Chemical Engineering Journal 479 (2024) 147205

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Chemical Engineering Journal

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Electrified steam methane reforming of biogas for sustainable syngas

manufacturing and next-generation of plant design: A pilot plant study
Thomas N. From a, b, Behzad Partoon a, Marené Rautenbach b, Martin Østberg b, Anders Bentien a,
Kim Aasberg-Petersen b, Peter M. Mortensen b, *
a
Department of Biological and Chemical Engineering, Aarhus University, Hangøvej 2, 8200 Aarhus N, Denmark
b
Topsoe A/S, 2800 Kongens Lyngby, Denmark

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

Keywords: Electrification of the traditional steam methane reforming (SMR) technology for syngas manufacturing has a
Biogas significant CO2 reduction potential and make it more feasible to operate in combination with carbon capture/
Steam methane reforming utilization, especially if renewable electricity is used. This pilot plant study demonstrates the first operational
Electrification
experience with industrial-scale electrified steam methane reforming (eSMR) technology using biogas as sus­
Sustainable chemicals and fuels
tainable carbon feedstock. Across an operating envelope spanning from combinations of 5 to 20 barg and 750 ◦ C
Renewable energy
Industrial catalysis to 1000 ◦ C, the eSMR produces syngas as expected from thermodynamics. However, without the thermal re­
strictions inherent in the SMR design, the eSMR can achieve higher temperatures, enables fast transient oper­
ation, with high stability and control, thereby increasing the overall performance and design flexibility. Initial
thermal responses of the eSMR were tested, demonstrating fast start-up from an idle state to operating conditions,
within 2.6 h, including heating from 630 ◦ C to 900 ◦ C. Furthermore, dynamic temperature control was also
demonstrated with heating rates up to 330 ◦ C/h. Experimental energy efficiency of the pilot reactor was
quantified between 72 % and 80 %, with the residual being heat loss to the surroundings due to the relatively
small scale. With further scale-up to ≥1 MW reactor capacity, efficiencies of ≥99 % are predicted with a specific
electrical energy consumption of 1.0 kWh/Nm3 H2. Overall, the efficiency and operational flexibility are
improved due to the direct electrical heating of the catalytic system. Combined with biogas as feedstock, this
paves the way for attractive and competitive plant designs for sustainable and renewable production of chemicals
and fuels.

1. Introduction ammonia, methanol, synthetic fuels) will be a requirement to meet the

targets [2].
The global transition to a low-carbon and sustainable production Despite green hydrogen (generated from a renewable energy source)
requires purposeful, transformative, and non-marginal technological, is considered as a central element in decarbonizing the global chemical
systemic, and socio-behavioral changes that disrupt existing develop­ and fuel production, 96 % of the global hydrogen production is still
ment trends. In line with this perspective, the European Union (EU) has derived from fossil fuels, (grey hydrogen), where natural gas counts for
put forward “Fit for 55” package targeting a 55 % reduction of GHG 48 %, heavy oil and naphtha for 30 %, and coal for 18 % of the global
emissions from EU countries by 2030. The proposed package targets feed stock. Only 4 % of the global hydrogen production comes presently
legislation in different areas, aiming to move towards a more sustainable from electrolysis, whereof only 25 % is directly based on renewable
world [1]. Low-carbon energy systems are expected to depend increas­ electricity [3]. The steam methane reforming process is the most
ingly on electrification, where electricity is produced with low global widespread route for producing hydrogen from natural gas, and it is
greenhouse gas (GHG) emissions, such as wind and solar power [2]. expected to remain the dominant process for large-scale hydrogen pro­
However not all industries, in particular shipping and aviation, will be duction because of its favorable economics and existing infrastructure
able to use electricity as a direct propulsion source, and therefore, sus­ [4,5]. In that perspective, blue hydrogen has an increasing interest, as its
tainable fuels such as hydrogen and hydrogen derivatives (e.g., origin is based on fossil fuel, but where some or nearly all the CO2

* Corresponding author.
E-mail address: pmor@topsoe.com (P.M. Mortensen).

https://doi.org/10.1016/j.cej.2023.147205
Received 14 August 2023; Received in revised form 3 November 2023; Accepted 6 November 2023
Available online 10 November 2023
1385-8947/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC license (http://creativecommons.org/licenses/by-
nc/4.0/).
T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

emissions associated with its production are captured and sequestered. catalysts with higher conductivity [14–17], shorter characteristic length
Existing technologies like fired tubular reforming (SMR) and auto­ scales for heat transfer [17–19], different reactor concepts [20,21],
thermal reforming (ATR) in combinations with carbon capture have reduced temperature by shifting the equilibrium [22,23], or heating of
therefore already been proposed and implemented to produce blue magnetic catalysts by induction [24–26]. Recently, Wismann et al. [10]
hydrogen [5,6]. successfully integrated an electrically heated catalytic structure with the
In industrial fired tubular reforming plants (SMR), natural gas is steam methane reforming reaction. The integrated solution gave an
mixed with steam, and where applicable CO2, and converted into intimate contact between the electric heat source and the catalyst,
hydrogen and carbon oxides; referred to as synthesis gas (syngas). The thereby supplying energy directly to the catalytic active site with
steam methane reforming process is governed mainly by the thermo­ practically no temperature difference from heat surface to catalytic site.
dynamically independent steam methane reforming and water gas shift This integration overcomes the heat transfer limitations known from
reactions shown in Reaction (1) and (2), respectively. In the case of CO2- industrial SMR plants. Having a uniform supply of heat to the process
reforming, the water gas shift reaction (Reaction (2) plays an increased also ensures that gas composition is kept close to equilibrium
role. Combining Reactions (1) and (2) gives the dry methane reforming throughout the entire catalytic length, reducing reactor volume and
reaction (Reaction (3). Despite many combination possibilities, the leading to a higher utilization of the catalyst material. Numerous ex­
overall reaction scheme is for all cases strongly endothermic. amples of electrified reforming processes have been reported, which
involve the use of structured catalysts. These include induction heating
kJ
(1) of ferromagnetic catalyst [24,25], microwave heating of a structured Ni/
◦
CH4 (g) + H2 O(g)⇄3 H2 + CO(g) (ΔHr = 206 )
mol
SiC catalyst [27,28] or ohmic heating [29,30]. Fast temporal response
kJ and dynamic operation is achievable as a result of the electrical heating,
(2)
◦
CO (g) + H2 O(g)⇄CO2 (g) + H2 (g) (ΔHr = − 41
mol
) contrary to industrial SMR plant where low heating rates and steady
state operation are required to avoid thermal stress or formation of
CH4 (g) + CO2 (g)⇄2 H2 (g) + 2CO(g) (ΔHr = 247
◦ kJ
) (3) hotspots [12,13]. These features are especially interesting in a world
mol where the need for more flexible technologies is in high demand for
dynamic operations.
Syngas as an intermediate facilitates a production platform of large-scale
The electrified steam methane reforming (eSMR) technology effec­
chemicals including ammonia, methanol, and liquid fuels, among
tively removes the need for a combustion section in the steam methane
others. Configuration of these chemical production plants is favored by
reforming scheme, thereby eliminating the directly associated CO2
operating the SMR plants at high pressure. However, following the Le
emissions, assuming use of renewable electrical power. If, in addition,
Chatelier’s principle, this limits the conversion of the reforming reac­
biogas or SNG, from renewable sources, is introduced as carbon feed­
tion, and in order to compensate for this, higher temperatures are
stock, the process has a great potential for sustainable and renewable
required to drive the endothermic reforming towards sufficient methane
production of syngas. Biogas consist of biogenic carbon with a CH4 and
conversion [7].
CO2 concentrations between 50 and 75 mol% and 25–50 mol%,
The industrial (grey) SMR process has a significant CO2 footprint, as
respectively [31]. This high concentration of CO2 in biogas is within the
approximately 8.6–9.3 tons of CO2 are produced per ton H2, where
range already applied for SMR feeds in industrial scale [32]. Biogas
17–41 % is a direct result of combustion of fuel and off-gas to provide the
production is also a common and mature process that has gained focus
required heat for the syngas production [5,8–10]. Typically, the fired
for its potential role as sustainable carbon source and waste handling. In
reformer is the largest, most complex, and most expensive unit operation
a biogas plant, biomass waste and manure from primarily agriculture are
in syngas production. It consists of catalyst loaded in a large number of
used in an anaerobic digester (AD) operating under mild conditions
high-alloy steel tubes that are placed in a large furnace, heated by
(35–60 ◦ C) to produce biogas and residue streams. The residue is rich in
combustion of fossil fuels and off-gases from the process. This configu­
minerals and can work as an excellent fertilizer, and is often returned to
ration allows for around 50 % of the supplied heat to be directly
the agriculture sector [33–35]. However, biogas contains sulfur com­
transferred to the reforming reaction in the catalyst bed, while the rest
pounds mainly in the form of H2S (1000–2000 ppm) that need to be
leaves as latent heat in the above 1000 ◦ C hot flue gas [11]. The com­
removed to enable catalytic steam methane reforming of biogas, as
bustion temperature of the burners must therefore be significantly above
sulfur contamination, even in the range of 1–10 ppb, can lead to deac­
the reaction temperature in order to generate the required inward heat
tivation of the Ni-based catalyst [36,37]. Nonetheless, the work of
flux [7,10]. To achieve a high energy efficiency of a SMR plant config­
Dannesboe et al. [37] proved, in full scale with 1000 h operation, that
uration, an integrated flue gas waste heat sections is a requirement,
deep sulfur removal of biogas for catalytic reforming on a nickel based
where the efficiency can be increased up to ca. 95 % if production of
catalyst is possible, using combination of well-known technologies like a
excess steam is included [7]. Performance of industrial SMR plants is
biotrickling filter, activated carbon, and sulfur guard.
typically limited by the heat transfers across the fired reformer.
Biogas production needs integration with a downstream process to
Combining low thermal conductivity with strong endothermic steam
convert the produced gas into a valuable end-product. The simplest use
methane reforming creates a steep temperature gradient across the
is for energy production (electricity and/or heat) by a gas engine, but the
catalyst bed, increasing the risk of hot spots, and cause thermal stress
relative low heating value (LHV) of raw biogas of 16–28 MJ/m3 makes it
detrimental to reactor lifetime. Typical economic and practical opera­
less sufficient as fuel compared to natural gas with LHV of around 36
tion of industrial SMR plant is therefore around 15–30 barg and
MJ/m3 [38]. This is due to the high CO2 content in the biogas. Alter­
850–920 ◦ C limited by material constraints [7,10,12,13]. Large furnace
natively, biogas can be upgraded to bio-methane as a substitute for
chambers, compression of gas, and extensive heat recovery favor oper­
natural gas. This is typically done today by separating the CO2 by an
ation at large scale, restricting economic operation to large centralized
energy intensive gas cleaning step such as amine or water scrubbers as
SMR plants [7,11]. In addition, during start-up, flowrates and heat in­
well as pressure swing adsorption [36]. The residual byproduct of CO2 is
puts are gradually increased over several days before reaching steady
typically emitted to the atmosphere, resulting in large amounts of car­
state operation as the fired section and catalytic section of the SMR al­
bon being wasted. This emission is technically green, but it is still un­
ways needs to be balanced. Consequently, industrial SMR plants perform
desired because CO2 can be used as a building block for sustainable fuels
best when operated under steady state operation, as they are not suited
and chemicals production [39–42]. In 2021, Europe had almost 18,000
for dynamic change in temperature, pressure, or load [7,10–13].
biogas production plants, where 97 % of them used the biogas for local
For decades, the low thermal conductivity of fired reformers has
heat and power generation. Only the remaining 3 % of the plants
been a topic of research. This includes investigation into materials and
upgraded biogas to biomethane to be injected into the natural gas grid

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

Fig. 1. Flow diagram of biomass to sustainable chemicals and fuels utilizing the electrified steam methane reformer (eSMR).

[43]. This presents an opportunity for valorization of the biogenic car­ compressor, and a high-pressure/high-temperature sulfur guard for
bon to more sustainable products, which prospectively could substitute removing possible remaining H2S and other sulfur compounds. The
fossil carbon in other sectors. With the present attention to emerging biogas is pressurized to the process pressure (10–25 barg) using a two-
Power-to-X (PtX) technologies, this expands the possibilities beyond stage diaphragm compressor, MV 4722IIK, from Sera (Fig. 2B). The
using green hydrogen (e.g. from electrolysis) either for direct metha­ steam generator consists of a water pump, high-pressure electric boiler,
nation of biogas over a high-surface-area nickel catalyst converting CO2 and a steam superheater. In the steam generation section, demineralized
to CH4 (biomethane) [37,42,44] or converting captured CO2 to valuable water is pumped to a steam generator where it is evaporated under
chemicals or fuels [43,45]. pressure up to 60 barg. The generated steam is subsequently super­
This work focuses on the combination of biogas and the eSMR heated. The superheated steam and desulfurized biogas are mixed
technology, which provides an alternative PtX route for sustainable forming the process gas which is preheated to 350–400 ◦ C. Hereafter,
chemical and fuel productions. This is achieved by utilizing a combi­ the process gas enters the prereformer, which contains a commercial
nation of renewable electricity and sustainable carbon feedstock to nickel-based catalyst, AR-401 from Topsoe. Prereforming is used to
produce syngas, enabling sustainable production of green fuels and convert higher hydrocarbons if present in the process gas [32,47]. The
chemicals. In practice, this configuration allows for almost zero- process gas then enters the eSMR reactor shown in Fig. 2C. The reactor
emission chemical plant with high carbon utilization. This new config­ includes an alumina-based refractory lining encapsulate the catalyst
uration demonstrates the potential for disruption of the chemical in­ zone from the surrounding reactor shell, thereby keeping a low tem­
dustry towards a more sustainable approach. This scheme is summarized perature on the reactor pressure shell. The reactor is loaded with a
in Fig. 1. Topsoe industrial eREACT™ catalyst system constituting a direct elec­
trical heated catalytic structure with nickel as the active material. The
2. Material and methods reactor is operated using electric heating, similar to previous work on
the analogous bench-scale design [10,12,48]. Electricity is supplied
Experimental work was commenced at the first-of-a-kind pilot-scale from a N8951A Power Supply Unit from Agilent Technologies. Reactor
eSMR unit on Topsoe eREACT™ technology. The eSMR unit is installed in temperature was measured with K-type thermocouples positioned at the
the Power-to-X process hall of the biogas research facility located at the catalyst exit.
Aarhus University (AU), Viborg campus, Denmark. The unit receives a The eSMR reactor produces syngas at exit temperatures of
raw biogas feedstock from a small industrial scale biogas production 750–1000 ◦ C, which is then cooled, first down to 100–130 ◦ C in an waste
plant having a 1200 m3 anaerobic digester [37]. The eSMR unit consists heat boiler shown in Fig. 2D [49], and then further to ≤40 ◦ C in a water-
of a pre-treatment section, steam generator, prereformer, eSMR, waste cooled plate heat exchanger. Condensate is subsequently removed in a
heat boiler (WHB), condensate separation and utilities sections, as high-pressure separator. The dry syngas is analyzed by a gas chro­
shown in Fig. 2A together with pictures from the installation. matograph (GC) (7890B, Agilent Technologies) for CO, CO2, CH4, N2, and
The raw biogas mostly consists of methane (50–75 mol%) and carbon H2. Higher hydrocarbons up to C6 can also be analyzed if present. The
dioxide (25–50 mol%) with small impurities like nitrogen (up to 2 mol GC is equipped with two columns (MS5A and Rt-Q-BOND), thermal
%) and hydrogen sulfide (~1000 to 2000 ppm), and it is saturated with conductivity (TCD) – and flame ionization detectors (FID). System
water at ambient conditions (20–60 mbarg) [46]. In order to protect the pressure is controlled using an equilibar back pressure regulator placed
catalyst in the downstream reforming section, the hydrogen sulfide and after the HP separator. After depressurization, the syngas is flared to
any other potential sulfur compounds are removed from the biogas. The avoid releasing CO, unconverted CH4, and H2 into the environment. The
biogas pretreatment was done in the same setup used in previous work condensate is after depressuring passing a low pressure condensator
of Dannesboe et al. [36], which consists of low-pressure/low- separating released gas from condensate. The released gas is re-mixed
temperature sulfur guards for bulk removal of H2S, a biogas with the main gas stream after depressuring.

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

Fig. 2. (A) Simplified block diagram of the eSMR setup; (B) compressor section; (C) the electrified steam methane reformer (eSMR); (D) the waste heat boiler.

3. Results and discussion tested operating regime covers 750 ◦ C–1000 ◦ C, 3–20 barg and steam-to-
carbon ratio (S/C) 2.1 to 2.7. The pilot plant data presented in this work
To enable an industrial relevant evaluation of the performance in the covers initial operation close to 2000 h.
pilot scale, test was made with respect to; thermal response, stability,
verifying thermodynamic performance, operation envelope, energy ef­ 3.1. Start-up of electrified steam methane reactor
ficiency, and energy consumption as well as investigate the synergy of
using biogas as a sustainable carbon source for syngas production. The The pilot scale eSMR reactor was tested with a start-up procedure
data were compared with industrial SMR performances and, in the end, from idle condition to stationary operation including steam and subse­
a potential process design including the eSMR technology was compared quently biogas introduction, and temperature increase using full auto­
with an industrial SMR plant design for production of syngas. The total mation control based on electrical heating. Fig. 3 shows the temperature

Fig. 3. Start-up of the industrial representative pilot scale eSMR reactor from idle state at 645 ◦ C to operation at 900 ◦ C. Conditions: Inlet temperature 400 ◦ C,
pressure 10 barg, and steam-to-carbon ratio 2.7.

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

development for the eSMR reactor as a function of time on stream (TOS), Operating temperatures are therefore limited as well as steady state
covering feed introduction and thermal heating from 645 ◦ C to 900 ◦ C, operation due to material constraints. In that perspective, the agility of
showing the transient from idle state to stationary operation. Experi­ operation the eSMR technology at industrial representative scale was
mental data of methane conversion (calculated from the carbon balance) investigated at different exit temperatures. In Fig. 4, the power load is
is included in Fig. 3. shown as function of TOS while varying the exit temperature from
In Fig. 3, steam was added at TOS = − 0.3 h to the nitrogen flow, 900 ◦ C to 750 ◦ C to 1000 ◦ C. The initial exit temperature of 900 ◦ C was
which results in a temperature drop due to higher heat capacity and flow used as a reference point for the power load at 100 %. The initial set
rate, this was subsequently counteracted by increasing the power. The point was changed to 750 ◦ C at TOS = 0, and the new exit temperature
biogas was added at TOS = 0 where a second temperature drop occurred was reached after 10 min having a small undershoot of 19 ◦ C but stable
due to the endothermic reforming of biogas. The temperature control of again after 70 min with a deviation of 0.8 ◦ C based on 1 min sampling
the eSMR reactor was switched to auto control at 645 ◦ C after 4 min frequency. The temperature drop corresponds to a power cut of 49 %
(TOS = 0.08 h) with 900 ◦ C as final set point and having a heating rate of with a cooling rate of 1000 ◦ C/h and demonstrates a fast thermal
120 ◦ C/h. The exit temperature began to increase after 8 min in auto response and accurate control of the electrified system. The fast-cooling
control, and the eSMR reactor reached a fast and stable heating rate of rate is facilitated by direct cooling from the endothermic reaction
120 ◦ C/h at TOS = 0.7 h, controlling with an average deviation of 5.2 ◦ C environment. The exit temperature was then increased in 50 ◦ C intervals
from the set point value during ramping (1 min sampling frequency). where heating rates up to 330 ◦ C/h were demonstrated in this current
The methane conversion followed the increasing temperature until configuration. In between step changes, the exit temperature was kept at
reaching a steady state conversion of 97 % after 2.3 h, which was in steady state conditions for 1–2 h to collect data and investigate stability.
thermodynamic equilibrium with respect to the reforming reactions (1) In all step changes, the temperature overshoot was not more than 5 ◦ C
and (2). In this start-up experiment, the eSMR reactor reached the set from the set point value with a maximum deviation of 1.3 ◦ C, and a new
point temperature at 900 ◦ C after 2.6 h. The time between initializing steady state condition reached within 30 min. However, since exit
auto control for the temperature increasement and reaching the desired temperature of 1000 ◦ C was new ground of the steam methane
heating rate was affected by heat losses from the pilot plant reactor reforming, a lower heating rate of 52 ◦ C/h was selected resulting in
beside the endothermic reforming. This delays the time before reaching steady state operation after 60 min. The expansion of the temperature
a stable regulation of the system. It is worth mentioning that the initial operating regime up to 1000 ◦ C improves the methane conversion and
parameters used in the PID feedback-control in Fig. 3 were selected for thereby reduces the methane slip out of the eSMR reactor, which will
optimal steady state operation. Although, the presented start-up time is increase the feed utilization in an eSMR configuration.
much faster than conventional fired SMR, further PID tuning towards The exit temperature control system of the eSMR reactor is a direct
fast dynamic changes could increase the heating rate further to obtain feedback-control of power input to the eSMR reactor controlling the
even faster thermal responses. The total time of 2.6 h is therefore an desired exit temperature. This is found to be very efficient when
initial result and could be further optimized. combining the intimate contact between the heat source and the catalyst
in the eSMR reactor, having a fast power response occurring on a
millisecond level, which enables fast and precise temperature changes.
3.2. Exploration of operating envelope
As in previous section, Fig. 4 had a PID feedback control system optimal
for steady state operation and therefore temperature response could be
Industrial SMR is limited in performance due to low thermal con­
further optimized. The eSMR reactor technology has already show great
ductivity across the reactor wall and catalyst bed. Temperature differ­
opportunities for dynamic operation, suitable to address the intermittent
ence up to 100 ◦ C between the reactor wall and the catalytic center are
nature of different sources of renewable electricity used for P2X
reported for packed-bed steam-methane reformers [13,50–52].

Fig. 4. Temperature and power profiles. Conditions: 16 barg and a steam-to-carbon at 2–2.2 [-]. Initial power load of 100% is relative to the base case condition
operation at 900 ◦ C.

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

operation. production is 3.6 kWh/Nm3 H2 as there is an additional 2.6 kWh/Nm3

H2 due to the LHV equivalent of the natural gas feed. For comparison
3.2.1. Catalytic stability test with other industrial hydrogen processes, a classical SMR plant has a
The eREACT™ catalyst system has consistently displayed stable specific net energy consumption of 4.2 kWh/Nm3 H2 all being LHV
performance, despite exposure to various operating scenarios, including equivalent of natural gas feed [53], 17 % higher than the eSMR based
multiple start-ups and shutdowns, transient operation, as well as high layout. The lower energy consumption is a consequence of the improved
temperature. This is shown in Table 1, which compares two steady-state thermal contact in the eSMR reactor resulting in higher energy efficiency
operating points, at similar conditions, with 1050 h of operation in be­ and better feedstock utilization compared to the SMR counterpart. In
tween. The variation in S/C and CH4 conversion can be attributed to the addition, these numbers also display that the eSMR uses 38 % less nat­
fluctuating methane concentration of biogas, a common occurrence in ural gas feedstock compared to SMR for production of the same quantity
biogas reforming. Methane conversion was according to thermodynamic of hydrogen. This is a result of the high temperature service at
principles, and without any sign of catalyst deactivation. 900–1000 ◦ C of the eSMR allowing for high feedstock utilization and
consequently obtaining near stoichiometric consumption figures on the
feedstock side. When used for e.g. blue hydrogen application, this results
3.3. Energy efficiency and scale up production in a reduced amount of CO2 that needs to be handled, compressed and
sequestrated.
The energy efficiency of the eSMR reactor was tested at different As alternative to syngas (or hydrogen) production by steam
biogas flow rates at inlet temperature of 400 ◦ C, exit temperature of reforming, the specific net electrical energy consumption in water
900 ◦ C, pressure at 10 barg, and S/C ratio between 2 and 2.2. The energy electrolysis systems are in the range 3.7–6.6 kWh/Nm3 H2, depending
efficiencies, based on enthalpy of reaction, were calculated at four on choice of electrolysis technology and system integration [54].
different low flow ranges varying from 15 Nm3/h to 27 Nm3/h, resulting Comparing the electrical demand in the water electrolysis systems with
in an efficiency of 72 % to 80 % for low capacities, indicated in Fig. 5. the total energy demand in the eSMR solution of 3.6 kWh/Nm3 H2,
The remaining energy is heat loss, primary to the surroundings and eSMR is lower than best in class electrolysis solution. More markedly
minor to electrical parts. Low capacities were investigated to give a though, when comparing specific electrical energy consumption of
larger description of the energy efficiency development, which subse­ eSMR to electrolysis solutions, eSMR is 75–85 % lower. The markedly
quently was used to derive a simplified energy efficiency model of the lower electrical energy consumption in the eSMR reactor is firstly due to
eSMR reactor derived from the basic energy balance of the reactor for the lower heat of reaction and secondly due to the very high energy
extrapolation to higher capacities and industrial comparison. Fig. 5 efficiency inherent in the eSMR reactor. Syngas (or hydrogen) produc­
summarizes experimental calculated efficiencies as a function of ca­ tion consequently scales better with eSMR technology relative to elec­
pacity as well as the energy efficiency and energy consumption model. trolysis technology relative to available (renewable) electricity supply.
Using the derived model, expected energy consumption was calculated
based on equilibrated gas for hydrogen production at S/C 1.8, inlet 3.4. Industrial perspective
temperature 400 ◦ C, exit temperature 920 ◦ C and pressure 30 barg.
Natural gas operation was modelled in the energy consumption for in­ The presented experimental work demonstrates how the eSMR
dustrial comparison. A detailed description of the model implementa­ technology allows for agile operation, precise process control, and
tion of the energy efficiency and energy consumption is included in syngas production according to thermodynamics. By extrapolating the
Supporting Information. design of the current unit shown in Fig. 2 to an industrial counterpart, it
Based on simple modelling, Fig. 5 shows as expected increased effi­ is demonstrated that a simplified process configuration is achievable
ciency of the eSMR reactor as capacity is increased and extrapolates to with the eSMR technology. This simplification is illustrated in Fig. 6,
above 99 % at capacities above 1 MW. The model assumes that the which schematically shows an industrial fired SMR (A) compared with
principal loss mechanism of the eSMR is heat loss to the surroundings an electrically driven eSMR (B). The central difference between the
through the surface area of the reactor. Consequently, when scaling up eSMR and SMR design is the replacement of fossil fuel (natural gas) and
the capacity of the eSMR, the surface area heat loss in the end becomes off-gas with renewable electricity to provide the necessary heat to drive
relatively low. For reference, an industrial hydrogen reforming plant at the reforming reactions, which remove the hottest and largest stream
1 MW capacity based on the eSMR technology could produce in the from the plant. This completely removes the furnace section and sub­
order of 1000 Nm3 H2/h with an energy efficiency of 99 %. sequently several additional unit operations, including flue gas fan,
The energy consumption curve in Fig. 5 represents the specific combustion air blower, flue gas stack, heat exchangers for heat recovery
electrical energy consumption of the eSMR and translates into the of the hot flue gas as well as the utilization of combustion air.
enthalpy of reaction for the steam methane reforming reaction (CH4 + Where the SMR plant design is configured around the flue gas waste
H2O). The energy consumption is consequently calculated per Nm3 heat section to facilitate process pre-heating, the eSMR plant design has
syngas (combined H2 + CO), however, in case of hydrogen production, a higher degree of freedom. In this layout pre-heating can be done by
CO would be shifted to H2 through a WGS reactor downstream the eSMR any suitable technology according to best practice. Steam pre-heaters
and thereby can be assumed equivalent to H2 [7], resulting in a 1.0 can be used if excess steam is available in the steam balance, electrical
kWh/ Nm3 H2 at a capacity above 1 MW completely covered by heaters or firring with H2 can be used for separate process heaters. In
(renewable) electricity. Adding the natural gas feedstock, the specific case of excess fuel gas in the plant design, a fired heater can be
net energy consumption of an eSMR based process for hydrogen considered. The latter is however least preferred due to an associated
CO2 emission. With increasing operation temperature in the eSMR
Table 1 design, tested up to 1000 ◦ C in this study, the methane conversion will
Evaluation of the stability of the eREACT™ catalyst system after 1050 h of increase accordingly and thereby reduce the methane slip. Together
operation at industrially representative reforming conditions. with the absence of the furnace section, this enables better feedstock
Time 1 Time 2 utilization. In that perspective, the eSMR design allows for several
TOS [h] 485 1535 attractive process configurations with natural gas or biogas.
S/C [-] 2.1 ± 0.1 2.1 ± 0.1 This could e.g. be production of blue hydrogen from natural gas with
Temperature [⁰C] 950 950 complete carbon capture due to the absence of associated flue gas [5].
Pressure [Barg] 20 20 For comparison, hydrogen production in traditional SMR layout result in
CH4 Conversion [%] 94 ± 1 94 ± 1
a carbon intensity of 9.2 kg CO2/kg H2 without carbon capture, and

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

Fig. 5. Energy efficiency and energy consumption as a function of capacity of the eSMR reactor. The Experimental data (dots) were carried out at biogas flow ranges
from 15 Nm3/h to 27 Nm3/h, inlet temperature of 400 ◦ C, exit temperature of 900 ◦ C, pressure at 10 barg and steam-to-carbon ratio between 2 and 2.2. Low ca­
pacities were investigated to give a larger description of the energy efficiency development. The energy consumption model for hydrogen production predicted with
an inlet temperature of 400 ◦ C, exit temperature of 920 ◦ C, and pressure at 30 barg and steam-to-carbon ratio 1.8.

Fig. 6. Flowsheet of A) Industrial fired SMR design utilizing natural gas as fuel and B) potential eSMR design utilizing renewable electricity as fuel.

about 3.6 kg CO2/kg H2 with carbon capture from the process side only. operation of different reactor sizes, which promote delocalization de­
The eSMR configuration allows carbon intensity to be lowered to signs [10]. This is especially important for eSMR plants utilizing biogas
approximately 5.7 kg CO2/kg H2 without carbon capture corresponding as carbon feedstock, since the low capacity of typical biogas plants has
to process stoichiometry, and less than 0.1 kg CO2/kg H2 with carbon made integration of traditional SMR’s unattractive at such sites due to
capture. This makes it an excellent option for producing blue hydrogen capacity of scale [7,10,25]. Combining the high energy efficiency with
from natural gas [53]. the biogenic carbon provided from biogas, an attractive solution is given
Additionally, the eSMR configuration enables dynamic and feasible for a potential competitive production of sustainable and renewable

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T.N. From et al. Chemical Engineering Journal 479 (2024) 147205

chemicals and/or fuels with near zero carbon emission and high carbon facility at Aarhus University, Viborg Campus, to host and support the
utilization. operation of the pilot plant. We would also like to thank the support
from TOPSOE R&D for technical assistance and supports during
4. Conclusion commissioning and operation of the eSMR pilot plant.

This study demonstrates that replacing a fired steam reformer (SMR) Appendix A. Supplementary data
with an electrically heated steam methane reformer (eSMR) based on
integrated electrical heating is feasible and that it provides an improved Supplementary data to this article can be found online at https://doi.
thermal response and control. The eSMR demonstrated electrical heat­ org/10.1016/j.cej.2023.147205.
ing feedback-controlled operation from an idle state at 630 ◦ C to oper­
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