Available online at www.sciencedirect.
com
ScienceDirect
Mobile hydrogen reformers as a novel approach to
decarbonise the transport sector
John Chiefari and Christian Hornung
As part of a concerted global effort to move towards net
zero greenhouse gas emissions by mid-century, a focus on
moving away from a fossil fuel-based economy is driving
technical developments in decarbonising energy
production. A key platform in a ‘post-fossil fuel’ economy is
hydrogen. The optimism with hydrogen is that it can be
utilised from a number of sources or energy carriers, such
as ammonia or liquid organic hydrogen carriers (LOHC),
which in turn enables a range of specific use cases in
multiple application areas. Reforming hydrogen from
hydrogen carriers requires the use of efficient catalytic
processes and smart reactor engineering. Over recent
years a new generation of 3D printed metallic or ceramic
catalytic reactors has entered the chemical reactor scene,
fundamentally changing how reactors are designed and
catalyst handling is performed. Herein we focus on recent
advances using these reactor systems for hydrogen
reforming in a mobile setting.
Address
CSIRO Manufacturing, Private Bag 10, Clayton South, Victoria 3169,
Australia
Corresponding authors: Chiefari, John (john.chiefari@csiro.au),
Hornung, Christian (christian.hornung@csiro.au)
Current Opinion in Chemical Engineering 2021, 34:100756
This review comes from a themed issue on Reaction engineering and
catalysis: microreactor engineering
Edited by Roland Dittmeyer and Simon Kuhn
For a complete overview see the Issue
Available online 27th October 2021
https://doi.org/10.1016/j.coche.2021.100756
2211-3398/Crown Copyright ã 2021 Published by Elsevier Ltd. All
rights reserved.
Introduction
The transportation sector accounts for approximately 25%
of greenhouse gas emissions and is overwhelmingly
dependant on fossil fuels. Interestingly, emissions in this
sector continue to grow despite more efficient vehicles
and policies being introduced [1]. Since the transporta-
tion sector relies heavily on fossil fuels, it is an important
sector to focus efforts on decarbonisation. However, dec-
arbonising the transport sector will likely require differing
technologies that are fit for purpose across the sector. For
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example, small vehicles such as passenger cars lend
themselves to battery powered electrification as most
uses are for shorter travel with lighter loads. In contrast,
medium and heavy trucking and other forms of heavy
ground transport particularly those driving longer dis-
tance, with heavier loads and/or with longer operating
hours require a different energy solution as batteries
cannot address their needs for fast charging and high-
power demands. In a similar way, aviation and maritime
shipping may also require a different technology solution.
This sector carries heavier loads over longer distances
with little to no refuelling options between (international)
ports.
The diversification of transportation energy sources is a
balancing act with many factors like capital investment,
energy costs, energy consumption. However, alternative
and renewable energy carriers are becoming more viable
and can already be used in certain applications today. The
main alternative energy sources for decarbonising the
transport sector currently being evaluated are sum-
marised in Figure 1.
There is a clear delineation between these five technol-
ogy areas; one is the development of fuels from sustain-
able sources that continue the use of combustion engines
to power transport and the other is the development of
fuels/energy from an alternative power train containing an
electric engine in combination with either a battery or a
fuel cell. Clearly the use of biofuels and e-fuels (or
synthetic fuels), such as fuels derived via the Fischer-
Tropsch synthesis route, is aimed at providing a non-fossil
fuel source to a conventional combustion engine to con-
tinue to utilise all the technical and efficiency improve-
ments to date [2,3]. Importantly, the use of the combus-
tion engine, even with these new sources of fuels, does
still produce typical greenhouse gas emissions, however,
the key differentiator to fossil fuels is that the bio-fuels
and e-fuels are produced sustainably making them theo-
retically carbon neutral. While they offer similar perfor-
mance to petrol and diesel [4], e-fuels are produced using
renewable energy. They are synthesised from CO2 and
hydrogen, meaning the environmental impact is low. To
make the fuel, renewable electricity is used to split water
into oxygen and hydrogen. The e-fuel is then manufac-
tured using this hydrogen and CO2 captured, for example,
from the atmosphere via direct air capture. An important
component for successful widespread uptake of this
technology are primarily the input costs for production,
for example, the cost of CO2 from direct air capture,
Current Opinion in Chemical Engineering 2021, 34:100756
2 Reaction engineering and catalysis: microreactor engineering
Figure 1
Batteries
+ zero emissions - low power to
+ high energy weight ratio
conversion
efficiency
- long charging
time
Hydrogen
+ zero emissions - low energy
+ high energy density
conversion - flammable gas
efficiency
H2 Carriers
+ zero emissions - low energy + liquid fuel
+ liquid fuel conversion
+ existing refuelling efficiency
+ high energy
density
infrastructure
+ non-flammable
- complex conv.
process
+ existing refuelling conversion
infrastructure
(some)
Current Opinion in Chemical Engineering
Alternative energy sources for reducing or eliminating greenhouse gas
emissions in the transport sector.
renewable energy, the electrolyser and associated plant
infrastructure [4–6].
Biofuels can be produced from various types of biomass
via numerous pathways. Biofuels are already widely used
as an alternative energy source in transportation. The
liquid biofuel in greatest production is ethanol. Brazil and
the United States are among the leading producers of bio-
ethanol. In the United States ethanol biofuel is made
primarily from corn (maize) grain, and it is typically
blended with gasoline to produce a fuel that is 10%
ethanol. In Brazil, ethanol biofuel, made primarily from
sugarcane, is commonly used as a 100% ethanol fuel or in
gasoline blends containing 85% ethanol. The second
most common biofuel is biodiesel, which is made primar-
ily from oily plants (such as soybean or oil palm) and to a
lesser extent from other sources such as waste cooking oil.
Biodiesel, which has found most acceptance in Europe, is
usually blended with petroleum diesel in various percen-
tages. The limitation is that it can only be blended below
20% because any higher and there is the potential for
crystallisation at colder temperatures. Ultimately, the cost
of production and possible ecological impacts of biofuels
somewhat mitigates widespread adaptation [7,8,9].
Lastly, synthetic diesel is made from natural gas through
either gas-to-liquid (GTL) technology or Fischer-
Tropsch conversion processes. However, even though
synthetic diesel is regarded as cleaner burning than oil
derived diesel with less NOx and SOx emissions, it does
rely on fossil fuel for its production and produces signifi-
cant greenhouse gas emissions.
The development and uptake of the electric vehicle (EV)
has mirrored the significant developments in lithium-ion
battery (LiB) technology. This coupled with significant
investments in large scale manufacturing of LiB and
Current Opinion in Chemical Engineering 2021, 34:100756
investments in battery charging infrastructure has driven
down the cost of EVs and made it an attractive alternative
to drive down emissions from cars [10,11]. The wide-
spread uptake of EV has led to the need to continue
technical developments to address consumer and industry
Biofuels needs. In particular, the need for safer [12], higher energy
+ liquid fuel
+ high energy
- emissions from
int. combustion
and higher capacity batteries [13], faster charging [14],
density
+ existing
- bio feedstock
resource constraints
end of life cycle and associated environmental impacts
refuelling
infrastructure
- low energy conv.
efficiency and material supply chain integrity and geopolitical impli-
cations [15,16].
E-Fuels
- emissions from
int. combustion
- low energy
The generation and use of hydrogen is seen as an impor-
efficiency
tant driver for reducing greenhouse gas emissions while
still feeding the continued growth of global energy needs.
The key to realising the potential of the hydrogen econ-
omy is the production, transport, storage and utilisation of
hydrogen. There are many processes for hydrogen pro-
duction using both non-renewable and renewable energy
sources such as natural gas, coal, nuclear, biomass, elec-
trolysis, solar and wind [17,18]. Currently, liquefied
hydrogen and compressed hydrogen are two of the most
common methods of hydrogen storage and transport over
long distance. Storage of hydrogen as a gas typically
requires high-pressure tanks (350–700 bar tank pressure).
Storage of hydrogen as a liquid requires cryogenic tem-
peratures as the boiling point of hydrogen at one atmo-
sphere pressure is 252.8  C. Whilst some of the require-
ments for hydrogen transport and storage are similar,
some are application-dependant, consequently several
hydrogen storage and transport solutions may be neces-
sary. This is an important consideration if hydrogen is to
play a role in decarbonising the transport sector [19].
Hence the increased interest in investigating the use of
hydrogen carriers for safely transporting, storing and
utilising hydrogen. Hydrogen carriers currently under
investigation for large scale use include cyclic liquid
organic hydrogen carriers (LOHC) such as methylcyclo-
hexane (MCH), perhydro-dibenzyl toluene (H18-DBT),
and acyclic carriers such as methanol (MeOH), formic
acid (FA) and ammonia.
Liquid organic hydrogen carriers (LOHC)
LOHCs appear to address most of the important char-
acteristics for ideal hydrogen storage and use [20–23].
These characteristics should include a material that: has a
high energy density, is safe and easy to handle, possesses
fast hydrogen release kinetics coupled with a high quality
of released hydrogen, has the ability for long-term stor-
age, is economic with the potential to use existing infra-
structure, particularly so for the transport sector. LOHC
store hydrogen in the form of hydrogen rich organic
molecules which through catalytic dehydrogenation can
then release the hydrogen. The hydrogen depleted
organic carrier (spent fuel) is then collected and re-
hydrogenated into the original molecule to undergo the
cycle again (Figure 2) [23]. The efficiency of hydrogen
production from LOHC systems may be affected by the
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 Mobile hydrogen reformers as a novel approach to decarbonise the transport sector Chiefari and Hornung 3

Figure 2

H2 RICH fresh fuel

HYDROGENATION DEHYDROGENATION

H2 H2
in local plant on board vehicle
H2 LEAN spent fuel

Current Opinion in Chemical Engineering

A hydrogen rich LOHC (e.g. H18-DBT) undergoes catalytic dehydrogenation to generate hydrogen for use in a fuel cell on board a vehicle. The
hydrogen lean LOHC (e.g. DBT) can be collected and undergo catalytic re-hydrogenation ready for re-use.

stability of the LOHC over repeated hydrogenation/de- applications such as large-scale hydrogen storage and
hydrogenation cycles. This is due to catalytic de-hydro- transport. Importantly, LOHC systems allows for energy
genation typically requiring temperatures above 350 C, release at the time and at the location of highest energy
which may cause by-products and thus the storage capac- need, a fact that adds significantly to the economics of
ity could be compromised by partial dehydrogenation local or mobile applications such as is needed in the
[24]. transport sector [23]. One can distinguish two general
types of LOHCs, cyclic and acyclic. While cyclic
Table 1 shows the typical properties of LOHC materials, LOHCs such as MCH and H18-DBT produce no CO2
such as MCH, H18-DBT and MeOH compared to other emissions at the point of use, acyclic carbon-based
hydrogen sources such as liquid hydrogen and ammonia. LOHCs such as methanol on the other hand, releases
In contrast to liquid hydrogen, the LOHC can be han- CO2 during the dehydrogenation process. Depending on
dled (stored, transported) at ambient conditions and is the application scenario and where this CO2 is released
considered generally safe and stable in much the same to the environment, this might either be acceptable or
way as crude oil-based fuels (e.g. diesel, and gasoline). In undesirable; however in both cases the methanol would
some cases, such as H18-DBT, where the boiling point have to made from CO2 that was captured from the
lies significantly higher than most common hydrocarbon atmosphere in the first place for this solution to be
fuels, flammability and therefore safety hazards are carbon neutral and renewable. The emissions from the
much reduced compared to diesel or gasoline. This reforming of ammonia is dependent on the technology
makes the use of LOHCs well suited for a range of approach used, but consist predominatly of the by-prod-
uct nitrogen. In general, reforming ammonia outside of a
fuel cell releases nitrogen as a by-product, which may
have to be separated from the hydrogen stream before
Table 1
use in the fuel cell. Two alternative approaches, without
General properties of hydrogen carriers that determine applic- the use of an external reformer, have received a lot of
ability [41,42–44] attention and they are (i) the use of ammonia directly in a
Liq. H2 MCH H18-DBT Ammonia Methanol solid oxide fuel cell (SOFC) or (ii) a direct ammonia fuel
Density 706 769 912 682 792 cell (DAFC). In both the SOFC and the DAFC, some
(kgm 3) (0.1 MPa) NOx emissions are present [25,26].
Boiling Point 252.9 101 390 33.3 65
( C) Structured catalysis & advanced design
Freezing Point 259.2 126 34 77.7 97.6
( C)
Catalytic fixed beds have been a major pillar of indus-
H2 density (wt 100 6.2 6.2 17.8 12.5 trial processes for many years and a standard way of
%) employing heterogeneous catalysts in chemical man-
H2 density (vol 7.1 4.7 6.4 12.1 9.9 ufacture. While simple to design and implement, they
%)
suffer from a number of well-known drawbacks during
H2 release 252.9 200 400 200 400 350 900 420
temp. ( C) operation, such as high pressure drop, irregular flow
Regeneration – 100 200 100 200 400 600 250 patterns, and poor temperature control [27]. The
temp. ( C) advent of additive manufacturing techniques such as
direct 3D printing of metals or ceramics have enabled

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4 Reaction engineering and catalysis: microreactor engineering
the preparation of novel structured catalyst systems
and the use of geometries and designs previously not
feasible with conventional subtractive manufacturing
methods. In recent years, engineers and scientists
have utilised the potential of 3D printing to develop
new catalytic reactor systems which can outperform
traditional fixed beds [28–34,35,36].
The ability to tailor the reactor geometry to best suit a
chemical process, and the ability to rapidly prototype the
device, can give 3D printed reactors a competitive advan-
tage, especially in highly specialised or space-critical
applications. By using a 3D printing approach most of
these new reactor configurations can be considered hier-
archical catalyst system, a concept of significant research
focus in the catalyst field [37–39], as different length
scales are addressed by different preparation methods.
The 3D printing process is used to form features on the
mm-scale and mm-scale that act as flow guides and in most
cases as a scaffold for the catalytic layer. The outer shell
around the catalytic section can either be made from
traditional engineering components such as metal tubing
or 3D printed as well and is usually of diameters between
several mm and decimetres. Finally, the porous catalyst
containing mm-scale and nm-scale porosity is either
applied as a coating using electrodeposition, wash coating
or other methods, or formed directly by the 3D printing
process, such as in the case of 3D printing of ceramics,
followed by wet impregnation with the catalytically active
metal species. Such a hierarchical approach results in a
highly efficient catalyst and reactor configuration, espe-
cially for liquid-gas and gas phase processes. Our group at
Figure 3
(b) Ni Ni
Ru
Au
Pd
Pd
(a)
(c)
3D printed catalyst system termed Catalytic Static Mixers (CSM) manufactured by Precision Catalyst (http://precisioncatalysts.com.au/); (a)
uncoated stainless steel mixer inside a 6 mm ID tube, (b) coated CSM with various catalyst coatings, (c) SEM image of a Pd catalyst layer, (d)
reactor cartridge for (de-)hydrogenation reactions housing up to 10 cylindrical CSMs, (e) oil heated shell & tube reactor (Ehrfeld Miprowa1) for
(de-)hydrogenation reactions housing up to 16 flat CSMs.
Current Opinion in Chemical Engineering 2021, 34:100756
CSIRO has employed these 3D printed catalyst systems
in a variety of hydrogenation applications, mainly for the
manufacture of high value chemicals, such as pharma-
ceuticals [40], fragrances and flavourings [41] and fine
chemicals [42]. Figure 3 shows some of these 3D printed
catalyst structures.
Compared to classical packed bed systems, 3D printed
structured catalysts, can significantly decrease pressure
drop across the reactor and improve the heat management
and overall reaction performance [43]. The much-
enhanced freedom over engineering design of 3D printed
catalytic reactor systems and their high efficiency, makes
them particularly suitable for space-critical applications,
such as a mobile reformer unit on board of a vehicle
platform, supplying hydrogen to a fuel cell. As compact-
ness and weight efficiency of such a catalytic reformer are
crucial, the degree of process intensification required for
its use in mobile applications is high, and integration with
other components of the power train are imperative. As
the hydrogen reforming step for the LOHC systems
named above is always endothermic, integration of waste
heat generated by the fuel cell can help optimise the
overall energy balance and therefore the efficiency of the
vehicle.
However, such a powertrain consisting of an LOHC fuel
tank, a hydrogen reformer, a hydrogen fuel cell and an
electric engine constitutes a highly complex energy con-
version system, and its efficiency and reliability would
have to be benchmarked against simpler solutions such as
a compressed hydrogen tank and a fuel cell or a battery.
(d)
Pt
Pt
Rh
(e)
Current Opinion in Chemical Engineering
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 Mobile hydrogen reformers as a novel approach to decarbonise the transport sector Chiefari and Hornung 5

For smaller vehicles and use cases with infrequent refuel-
ling/recharging times and short distances, such as in urban
and personal transportation, the LOHC model may not be
attractive or economic. For long distance transport and
larger vehicles however, it might outperform the other
energy sources. These could include both passenger and
freight applications for trains (mainly replacing existing
diesel trains) and ships (replacing marine fuels), freight
trucks (especially for long distance transport), large agri-
cultural vehicles, mining vehicles or construction vehicles
(see Figure 4).
In the Australian context, applications in the mining
and agricultural sectors are particularly interesting, as
heavy machinery is required in often very remote
locations. In these scenarios, the use of battery EVs
is not feasible due to the large power demand, and
transport, handling and storage of large amounts of
compressed hydrogen might be less attractive due to
the associated hazards. Renewable hydrocarbon fuels
such as E-fuels and LOHCs are believed to be most
suitable in these applications, and their implementation
would require very little changes to the existing infra-
structure, which is mainly based on the use of diesel.
Furthermore, the example of a remote mining site also
highlights another very interesting aspect of LOHCs.
Allowing for the potential loss of small amounts of
LOHC from repeated hydrogenation/de-hydrogenation
cycles, there is the potential to largely regenerate the
spent LOHC on site, using hydrogen generated from
renewable energy such as solar panels or wind turbines.
In this scenario a fleet of LOHC-operated mining
vehicles would operate from a central mining hub
which contains a local hydrogenation plant, that can
regenerate spent LOHC fuel on site, using hydrogen
from a bank of electrolysers (see Figure 2). Such a
mining fleet would be fuel-independent, and the cost
associated with the transport of diesel fuel to such a
remote site would be eliminated.
Concluding remarks & future work
At the current stage of development of the hydrogen
economy ecosystem (i.e. the development of different
hydrogen carrier fuels, hydrogen reforming technologies,
fuel cell developments), it is unlikely that there will be
one hydrogen system to cater for all applications across all
geographic regions. This is highlighted by the range of
different activities such as the European Commission
Horizon 2020 project that focuses on the use of H18-
DBT (https://cordis.europa.eu/project/id/779694 and
technical publications https://cordis.europa.eu/project/
id/779694/results) whereas in Asia, Japan has made sig-
nificant investments in demonstrating the first global
supply chain demonstration project which is based on
MCH (https://www.mitsui.com/jp/en/release/2017/
1224164_10832.html). Other fuels such as ammonia will
also likely become a major contributor simply because
there is a major supply chain and infrastructure already in
place that manufactures and safely transports and stores
ammonia [44] (https://www.ammoniaenergy.org/articles/
ammonia-figures-prominently-in-iea-hydrogen-report/).
In a similar way, the successful adoption of the hydrogen
economy by governments, industry, society and consu-
mers will be dependent on having different hydrogen fuel
options and the ability to transport hydrogen safely in the
form of a liquid carrier and reform it close to or at the point
of use. A 3D printed catalytic reactor system as described
above provides the ability to generate hydrogen in a small
footprint, easily scalable unit. The transport sector would
be ideal for such a mobile unit with the benefit that it
could easily be applied in remote communities.

Figure 4

H fresh H2 carrier
2
H2 fuel cell Catalytic H2 reformer Liquid fuel tank
heat spent H2 carrier

Using hydrogen carriers in transport

Current Opinion in Chemical Engineering

Powertrain of an LOHC vehicle consisting of an LOHC fuel tank, a hydrogen reformer and a hydrogen fuel cell.

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6 Reaction engineering and catalysis: microreactor engineering
There are some key engineering challenges that will need
to be addressed for successful implementation of this
technology which include; the separation of hydrogen gas
from the fuel, the integration of the reforming unit with
the fuel cell to maximise the energy efficiency and the
access to robust and high performing catalysts with a long
lifetime.
Conflict of interest statement
Nothing declared.
Declaration of Competing Interest
The authors report no declarations of interest.
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