasaki Heavy Industries [78] 1.079 1.259 0.692 0.555
Mean 0.906
Standard deviation 0.233

Table A4. LH2 boil off rate of liquid hydrogen while ocean transport.

Reference Boil off Rate (%/day)

IAE (2010) [65] 0.4
IAE (2016) [66] 0.2
Mean 0.3
Standard deviation 0.1

Table A5. Electricity input for MCH production.

Reference Electricity (kWh/t-MCH)

IAE (2010) [65] 7.54
IAE (2016) [66] 93.3
Hondo et al. [93] 21.2
Mean 40.68
Standard deviation 37.62
Sustainability 2017, 9, 1101 17 of 26

Table A6. Electricity input for MCH storage at loading/unloading port.

Reference Electricity (kWh/t-MCH)

IAE (2010) [65] 0.83
IAE (2016) [66] 1.00
Mean 0.915
Standard deviation 0.085

Table A7. Electricity input for MCH dehydrogenization.

Reference Electricity (kWh/Nm3 -H2 )

IAE (2010) [65] 0.335
IAE (2016) [66] 0.352
Hondo et al. [93] 0.244
Mean 0.310
Standard deviation 0.047

Table A8. Electricity input for TOL storage at loading/unloading port.

Reference Electricity (kWh/t-MCH)

IAE (2010) [65] 0.83
IAE (2016) [66] 1.00
Mean 0.915
Standard deviation 0.085

Table A9. NG input for hydrogen production via NG steam reforming.

Reference Natural Gas (MJ(LHV)/Nm3 -H2 )

General Moters et al. [95] 15.27
Ramsden et al. [97] 14.80
Mean 15.04
Standard deviation 0.24

Table A10. Electricity input for hydrogen production via NG steam reforming.

Reference Electricity (kWh/Nm3 -H2 )

General Moters et al. [95] 0.323
Ramsden et al. [97] 0.100
Mean 0.211
Standard deviation 0.110

Table A11. Electricity input for hydrogen compression at NG steam reforming hydrogen production
plant; individual values of inventory data from each literature are shown side by side.

Reference Electricity (kWh/Nm3 -H2 )

JHFC (2011) [39] 0.119 0.440
Mean 0.272
Standard deviation 0.135
Sustainability 2017, 9, 1101 18 of 26

Table
Sustainability 2017, 9, 1101 A12. Capacity and fuel economy of CGH2 tank trucks. 17 of 24

Sustainability 2017, 9, 1101 17 of 24

Reference Table A12. Capacity and fuel (Nm
Capacity 3 -H of) CGH2 tank trucks.
economy Fuel Efficiency (km/L-diesel oil)
2

Toyota & Mizuho [40] Table A12. Capacity

Reference Capacityand fuel
(Nm economy
3-H
2460 2) of CGH
Fuel 2 tank trucks.
Efficiency (km/L-diesel3.00
oil)
JPEC [98]
Toyota & Mizuho
Reference [40] 2460 2200
Capacity (Nm -H2)
3 3.00 2.50
Fuel Efficiency (km/L-diesel oil)
Mean 2200 2330 2.75
ToyotaJPEC [98] [40]
& Mizuho 2460 2.50
3.00
Standard deviation
Mean 2330 130 2.75 0.25
JPEC [98] 2200 2.50
Standard deviation
Mean 130
2330 0.25
2.75
Appendix B Standard deviation 130 0.25
Appendix B
Appendix B

Figure A1. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A1. Probability
produced histograms
using wind power in of WtT GHG
Australia (base emissions
case). from hydrogen supply chains for hydrogen
Figure A1. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
produced using wind power in Australia (base case).
produced using wind power in Australia (base case).

Figure A2. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
produced using wind power in Australia (low-carbon case).
Figure A2. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A2. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
produced using wind power in Australia (low-carbon case).
produced using wind power in Australia (low-carbon case).
Sustainability 2017, 9, 1101 19 of 26
Sustainability 2017, 9, 1101 18 of 24
Sustainability 2017, 9, 1101 18 of 24

Figure A3. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A3. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A3.using
produced Probability histograms
solar PV power inofAustralia
WtT GHG emissions
(base case). from hydrogen supply chains for hydrogen
produced using solar PV power in Australia (base case).
produced using solar PV power in Australia (base case).

Figure A4. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A4. Probability histograms
power inof WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A4.using
produced solar PV
Probability histograms Australia
of WtT GHG (low-carbon
emissions case).
from hydrogen supply chains for hydrogen
produced using solar PV power in Australia (low-carbon case).
produced using solar PV power in Australia (low-carbon case).
Sustainability 2017, 9, 1101 20 of 26
Sustainability 2017, 9, 1101 19 of 24
Sustainability 2017, 9, 1101 19 of 24

Figure A5. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A5. Probability histograms of WtT GHG emissions from hydrogen supply chains for hydrogen
Figure A5.using
produced Probability histograms
wind power of WtT GHG emissions from hydrogen supply chains for hydrogen
in Norway.
produced using wind power in Norway.
produced using wind power in Norway.

Figure A6. Probability histogram of WtT GHG emissions for supply chain for hydrogen produced
FigureNG
using A6. Probability histogram of WtT GHG emissions for supply chain for hydrogen produced
Figure A6.reforming.
Probability histogram of WtT GHG emissions for supply chain for hydrogen produced
using NG reforming.
using NG reforming.
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