Article

Concept for Temperature-Cascade Hydrogen

Release from Organic Liquid Carriers Coupled
with SOFC Power Generation
Boris Brigljevic, Boreum Lee,
Rofice Dickson, Sanggyu Kang,
J. Jay Liu, Hankwon Lim
[email protected] (S.K.)
[email protected] (H.L.)

HIGHLIGHTS
A concept for LOHC
dehydrogenation process
intensification is presented

Energy efficiency is evaluated

through process simulation using
Aspen Plus

SOFC is used as a proven system

for clean stationary power
generation

Current concept increases energy

efficiency by a factor of 1.3–2

Liquid organic hydrogen carriers (LOHCs) are a potentially safer alternative to

conventional hydrogen storage processes. Here, Brigljevic et al. select four similar
LOHC compounds and exploit differences in their physical chemistry, presenting
the concept of a temperature-cascading process for a more energy-efficient
dehydrogenation.

Brigljevic et al., Cell Reports Physical Science 1,

100032
March 25, 2020 ª 2020 The Author(s).
https://doi.org/10.1016/j.xcrp.2020.100032
Article
Concept for Temperature-Cascade Hydrogen
Release from Organic Liquid Carriers
Coupled with SOFC Power Generation
Boris Brigljevic,1 Boreum Lee,1 Rofice Dickson,3 Sanggyu Kang,2,* J. Jay Liu,3 and Hankwon Lim1,4,*

SUMMARY
For a sustainable hydrogen economy, large-scale transportation and storage of
hydrogen becomes increasingly important. Typically, hydrogen is compressed
or liquified, but both processes are energy intensive. Liquid organic hydrogen
carriers (LOHCs) present a potential solution for mitigating these challenges
while making use of the existing fossil fuel transportation infrastructure. Here,
we present a process intensification strategy for improved LOHC dehydrogena-
tion and an example of clean power generation using solid oxide fuel cells. Four
LOHC candidates—ammonia, biphenyl-diphenylmethane eutectic mixture,
N-phenylcarbazole, and N-ethylcarbazole—have been compared as stand-alone
and integrated systems using comprehensive process simulation. ‘‘Temperature
cascade’’ dehydrogenation was shown to increase the energy generated per
unit mass (kWh/kg LOHC) by 1.3–2 times in an integrated system compared to
stand-alone LOHC systems, thus providing a possibility for a positive impact
on a LOHC-based hydrogen supply chain.

INTRODUCTION
Utilization of hydrogen as an energy vector in a renewable-energy economy pre-
sents significant advantages as it is abundant, has a high gravimetric energy den-
sity1 (120 MJ/kg), and the production can (and has been) integrated with surplus
renewable electricity. The price of H2 produced from renewably generated elec-
tricity can be expected to decrease as the total global supply of renewable elec-
tricity sources increases. Coupled with emerging high-efficiency conversion tech-
nologies such as reversible protonic ceramic electrochemical cells, with a
reported 97% electric-to-hydrogen efficiency,2 the price of renewably generated
hydrogen should become more competitive as the industrial supply of these con-
version technologies is increased within the next decade, according to Glenk and
1Ulsan National Institute of Science and
Reichelstein.3 One of the challenges of the utilization of hydrogen as an energy
Technology, School of Energy and Chemical
vector lies in storage and transportation technologies. Elemental hydrogen under Engineering, 50 UNIST-gil, Eonyang-eup,
25 C and 1 atm has a low density of 0.08375 kg/m3 (8.38e 5 kg/L),4 and thus the Ulju-gun, Ulsan 44919, Republic of Korea

lowest volumetric energy density of 0.01 MJ/L compared to most of the 2Gwangju Institute of Science and Technology,
School of Mechanical Engineering, 123
commonly used fuels. Consequently, to store (for later utilization or transport) Cheomdangwagi-ro, Buk-gu, Gwangju 61005,
any quantity of hydrogen, most common, large-scale hydrogen storage techniques Republic of Korea
such as compressed hydrogen (200–700 bar),5 and liquefied hydrogen ( 253 C)6 3Pukyong National University, Department of
Chemical Engineering, 45 Yongso-ro, Nam-gu,
require somewhat rigorous conditions of pressure and temperature, which trans-
Busan 48513, Republic of Korea
late into significant energy expenditures and safety considerations. As this inhibits 4Lead Contact
the progress of the hydrogen economy, alternative hydrogen storage techniques
*Correspondence: [email protected] (S.K.),
in the form of a liquid organic carrier have been extensively researched and devel- [email protected] (H.L.)
oped in the past decade.7–10 https://doi.org/10.1016/j.xcrp.2020.100032

Cell Reports Physical Science 1, 100032, March 25, 2020 ª 2020 The Author(s). 1
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Numerous advantages of liquid organic hydrogen carriers (LOHCs) as attractive stor-
age compounds, owing to their cyclical nature, relative safety, well developed pro-
duction technology, and comparative lack of carbon emissions, have been widely re-
ported elsewhere, particularly by Reuß et al.,11,12 Preuster et al.,13 Runge et al.,14
and many others, and are not discussed here in detail. Compared to conventional
storage technologies, the use of LOHCs essentially allows for a wide selection of
globally produced and well-characterized chemicals (in terms of their handling
and chemistry), providing a suitable selection for integration in the present liquid-
fuel-based transportation infrastructure. A suitable LOHC candidate can ideally be
used to bridge the distance between locations of high renewable energy supply
and high clean energy demand, which are, on a global average, non-urban and ur-
ban, respectively. On the energy-demand side, hydrogen must be released from its
LOHC in an endothermic chemical reaction at high temperatures. The source of the
energy for that release (fossil fuel or renewable) and the efficiency of its usage will
directly affect the overall efficiency of the LOHC-derived renewable electricity.
Dehydrogenation processes for various LOHC candidates have been designed
and theoretically evaluated.15–17 Eypasch et al.18 have modeled and performed an
economic evaluation of an industrial-scale LOHC system based on dibenzyltoluene
(DBT) (an LOHC used partly in this work) and have concluded that an energy-self-suf-
ficient system (at this time) has a 47% higher cost per unit of electricity produced than
an average grid price.

This study presents a previously unexplored process-intensification strategy for

LOHC dehydrogenation, with an ultimate goal of increasing the energy efficiency
of the process and consequently improving the viability of LOHCs in a hydrogen-
based energy economy. A dehydrogenation process has been designed and simu-
lated in which four LOHC chemicals are combined in a cascading fashion using the
same energy source. This process is then compared with single LOHC systems,
which use equal energy input and are compared based on the hydrogen yield.
Finally, all of the processes are integrated with a solid oxide fuel cell (SOFC) model
and compared based on the total kilowatt hours generated per kilogram of the
LOHC chemical. The temperature-cascade (TC) LOHC dehydrogenation process
was demonstrated to yield substantial performance improvements compared to sys-
tems that use single LOHC chemicals and can be used (e.g., in SOFCs) for a carbon-
free stationary power generation system.

RESULTS AND DISCUSSION

Heat Source Flowrate and Temperature Comparison
Single LOHC systems and the TC LOHC system were first compared based on the
same fixed heat source (flue gas), with a flowrate and temperature of 240 kg/h
and 580 C, respectively (Figure 1). As can be observed, when compared to LOHC
systems 2, 3, and 4, the TC LOHC system performs second best in terms of H2 gener-
ated (4.36 kg/h) and the best in terms of total electrical energy produced per kilo-
gram of LOHC (1.06 kWh/kg). This value was chosen as a goal to be maximized as
it potentially has a beneficial impact on the LOHC supply chain, since more energy
can be cleanly produced for the same mass of LOHC.

An obvious outlier here is the LOHC 1 system (ammonia), which produces 2.53 kWh/
kg (LOHC). Although comparatively higher, this value must be observed differently
from other systems because ammonia converts into hydrogen and nitrogen and
therefore cannot be hydrogenated again, but rather synthesized. Therefore, in terms
of the LOHC supply chain, the energy difference of ammonia synthesis and LOHC

2 Cell Reports Physical Science 1, 100032, March 25, 2020

Figure 1. Hydrogen and Electricity Generation Comparison
(A) Comparison of single LOHC and TC systems based on optimal LOHC flowrate and resulting H 2
generated.
(B) Electricity produced in kilowatt hours per kilogram of LOHC.

hydrogenation (charging) must be taken into account, which is beyond the scope of
the present study.

Heat Source Variable Temperature Comparison and Relative System Sizing

As the temperature of the flue gas can be adjusted by varying the air:fuel ratio, a
sensitivity analysis was performed to account for the effect of different temperatures
(and, consequently, flows) of the heat source (Figures 2A and 2B). It can be observed
that the change in total power generated is the greatest in LOHC systems that have
higher reaction temperatures (LOHC 1 and 2) as the temperature of the heat source
increases. For the temperature variation in [580 C–730 C], the TC system outper-
forms LOHCs 2–4 in terms of power generated per kilogram of LOHC by an average
factor of 1.3 compared to LOHC 3, and an average factor of 2 compared to LOHC 2,
while LOHC 4 is between LOHCs 2 and 3. Analogous to Figure 1, LOHC 1 is an outlier
in terms of the sharp increase of kilowatt hours per kilogram LOHC with respect to
increasing temperature and must be viewed differently because of the reasons out-
lined earlier.

To provide a relative comparison of the reactor system complexity between the sin-
gle and TC LOHC systems’ reactors, they were sized assuming a tube bundle contin-
uous reactor with set dimensions of a single tube of 1.5 m length and 0.15 m diam-
eter (Figure 2C). The total reactor volume (as a sum of single tube volume integers)
for complete dehydrogenation was assessed assuming the dehydrogenation ki-
netics for DBT-pentahydrate (DBT-18) published by Peters et al.19 It was not pre-
sumed that these kinetics accurately model the actual kinetics of LOHCs in this study.
Rather, they were used simply to compare the relative reactor size differences since
the same LOHCs are compared in both single and TC systems.

Under this assumption, the total number of reactor tubes was determined for each
case (Figure 2D). The total number is an average for each LOHC system considering
the heat source temperature variation. From Figure 2D, it can be observed that the
average total number of reactor tubes for the TC system is comparable to LOHC 3,
which is between LOHCs 4 and 2. Net power produced per reactor tube, however,
provides a clear advantage for the TC LOHC system as it can generate more power
with the same number of reactor tubes compared to the single LOHC systems. This
metric is even higher than the outlier LOHC 1, which further demonstrates the in-
crease in efficiency (in terms of energy generated per same amount of equipment)

Cell Reports Physical Science 1, 100032, March 25, 2020 3

Figure 2. Heat Source Temperature Variation and Relative Reactor Sizing
(A) Heat source temperature variation effect on the total power produced and power per kilogram
of LOHC.
(B) TC system LOHC optimal distribution in relation to flue gas temperature.
(C) Required reactor volume in relation to LOHC conversion.
(D) Required number of reactor tubes for LOHC system and electricity generated per reactor tube.
LOHC 1, 2, 3, 4, and TC: green, purple, blue, red, and yellow, respectively.

compared to LOHCs with the highest H2 storage potential. Compared to single

LOHC systems, the net power generated per reactor tube for TC LOHC increased
by a factor range of 1.17–1.97.

To summarize, in this study, a process-intensification strategy for the increased effi-

ciency of LOHC dehydrogenation was comprehensively evaluated. Four LOHC can-
didates were combined into a single system that uses the same heat source for dehy-
drogenation through LOHC reaction temperature differentials in a TC fashion. Such
a system was integrated with an SOFC stack for zero-carbon electricity generation
and compared with dehydrogenation systems which use only a single LOHC.

TC LOHC outperforms its single LOHC counterparts in virtually every metric besides
the already-discussed outlier of ammonia. Including the temperature variability of
the heat source, TC outperformed other systems in electrical energy generated
per kilogram of LOHC by a factor of 1.3–2. Finally, it was shown how this integrated
system can considerably increase the amount of clean energy generated (1.17–1.97
times) with a reactor system of the same complexity compared to single LOHC
systems.

This leads us to draw the conclusion that the utilization of energy conservative and
integrated process designs such as TC dehydrogenation can notably increase the
hydrogen yield at zero-carbon emissions, thus providing a more energy-efficient
process for clean hydrogen release and utilization. A detailed techno-economic
assessment is required to fully define and quantify whether the benefits (increased
efficiency) outweigh the possible drawbacks (more expensive LOHC transport) of

4 Cell Reports Physical Science 1, 100032, March 25, 2020

Scheme 1. LOHC Structures and Relevant Properties
Selected and color-coded LOHC candidates with their respective dehydrogenation reaction
stoichiometries, structures, and H 2 storage capacities, ordered from top to bottom by descending
reaction temperature.

this design. If that were the case, then this strategy may be required if the economic
viability of renewable energy vectors and their faster implementation are to be
achieved.

EXPERIMENTAL PROCEDURES
LOHC Selection
Considering that the purpose of LOHCs is the secure transport and storage of
hydrogen, the likely candidates should possess some combination, or ideally all,
of the following features: (1) high H2 storage density (amount of H2 it can carry per
unit mass or volume); (2) preferably liquid with low volatility (for safe and convenient
transport and storage); (3) preferably low reaction enthalpy and temperature (rela-
tive to other candidates); (4) high reversibility (low degradation during H2 charging
and discharging); and (5) low environmental hazard and cost.

As the central point of this work is improving the energy efficiency of the hydrogen
release process using a shared energy source, the temperature gradient between
the LOHC candidates’ reaction temperatures was the additional feature considered
in their selection. Four selected candidates (Scheme 1) were described in experi-
mental and/or thermodynamic-computational dehydrogenation studies and were
deemed viable as LOHCs.

Ammonia (Scheme 1, denoted in green) is one of the prime LOHC candidates in the
literature, due to its outstanding hydrogen storage capacity (17.75 wild-type [WT]%)
and a well-established synthesis process (Haber-Bosch), which is a de facto industry
standard.20 Experimental study of energy-self-sufficient ammonia dehydrogenation
and subsequent electricity generation through SOFC by Cha et al.21 formed the ba-
sis of the present study. Although more recent research has demonstrated the pos-
sibility of using ammonia directly in a fuel cell, Zhao et al.22 note that, while prom-
ising, it still must develop to the point of the efficiency of the present fuel cell
systems.

A eutectic mixture of biphenyl and diphenylmethane (Scheme 1, denoted in purple)

is a novel LOHC candidate exhibiting properties similar to the somewhat popular
DBT-H18.23 Its dehydrogenation reaction conditions were determined in the Jang
et al.24 study and subsequently discussed applications for fuel cell integration.

Cell Reports Physical Science 1, 100032, March 25, 2020 5

Figure 3. Optimization Logic and SOFC Validation
(A) LOHC dehydrogenation simulation setup.
(B) SOFC model validation; experimental versus simulated current-voltage (I-V) curve.

Carbazole-based LOHCs N-phenylcarbazole and N-ethylcarbazole (Scheme 1 de-

noted in blue and red, respectively) were assessed in a thermodynamic computa-
tional study by Shin et al.,25 which was used as a basis for consideration in the pre-
sent study due to their high hydrogen storage capacities and reaction temperatures,
which are suitable for the TC process.

LOHC-SOFC Simulation, Validation, and Optimization Setup

The LOHC dehydrogenation and SOFC unit were simulated using Aspen Plus
version 11. For dehydrogenation, a thermodynamic property method based on
the Soave-Redlich-Kwong (SRK) cubic equation of state (EOS) was used as it is suit-
able for nonpolar mixtures such are hydrocarbons and light gasses. SOFC simulation
used the thermodynamic property method based on the Peng-Robinson cubic EOS
due to its applicability domain, which extends to high-temperature and high-pres-
sure regions.

SOFC was chosen as a representative hydrogen-to-electricity conversion route since

it is widely accepted as a future standard for stationary clean power generation.26
The experimental SOFC was a planar-type, co-flow fuel cell stack, with an active
area of 18 cm2, and inlet temperature and pressure conditions of 700 C and 1
atm, respectively. The air:hydrogen standard volume flow ratio was set to 4.5. Sub-
sequently, the SOFC model was designed and validated against the experimental
voltage-density measurements (Figure 3B). When scaled up linearly (achievable by
increasing the number of stacks), 1 kg/h of H2 produces 18.04 kW of power, which
translates into 54.1% SOFC efficiency and was used as a basis for the assessment of
the total power produced from an LOHC system.

Single LOHC dehydrogenation (Figure 3A) was conceptualized as a plug-flow tube

bundle reactor, which is heated to reaction temperature by a countercurrent flow of
hot flue gas (analogous to the natural gas reformer furnace). The system was scaled
to a constant 1 kg/h H2, which was used as a fuel for the dehydrogenation. Essen-
tially, the flowrate of fresh LOHC (+) (and consequently the produced H2) was opti-
mized to maximize the energy extraction from a constant fuel flowrate. Constraints
ensured that the system operates within a thermodynamic reality. For the reaction
to even occur, heat is required to bring the LOHC (+) to reaction temperature and
to ensure enough energy to satisfy the endothermic heat of dehydrogenation.

6 Cell Reports Physical Science 1, 100032, March 25, 2020

Figure 4. Main Process Design
TC LOHC dehydrogenation and SOFC electricity generation conceptual process design. The chart depicts flue gas temperature as it travels through the
system. (+), H 2 charged; ( ), H 2 discharged; C, compressor; FD, flash drum; HX, heat exchanger; HXW, water cooler; R, reactor.

Therefore, the flue gas temperature at the inlet must be higher than the reaction
temperature of the particular LOHC system (DT of 50 C was set as the minimum).
The flue gas temperature (and the flowrate) was controlled by varying the air:fuel ra-
tio. The second constraint ensured that the flue gas exited the system at a temper-
ature that was no greater than the reaction temperature of the LOHC system. The
bulk of the produced hydrogen was used in an SOFC stack for direct electricity gen-
eration, and the part of the H2 was used as a fuel. The flue gas contained no CO2,
yielding virtually zero-carbon electricity generation. It must be noted that trace
amounts of dehydrogenated LOHC vapors may remain in the hydrogen stream,
which would produce some COx when combusted. This, however, is a negligible
amount when compared to fossil fuel combustion and can be further minimized
with appropriate separation operations (adsorption and H2 selective membranes,
to name a few).

TC Process Design and Description

The main premise for the TC process design was the fact that the flue gas will exit the
LOHC system at the temperature close to but not lower than the reaction temperature
of that system. It is conceivable that one could use a combination of LOHC chemicals
with high enough reaction temperature gradients so that the flue gas exiting one system
would still have a high enough temperature for the dehydrogenation of the next system.
This concept was designed and tested using four LOHCs (Scheme 1), which were dehy-
drogenated in a series (TC) using the same heat source from combusting 1 kg/h of H2
(Figure 4). As detailed earlier, the flowrates of all LOHCs were maximized while being
kept within the thermodynamic constraints for each system. Here, the air:fuel ratio
was set (with reference to maximum flue gas temperature) so that the flowrate of
LOHC 1 (ammonia) would produce the required 1 kg/h H2 in a mixture with nitrogen.
This was chosen since other LOHCs are comparatively much simpler to separate from
the produced hydrogen (cooling + flash drum) and are recovered for subsequent
charging. Ammonia, however, is non-reversible from the perspective of LOHCs and is
therefore used entirely as a non-carbon heat source for a stand-alone LOHC

Cell Reports Physical Science 1, 100032, March 25, 2020 7

dehydrogenation system. LOHCs (+) (charged) 2, 3, and 4 are pre-heated in a heat
exchanger by a hot mixture by hot reactor products and dehydrogenated in a temper-
ature range tuned to that particular system (Figure 4). The LOHCs were cooled and
separated from the produced hydrogen in flash drums, after which they were pumped
to storage. Hydrogen from each LOHC system was combined and sent to the SOFC
stack for electricity generation.

To determine the benefits of this design concept, the TC system was compared to
each stand-alone LOHC system. All of the comparisons were made based on the
same fuel input (1 kg/h H2). Conductive and convective heat losses from the flue
gas to the reactor and the LOHCs were not assessed for this comparison as they
would equally affect the stand-alone systems and each LOHC system in the TC
concept. The primary objectives of this comparison were to quantify the amount
of electricity generated from each system, the amount of electricity generated per
kilogram of LOHC used, and finally the amount of electricity generated per total
number of reactor vessels (as a potential indicator of reduction of complexity of
the reactor system).

ACKNOWLEDGMENTS
This research was supported by the Hydrogen Energy Innovation Technology Develop-
ment Program of the National Research Foundation of Korea (NRF) funded by the
Korean government (Ministry of Science and ICT [MSIT]) (NRF-2019M3E6A1064290).

AUTHOR CONTRIBUTIONS
Conceptualization & Methodology, Writing – Original Draft, Writing – Review & Ed-
iting, B.B.; Investigation & Formal Analysis, B.B., B.L., and R.D.; Validation, Software,
S.K. and J.J.L.; Project Administration, B.L.; Supervision, Funding Acquisition, H.L.

DECLARATION OF INTERESTS
The authors declare no competing interests.

Received: December 22, 2019

Revised: January 20, 2020
Accepted: February 3, 2020
Published: March 25, 2020

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