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Energy Conversion and Management 258 (2022) 115513

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Energy Conversion and Management


journal homepage: www.elsevier.com/locate/enconman

Energy, environment, and economic analyses on a novel hydrogen


production method by electrified steam methane reforming with renewable
energy accommodation
Huchao Song a, b, Yinhe Liu a, b, *, Hao Bian a, b, Mengfei Shen a, b, Xiaolong Lin a, b
a
State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
b
School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China

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

Keywords: More and more attention has been paid to hydrogen due to its cleanity and high energy density. However,
Electrified Steam methane reforming hydrogen production from conventional steam methane reforming has high CO2 emission and heat loss in the
Renewable power accommodation flue gas. Hydrogen from water electrolysis has the defects of high cost and low efficiency. Electrified steam
Power to gas
methane reforming (E-SMR) process is proposed by integrating power to gas technology with steam methane
Hydrogen production
Techno-economic analysis
reforming based on the principle of efficient electrothermal conversion and energy cascade utilization. Electrical
equipment is used in the process to eliminate the above drawbacks and accommodate renewable electricity. The
novel process is simulated by chemical equilibrium and mass-energy conservation methods and analyzed from
energy, environment, and economy. The optimal performance of E-SMR processes is investigated by adjusting
the steam carbon ratio and reforming temperature under appropriate pressure. The optimal thermal efficiency
(97.27 %) is improved by 18 percentage points at least compared to current industrial steam methane reforming
processes. The optimal electrical efficiency (88.68 %) is at least 11.48 percentage points higher than that of
running commercial water electrolysis systems. The novel process achieves low carbon emission (even zero-
emission with CCS) since the required reforming energy is electricity instead of combustion. The cost of the
proposed process can be minimized to 2.47 $/kg H2 through economic analysis. This work may provide an
efficient, low-carbon, and economical option for hydrogen production.

electrolysis is a way of PTG, which converts renewable electricity into


hydrogen without CO2 emission for stable, long-term, and high-density
1. Introduction storage [2,4]. As an ideal clean energy carrier, hydrogen can play a
buffering and bridging role in the power system, transforming and uti­
With the development of the international economy, population and lizing the surplus electricity from renewable energy [5]. Hydrogen can
urbanization, the global energy demand keeps rising continually. be used in various fields such as transportation, construction, power
However, fossil fuel, as the main energy at present, has limited reserves. generation, and industry [6]. In addition to promoting demand for
The massive use of fossil energy results in serious climate problems, hydrogen, hydrogen transport infrastructure and low-cost and large-
which cannot meet the requirement of green energy in the future [1]. scale production of hydrogen are also critical factors for hydrogen
Recently the scale of renewable energy such as wind power and pho­ development.
tovoltaics is expanding rapidly. However, the fluctuation and intermit­ On the one hand, hydrogen transportation encounters problems of
tence of renewable energy have led to the low-grade utilization and even the poor economy and small scale due to its low density, corrosion of
partially abandonment of wind and solar energy. The development of metal, and wide explosive range [7]. Nowadays, wide attention has been
renewable energy depends on not only resources but also attracted to mixing hydrogen in natural gas pipelines for hydrogen
accommodation. transportation owing to its advantages of large-scale, long-distance, and
Energy storage systems can help solve the accommodation problem low-cost [7,8]. Demonstration projects with a hydrogen mixing ratio of
of renewable energy [2,3]. Power to gas (PTG), which is one of the up to 20 % have been launched worldwide, such as HyDeply [9] and
energy storage technologies, has received widespread attention. Water

* Corresponding author at: State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China.
E-mail address: yinheliu@mail.xjtu.edu.cn (Y. Liu).

https://doi.org/10.1016/j.enconman.2022.115513
Received 13 January 2022; Received in revised form 6 March 2022; Accepted 16 March 2022
Available online 23 March 2022
0196-8904/© 2022 Elsevier Ltd. All rights reserved.
H. Song et al. Energy Conversion and Management 258 (2022) 115513

Nomenclature Cfuel Fuel cost, $


CF Capacity factor
Abbreviations E-SMR Electrified steam methane reforming
CCS Carbon capture and storage GWP Global warming potential
COP Coefficient of performance HTHP High temperature heat pump
FCF Fixed charge factor NCF Net cash flow
HEX Heat exchanger ODP Ozone depression potential
NBP Normal boiling point WGS Water gas shift
NPV Net present value PTG Power to gas
LCOH Levelized cost of hydrogen SMR Steam methane reforming
PSA Pressure swing adsorption
S/C Steam carbon ratio Symbols
η Efficiency, % HHV Higher heating value, MJ/kg
ε Compressor pressure ratio μi The chemical potential of each component i
G Free Gibbs energy N Total number of components
△H298 The heat of reaction (298 K) ni Moles for each component, mol
M Mole mass, kg/mol Tref Reforming temperature, ◦ C
tcr Critical temperature, ◦ C pcr Critical pressure, bar
to Evaporation temperature, ◦ C po Evaporation pressure, bar
tk Condensation temperature, ◦ C pk Condensation pressure, bar
q Mass flow rate, kg/s nx Mole flow rate, mol/s
Etot Total electrical energy, MW Pa Production capacity, t/h
RCH4 Methane conversion, % n Economic lifetime, year
r Discount rate, % CO&M Operating and maintenance cost, $
Ct Annual cost, $ Ci Investment cost, $

Ontario [10]. H2 mixing ratio in natural gas can be in a fluctuation of 0 process with CCS technology, the CO2 emission is still more than 1 kg/kg
~ 20 % in the hydrogen injection in natural gas project of Ameland in H2 [22–24]. The additional CO2 emission and inefficiencies associated
The Netherlands [11]. On the other hand, the cost of hydrogen produced with combustion in conventional SMR processes have not been funda­
by water electrolysis is much higher than those of steam methane mentally addressed.
reforming (SMR) due to its high energy consumption [12,13]. Moreover, Suppose the electricity produced by renewable energy is introduced
the scale of the commercial water electrolysis project is still small. into the SMR process instead of combustion. Firstly, the flue gas heat loss
Hydrogen production from water electrolysis takes up only about 4 % of the conventional SMR process can be eliminated, avoiding the CO2
[14]. The primary process of hydrogen production is SMR, which ac­ released by the combustion of methane as fuel. At present, a large
counts for 48 % of the global hydrogen demand [15,16]. SMR process amount of industrial hydrogen comes from SMR. SMR with renewable
produces hydrogen by the reaction of steam and methane under high- electricity can significantly reduce the energy consumption and CO2
temperature catalysis, which is a conventional and cost-effective emission of hydrogen production. Centi et al. [25] proposed that the
method. The reforming reaction in SMR process is strongly endo­ integration of renewable energy in chemical production can effectively
thermic, as shown in Eqs. (1) and (2), requiring extra methane to be replace part of fossil energy. Secondly, the scale and efficiency of electric
burned in the combustion chamber for heating [17]. The burning of hydrogen production can be improved, and the SMR process can also be
methane not only brings significant heat loss but also induces additional optimized. Spagnol et al. [26] proposed using electricity to provide heat
CO2 emission. energy for the reformer in the SMR process. Their experimental studies
showed the size of the reforming reactor could be reduced by the electric
CH4 + H2 O ↔ CO + 3H2 ΔH298 = 206.2 kJ/mol (1)
heating method, and the methane conversion rate reached 80 %. Palma
et al. [27–29] conducted SMR experiments using Joule heating or mi­
CH4 + 2H2 O ↔ CO2 + 4H2 ΔH298 = 164.9 kJ/mol (2)
crowave heated reactors and found that electric heating could enhance
To improve the thermal efficiency of the reformer, some scholars catalyst activity and suppress the polymeric carbon formation. Tang
have done a variety of optimizations on the SMR process. Simpson et al. et al. developed a reactor with hybrid concentrated solar and electric
[18] performed energy and exergy analyses of SMR process and found heat supply for steam methane reforming and found the methane con­
that 42.8 % of exergy loss is caused by combustion in the reformer, and version rate approached the thermodynamic equilibrium of SMR [30].
19 % of exergy loss results from exhaust flue gas. The thermal efficiency Morten et al. [31] introduced induction heating method into the
can reach 71.1 % by optimizing the reactor temperature, pressure, and reformer and found that the catalyst can be heated evenly in this
steam carbon ratio (S/C). Peng [19] optimized the heat exchange pro­ configuration. The methane conversion rate and thermal efficiency can
cess of SMR process through pinch point analysis and obtained a thermal both be improved significantly. Ambrosetti et al. [32] reviewed the
efficiency of 88.82 % for the new process. Lee et al. [20] used artificial study of different electrified SMR technologies and concluded the im­
neural network to optimize the thermal efficiency of SMR system under provements brought by electrification on structural and efficiency of
different working conditions and found that the optimal thermal effi­ reformer. Thirdly, hydrogen produced by natural gas can be mixed into
ciency is 91.26 %, which is higher than that of the original system by the natural gas pipeline network for transportation. Large-scale ac­
8.40 percentage points. In general, the thermal efficiency of SMR pro­ commodation of renewable electricity and long-term energy storage can
cess has reached a bottleneck due to the low efficiency of combustion in be realized at the same time. Wismann et al. [33] conducted experi­
the reformer and the energy carried away by flue gas discharge [18]. mental verification on an electric reformer. The results showed that the
Besides, CO2 emission from SMR process without carbon capture and volume of reformer could be reduced by two orders of magnitude,
storage (CCS) device reaches 9.4–11.4 kg/kg H2 [21]. For the SMR making it easier to achieve wider capacity scale. Another advantage of

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Fig. 1. Process of Conventional SMR (a); Case 1: Process of the E-SMR with electric evaporator(b); Case 2: Process of the E-SMR with HTHP system(c).

electrified SMR is proposed in their study that electrical heating sub­ The electricity-coupled reformer is technically feasible, but the sys­
stantially improved temporal response, pushing start-up times to within tem design of the electricity-coupled SMR process is still blank at pre­
minutes, allowing the process to handle the intermittency of renewable sent. Specifically, the following questions should be answered via the
energy. studies on the SMR process electrification. (1) What are the problems

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Table 1 Table 2
Main parameters and assumptions for process simulation. Main parameters and assumptions for heat pump simulation [45].
Parameters Value Unit Parameters Value Unit Position

Reformer pressure [42] 10 bar Superheat degree of the evaporator 5.0 ◦


C /
Reformer temperature [42] 750–1000 ℃ Subcooling degree of the condenser 5.0 ◦
C
Steam to carbon (S/C) ratio [42,43] 3–5 – Parameters of water/steam
Water pump efficiency [41] 85 % Feedwater inlet temperature 25 ◦
C 1
Isentropic efficiency of Steam and heat pump compressor 83 % Feedwater inlet pressure 1 bar
[41] Feedwater pressurization pressure 4.5 bar 2
Mechanical efficiency of Steam and heat pump compressor 98 % Feedwater evaporation temperature 149.0 ◦
C 4–5
[41] Feedwater evaporation pressure 4.5 bar
Thermal efficiency of reformer 98 % Compressed steam pressure 10 bar 6
Separation rate of PSA [22] 90.9 % Ready steam pressure 10 bar 7
WGS temperature / ◦
C Ready steam temperature 363 ◦
C
WGS pressure 10 bar Parameters of HTHP
Feed natural gas inlet temperature 25 ◦
C Evaporation pressure 7.5 bar 3′
Feed natural gas inlet pressure 10 bar Evaporation temperature 90 ◦
C
HHV of H2 [44] 141.7 MJ/ Condensation pressure 32.0 bar 4′
kg Condensation temperature 163.0 ◦
C
HHV of CO [44] 10.10 MJ/
kg
HHV of CH4 [44] 55.5 MJ/ such as heat pumps, steam compressors, and electric evaporators pro­
kg
vide the heat required in water evaporation. Second, energy analysis is
performed to optimize the proposed E-SMR processes and obtain the
optimal operating parameters. Moreover, the feasibility and economic
performance of the novel process is evaluated by the techno-economic
and sensitivity analyses. This study provides a novel, economical, effi­
cient, green hydrogen production method, and renewable power ac­
commodation scheme, revealing the vital role of E-SMR in the energy
structure transition. E-SMR system may provide abundant hydrogen
sources for application scenarios such as the gas supply chain, synthetic
ammonia industry, and hydrogen refueling stations.

2. Process configuration and modelling

2.1. Process description of E-SMR

The flowchart of conventional SMR is shown in Fig. 1 (a). The feed


natural gas is divided into two parts, one as fuel and the other as the
reactant. Firstly, the reactant part is preheated to 363 ◦ C for refining
desulfurization reaction to eliminate the H2S in natural gas [34]. The
reforming reaction is accomplished by refined natural gas and steam
over a high-temperature catalyst in the reformer. The reaction is endo­
thermic and typically achieved over a nickel-based catalyst operating at
elevated temperatures (630–930 ◦ C) and pressures (5–25 bar) [18].
After cooling down, the outlet gas of the reformer performs a water gas
shift (WGS) reaction. The WGS reaction is exothermic, as shown in Eq.
(3), which occurs at the temperature of approximately 400 ◦ C in the
WGS reactor [35].
CO + H2 O ↔ CO2 + H2 ΔH298 = − 41.1 kJ/mol (3)
The final step in SMR is the separation of the hydrogen from the
syngas exiting the WGS reactor, which includes H2, H2O, CO2, CH4, and
CO. This separation process can be accomplished through several tech­
Fig. 2. The iterative logic diagram of the gas cycle and water flow matching. niques. The most common method is pressure swing adsorption (PSA),
which can separate high purity hydrogen and CO2 (up to > 99 %)
with the SMR process electrification for system integration design, and [18,36]. The separated CO2 can be captured after being compressed.
how to solve them? (2) Is the thermal and economic performance of the Hence the product needs to be cooled before entering in PSA. As shown
SMR process after electrification better than that of the conventional in Fig. 1, H2 product is separated in PSA-A and CO2 is separated in PSA-
hydrogen production process? (3) What are the application scenarios B. Unreacted CH4 and CO are burned for heat demand in the reformer.
and prospects for electrification for the SMR process? From the viewpoint of energy conservation, three challenges are
In this paper, a novel hydrogen production system named electrified presented to electrify the SMR process:
SMR (E-SMR) process is proposed by combining PTG technology with
the conventional SMR process. First, the problems existing in the system (1) The waste heat of flue gas and reaction products is recovered to
integration design of SMR electrification are solved. Two different E- evaporate water in SMR. However, the heat of products is not
SMR configurations are proposed based on the principle of efficient enough to evaporate water in the E-SMR system, the evaporation
electrothermal conversion. Waste heat recovery system is designed energy should be replaced by electricity.
based on cascade utilization principle of energy. Electric equipment

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Fig. 3. Model results and literature values [27] for CH4 conversion (a) and H2 yield(b) (S/C = 3, P = 1 bar).

high temperature heat pump (HTHP) to address the above challenges.


Table 3
Parameters and assumptions for economic analysis. 2.1.1. Case 1- E-SMR with electric evaporator system
Parameters Value Unit E-SMR system with an electric evaporator is named Case 1, of which
Equipment costs the simulation flowchart is shown as Fig. 1 (b). Heat required from water
Specific cost of reformer [46] 76.29 $/kW evaporation is provided from electric evaporator, which can be realized
Specific cost of Sulphur removal unit [47] 52.84 $/kW by using an electrode boiler or resistance boiler. WGS is an exothermic
Cost of PSA unit [46] 0.81 M$ reaction at 400 ◦ C, in which the released heat can be used for the natural
Cost of WGS reactor [46] 0.07 M$
gas preheating. Therefore, a heat exchanger (EX4, flow 1′ -2′ ) is adopted
Electric boiler [48] 54 $/kW
Cost of steam compressor [49] 0.014 M$ in the WGS reactor to absorb the WGS reaction heat. The unreacted CH4
Cost of heat pump [49] 0.051 M$ and CO return to the mixer for cyclic reaction (flow 15), which can
Cost of CO2 compressor [50] 0.15 M$ improve the reaction conversion rate, decarbonize the CH4 that enters
Cost of CO2 storage [50] 22.08 $/t
the system and satisfy the needs of pure hydrogen users. More detailed
Design and engineering 20% of total direct capital
costs of equipment
design considerations are as follows.
Contractor’s fee 5% of total direct capital Case 1 is equipped with three heat exchangers (EX1, EX2, EX3) to
costs of equipment realize the cascade utilization of product waste heat. The preheating
Contingency allowance 5% of total direct capital process of reactants in the mixer outlet (flow 6–7) is performed by
costs of equipment
recovering the heat load of the hot product gas from reformer (flow 8–9)
Fuel costs
Natural gas price [51] 0.373 $/Nm3 in EX1. The exit gas from the WGS reactor (~400 ◦ C, flow 10) is cooled
Electricity price [51] 0.06 $/kWh down to ~ 110 ◦ C (flow 11) by superheating the saturated steam (flow
Operating and maintenance costs 4–5) in EX2 and preheating water to saturation in EX3 (flow 2–3).
Process water (Including waste water treatment) [52] 4.278 $/m3
Finally, the product gas is cooled from ~ 110 ◦ C to 40 ◦ C (flow 13–14) by
Operating labor cost 10% of total production
cost
a cooler to satisfy PSA working temperature.
Direct supervisory and clerical labor costs 10% of operating labor
cost 2.1.2. Case 2-E-SMR with HTHP system
Utilities 10% of total product cost Although three heat exchangers have been set up in Case 1 to recover
Maintenance and repair costs 5% of fixed capital
the waste heat of the product, the exit product temperature of EX3 in
investment
Operating supplies 10% of maintenance and Case 1 is still higher than 100 ◦ C, resulting in a significant waste heat
repair cost loss. HTHP and steam compressor are introduced in the system to
Laboratory charges 10% of operating labor recover more waste heat of the product. The simulation flowchart of the
cost
E-SMR with HTHP system is presented in (c). Different from Case 1, the
Plant-overhead 50% operating labor,
supervision, and
evaporation of water in Case 2 is realized by the HTHP system. The
maintenance costs HTHP comprises the evaporator, condenser, compressor, and expansion
Administrative costs 30% Plant-overhead costs valve. Waste heat is absorbed by the evaporator to evaporate the
Distribution and selling costs 2% of total product cost working fluid at low pressure. The high temperature heat is released in
Research and development costs 2% of total production cost
the condenser from the condensation of the working fluid at high
Operation conditions
Capacity factor (CF) 0.95 pressure. In Case 2, the HTHP absorbs the waste heat from outlet
Inflation [53] 8.78% products (flow 14–15) of EX3 and releases high temperature heat to
Plant lifetime, year [46] 30 saturated water (flow 4–5) to complete the water evaporation.
The evaporation heat of water is provided by the condensation heat
of the working fluid of the heat pump. Hence the condensation tem­
(2) The reactant natural gas in SMR is preheated to 363 ◦ C by
perature of the working fluid should be higher than the evaporation
exhausted flue gas. Therefore, a new heat source for reactant
temperature of the water supply to satisfy the heat transfer re­
preheating should be applied in E-SMR.
quirements. At present, HTHP can provide a heat source up to 160 ◦ C
(3) Since combustion is not used in E-SMR, unreacted CH4 and CO
[37], which corresponds to the saturation water temperature of 150 ◦ C
treatment need to be considered.
(saturation pressure of 4.76 bar) considering the heat exchange tem­
perature difference of 10 ◦ C. However, the pressure of 4.76 bar cannot
This paper proposes two cases by coupling electric evaporator and

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Fig. 4. Effect of S/C and T on the thermal efficiency in Case 1 (a) and Case 2 (b).

Fig. 5. Effect of S/C and Tref on electric efficiency in Case 1 (a) and Case 2 (b).

Fig. 6. Effect of S/C on energy inlet/outlet in Case 1 (a) and Case 2 (b) (Tref = 850 ◦ C) (1 kg H2 production).

satisfy the pressure requirements of the reforming reaction. In this 2.2. Process modelling
paper, 4.5 bar is selected as the evaporation pressure. The water in Case
2 is evaporated by an HTHP and then compressed to reaction pressure by H2 production by E-SMR with different electric devices is proposed
a steam compressor. and modelled by the process simulation software. Reactor modeling in
R1233ZD (E) is selected as the working fluid of the heat pump in this the present study is based on theory of chemical equilibrium. The
system due to its remarkable environmental friendliness (GWP = 1), calculation method is based on the minimization of the Gibbs free en­
Safety (Safety Group: A1), and high temperature adaptability. The ergy, which makes the phase and chemical equilibrium achieved in the
properties of R1233ZD (E) and other widely used HTHP working fluids process without specification of the possible reactions. For the given
are shown in Table 9 (in Appendix A). temperature and pressure, the differential form of the Gibbs free energy
is described in Eq. (4). A more detailed description of the methodology

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Fig. 7. Effect of S/C on electric consumption in Case 1 (a) and Case 2 (b) (Tref = 850 ◦ C).

Table 4
Comparison of E-SMR performance with current SMR research and plants.
Vendor Year Thermal efficiency (HHV, %)

Osaka Gas [55] 2014 79


Air Liquide [56] 2015 75
Case 1 / 92.90
Case 2 / 97.27

Table 5
Comparison of E-SMR performance with water electrolysis technology [57,58].
Vendor Cummins Cummins Case Case
(HySTAT) (HyLYZER) 1 2

Year 2021 2021 / /


Type AEL PEM / /
Electric efficiency (HHV, 72 77.2 74.16 88.68
%)
Electricity consumption 55 51 11.89 9.74
(kWh/kg H2)

Fig. 8. Effect of Tref on electricity consumption in Case 2 (S/C = 3) (1 kg


H2 production).
Table 6
Main results of economic analysis of E-SMR hydrogen plants.
Parameters Unit Case 1 Case 2

with without with without


CCS CCS CCS CCS

Total investment costs M$ 2.34 2.21 2.41 2.28


Fuel Natural gas M$/a 1.76 1.76 1.76 1.76
costs cost
Electricity M$/a 1.17 1.14 0.95 0.92
cost
Total operating costs M$/a 1.20 1.18 1.16 1.13
LCOH $ /kg 2.82 2.65 2.65 2.47
H2

can be found in references [38,39].



N
dG = μi dni (4)
i=1

Physical properties are calculated using Peng–Robinson’s equation


[35], which is particularly suitable for non-polar or mildly polar com­
ponents and mixtures such as hydrocarbons and light gases (e.g., carbon
oxides, hydrogen, methane, etc.). To simplify the model, following as­
Fig. 9. Effect of S/C and Tref on CH4 return ratio. sumptions are proposed in this paper:

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

To verify the reliability of HTHP model, this modeling is compared


with the HTPT with R1233zd working fluids in the reference [45]. As
shown in Table 10 (in Appendix A), the error between the simulated COP
and the reference is less than 0.5%, which indicates that the calculation
of the HTHP model is accurate.

2.4. Performance parameters

With the aim of finding the optimal condition of the E-SMR pro­
cesses, the following performance indices are considered.
(1) Thermal efficiency
Thermal efficiency refers to the ratio of output energy to input en­
ergy in the hydrogen production process, reflecting the overall energy
conversion efficiency of the system. The thermal efficiency is calculated
according to Eq. (5) [43], which represents the ratio of the energy
contained in hydrogen to the total energy inlet, in which the total energy
inlet includes methane energy and electricity.
(qHHV)H2, (qHHV)H2,
Fig. 10. Distribution of different costs of LCOH for E-SMR processes. ηthermal = out
× 100\% = out
× 100\% (5)
ΔHtot (qHHV)CH4,in + Etot

Table 7 where q is the mass flow, kg/s, HHV is the higher heating value, MJ/kg,
Comparison of investment cost and lifetime of E-SMR and electrolytic water Etot is the total electrical energy, MW.
hydrogen production [59]. (2) Electric efficiency
Investment cost, $/kg H2/ Lifetime, year To investigate the storage efficiency of renewable electricity, the
h electrical efficiency is defined as ηE and shown in Eq. (6). Electric effi­
AEL 45000–84000 7–11
ciency is expressed as the ratio of gas chemical energy increment to inlet
PEM 79000–120000 3–7 electric energy. The electrical efficiency is less than 100% because of the
E-SMR equipment (Case 2 with 8772 greater energy loss in electric equipment and the heat loss of the product.
CCS) than30
(qHHV)H2, − (qHHV)CH4,
ηE = out in
× 100\% (6)
Etot
(1) The equipment is adiabatic, and the heat loss at the system
boundary is negligible. Pressure loss in pipelines and hydrogen (3) CO2 emission
production units is negligible [40]. The CO2 emission of the E-SMR processes all comes from hydrogen
(2) The simulations are in a steady state [41]. production reactions. The equation for CO2 emission per unit hydrogen
(3) The reference-environment temperature is 25 ◦ C and the pressure production is as follows:
is 1.013 bar [35]. mco2, out
RCO2 = (7)
(4) The isentropic efficiency of the heat pump compressor and steam mH2, out
compressor is 0.83, and the mechanical efficiency is 0.98 [41].
(5) Carbon deposition in the reactor is not considered [35]. where m is the mass flow rate, kg/s.
(6) Natural gas consists entirely of methane [35]. (3) CH4 return ratio
(7) Due to the low heat of reaction, the desulfurization reaction is not The CH4 return ratio means the proportion of unreacted CH4 back to
considered in modelling [35]. the process, and the equation is shown in Eq. (8).
nCH4,return
Two variable parameters of reforming temperature and steam carbon RCH4 = × 100% (8)
nCH4,in
ratio (S/C) are investigated to find the optimal operation condition of
the E-SMR processes. S/C means the molar ratio of steam to methane.
where nx is the mole flow rate, mol/s.
The ranges of variation for the two parameters are shown in Table 1. (4) Steam carbon ratio (S/C)
As shown in Fig. 1 (b) and Fig. 1 (c), the unreacted CH4 and CO re­
The steam carbon ratio means the molar of H2O to CH4. CH4 contains
turn to the system and react again. This process involves cyclic iterative the inlet part and return part is shown as follows:
calculation. The returned CH4 affects the given S/C condition, and the
feedwater flow rate needs to be changed to match the additional CH4. n H2 O
S/C = (9)
The logic diagram of iterative calculation is shown in Fig. 2. nCH4,in + nCH4,return
Hydrogen production capacity in the simulation is chosen to be 189
kg/h. The main parameters and assumptions used to simulate Case 1 and 3. Economic modelling
Case 2 are summarized in Table 1. The corresponding pressure and
specific parameters are given in Table 2. 3.1. Economic analysis

Detailed cost estimation of the above two E-SMR configurations is


2.3. Model validation conducted to compare their economic performance. The electric
equipment is adopted in two E-SMR systems, which leads to additional
The reactor model validation is proposed to verify the reliability of investment. The levelized cost of hydrogen (LCOH), net present value
the reformer model. The calculated results of CH4 conversion and H2 (NPV), and payback period are selected as the economic performance
yield are compared with reference [27] as shown in Fig. 3, which sug­ indicators, and relevant calculation assumptions can be seen in Table 3.
gests that the reformer model is reliable when temperature is above 700 The equipment cost is estimated by empirical formula and reference cost

C. in the literature. It should be noted that the cost of the electric reformer

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Fig. 11. Sensitivity analyses a) Electricity Price vs LCOH, b) Nature gas Price vs LCOH, c) Carbon tax vs LCOH.

is referred to the cost of the reforming furnace of conventional SMR E-SMR for hydrogen production. Hence, a sensitivity analysis is con­
process. In fact, the size of the electric reformer is much smaller, and the ducted to evaluate the impact of changes in electricity price, natural gas
structure is much simpler. Therefore, the cost of reformer adopted here price and CO2 tax on LCOH.
should be conservative. To evaluate the system profitability, NPV has been calculated ac­
The levelized cost of hydrogen is defined as the ratio of the annual cording to Eq. (13), and different H2 selling prices are used to reflect the
cost to the annual hydrogen output [54], as shown in Eq. (10). profitability performance of the proposed cases.
Ct ∑
n=t
LCOH = (10) NPV =
NCFn
(13)
(CF × 8760) × Pa (1 + r)n
n=1

where Pa is the production capacity, t/h, Ct is the annual cost, $.


where NCF is the net cash flow, $, which is calculated as follows:
Ct = FCF × Ci + Cfuel + CO&M (11)
NCF = Ct − CF × 8760 × Pa (14)
where Ci is the investment cost, $, Cfuel is the cost of fuel, which
includes nature gas cost and all electricity cost, $, CO&M is the operating 4. Results and discussion
and maintenance cost, $, FCF is the fixed charge factor as defined in Eq.
(12). In this section, the effects of reforming temperature and S/C on the
performance of Case 1 and Case 2 were analyzed to find the optimal
r(1 + r)n
FCF = (12) operating conditions and process configurations for the high-efficient
(1 + r)n − 1
hydrogen production. Economic analysis was conducted to evaluate
where n is the economic lifetime of the plant relative to its base year (n the feasibility of the E-SMR processes.
= 30 years), and r is the discount rate, %.
4.1. Performance evaluation of E-SMR
3.2. Economic sensitivity analysis method
4.1.1. Thermal and electric efficiency analysis
It is necessary to find the key parameters and consider their un­ The thermal efficiency of the two Cases under different reforming
certainties that can influence the economic performance of the proposed temperatures and S/C conditions is shown in Fig. 4. The thermal

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Fig. 12. Cumulative discounted cash flow of E-SMR plants under different hydrogen selling prices.

Fig. 13. Application scenarios of E-SMR process in gas supply chain.

efficiency of two cases increases with the decrease of S/C. The thermal (1) S/C analysis
efficiency increases firstly and then decreases with the rise of tempera­ Tref = 850 ◦ C is taken as an example to analyze the variation of en­
ture, and the optimal thermal efficiency is 92.56 % (S/C = 3, Tref = 950 ergy inlet and outlet under different S/C in Fig. 6. Electric energy ac­

C). The change of thermal efficiency of Case 2 with temperature is counts for less than 30 % of the energy input, which greatly reduces the
shown in Fig. 4 (b) and the trend is similar to Case 1. The optimal electric energy input in hydrogen production compared with electrol­
thermal efficiency of Case 2 is 97.27 % (S/C = 3, Tref = 850 ◦ C). ysis. The inlet CH4 and the outlet H2 are stable because of the principle of
The storage efficiency of electricity to chemical energy is illustrated matter conservation, thus the only factor that affects thermal efficiency
by analyzing the electric efficiency as shown in Fig. 5. The trend of is electricity. Fig. 7 illustrates the electricity consumption of various
electric efficiency is the same as that of thermal efficiency. The electric electrical appliances under different S/C. Electricity consumption in
efficiency of Case 2 reaches the maximum when S/C = 3 and the Case 1 is shown in Fig. 7 (a). The power consumption of the electric
reforming temperature is 850 ◦ C (ηE = 88.68 %). Further analysis of the evaporator increases with the increase of S/C, resulting in a sharp
effect of S/C and Tref on efficiency is shown below. decrease in thermal efficiency. As shown in Fig. 7 (b), the steam

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Table 8 4.1.2. Comparison of E-SMR performance


The capacity of E-SMR (Case 2 with CCS) to accommodate renewable energy in The proposed systems are compared with the current advanced SMR
China. and water electrolysis to evaluate the performance of the E-SMR pro­
Unit Value cesses. Table 4 shows the several SMR processes vendors. The compar­
Unit hydrogen production power accommodation kWh/kg H2 10.1
ison results indicate that the thermal efficiency of the system is 18.27
Unit hydrogen production methane accommodation kg/kg H2 2 percentage points higher than the maximum thermal efficiency of SMR
Power accommodation of methane kWh/Nm3 3.6 demonstrated in the available report.
CH4 Table 5 shows the comparison results of the E-SMR processes with
Annual natural gas consumption in China [60] Billion Nm3 328
the water electrolysis process, which includes alkaline electrolysis
Annual hydrogen production with E-SMR in China Million ton/ 117.5
(Convert all methane to hydrogen) year (AEL), polymer electrolyte membrane (PEM) electrolysis, and solid
Annual power accommodation with E-SMR in China Billion kWh/ 1185 oxide electrolysis (SOEL). SOEL is not compared because it is still far
(Convert all methane to hydrogen) year from commercialization due to issues such as service life, scale and cost,
Annual hydrogen production with E-SMR in China Million ton/ 22.4 while AEL and PEM are commercialized for hydrogen production. The
(Convert methane to hydrogen-rich gas mixed with 20% year
hydrogen)
electric efficiency of the E-SMR is at least 11.48 percentage points higher
Annual power accommodation with E-SMR in China Billion kWh/ 225.6 than that of commercial water electrolysis systems currently in opera­
(Convert methane to hydrogen-rich gas mixed with 20% year tion, which indicates that the E-SMR processes are more efficient in
hydrogen) storing electrical energy as chemical energy.
Photovoltaic power installations in China [60] GW 253.6
Wind power installations in China [60] GW 281.7
Annual supply of wind and photovoltaic energy in China Billion kWh 662
4.2. Economic evaluation

E-SMR has no additional carbon emission caused by combustion


Table 9 during hydrogen production compared with SMR process. The CO2
Properties of working fluids for high temperature heat pumps [61].
emission obtained by PSA separation is 5.5 kg/kg H2 and can be com­
Working fluid Unit R1233ZD R245fa R365mfc pressed and stored directly, which brings additional investment costs
(E) (CO2 compressor cost, electricity cost, and CO2 storage cost). Therefore,
Chemical formula / CF3CH = CHF2CH2CF3 CF3-CH2-CF2- four cases of Case 1 (with/without CCS) and Case 2 (with/without CCS)
CHCl CH3 are discussed in the economic analysis.
Group / HCFO HFC HFC
M g/ 130.50 134.05 148.07
mol 4.2.1. Economic analysis
tcr ◦
C 166.5 154 186.9 The operation consumption and capital cost for each hydrogen pro­
pcr bar 37.7 36.5 32.5 duction process option with and without carbon capture are summarized
NBP C 18.3 15.3 40.2
in Table 6. Case 1 has a subtle cost advantage over Case 2 due to its lower

GWP / 1 1030 890


ODP / 0.0002 0 0
equipment cost. However, the electricity cost of Case 1 is 23.15 % and
Safety group (ASHRAE / A1 B1 A2 23.91 %, respectively, higher than that of Case 2 with and without CCS,
Standards) respectively. Hence, Case 2 without CCS has the lowest LCOH (2.47 $/kg
H2). The cost details are listed in Table 11 (in Appendix B).
Fig. 10 shows the LCOH and its cost composition in two Cases. The
compressor consumes significantly more energy than the pump used in
fuel cost accounts for more than 60 % of the total cost in all four Cases,
Case 1, while using HTHP can bring more waste heat recovery so that the
which reflects that fuel prices obviously have a massive impact on the
electricity consumption of Case 2 is lower than Case 1. In addition, it can
cost of hydrogen production. It also can be concluded that the system
be concluded that the increase of S/C leads to the increase of energy
with CCS reduces CO2 emission from 5.5 kg/kg H2 to zero, and its lowest
consumption on water evaporation and thus the decrease of efficiency.
LCOH is 2.65 $/ kg H2. Table 7 compares the investment cost and life­
(2) Temperature analysis
time of E-SMR and water electrolysis. It proves that the investment cost
S/C = 3 is taken as an example to analyze the change of the thermal
of E-SMR is much lower than that of electrolytic water. Electric heating
efficiency as shown in Fig. 8. The increase in thermal efficiency is due to
is used in E-SMR process and the body of reformer is heated evenly.
the reduction in energy consumption of HTHP and steam compressor.
Thus, the lifetime can be longer than the SMR plant (30 years), which
The reason can be further analyzed in Fig. 9, which depicts the CH4
uses combustion as the heat resource.
return ratio curve in Case 1 and Case 2. The temperature decrease pre­
vents the reforming reaction and increases the CH4 return ratio. Ac­
4.2.2. Economic sensitive analysis
cording to the definition of S/C, the molar flow of water increases with
As described in Section 4.2.2, fuel prices impact dramatically on the
the increase of returned CH4, resulting in the increase of water evapo­
economics of the process. In addition, in the general trend of carbon
ration energy consumption. The promotion of the reaction is not
emission reduction, the carbon tax is important in industrial production,
apparent when the temperature continues to rise, while the reformer has
which can be used to evaluate the economy of installing CCS in this
more efficiency loss and the product takes away more waste heat so that
process. Hence, a sensitivity analysis including the effects of uncertainty
the thermal efficiency declines.
in the fuel prices and CO2 tax on the LCOH is conducted to investigate
the economic performance of E-SMR processes.

Table 10
Model results and literature values [45] for COP of HTPT with R1233zd as the working fluid.
t0 tk p0 pk ε qk Ecomp COP COPref Error

30 110 1.54 12.90 8.38 76.19 26.19 2.9092 2.9164 − 0.2479%


40 120 2.15 15.75 7.33 76.50 26.51 2.8857 2.8818 0.1352%
50 130 2.93 19.80 6.76 76.80 27.09 2.8351 2.8369 − 0.0617%
60 140 3.90 23.00 5.90 78.63 28.64 2.7455 2.7388 0.2448%
70 150 5.10 25.70 5.04 80.30 30.33 2.6474 2.6367 0.4062%

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

Table 11 Table 12
Main results of economic analysis of E-SMR hydrogen plants. The capacity of E-SMR (Case 2 with CCS) to accommodate renewable energy in
Parameters Unit Case 1 Case 2
Japan, the United States, and Europe.
Unit Value
with without with without
CCS CCS CCS CCS Annual natural gas consumption in Japan [62] Billion Nm3 107.8
Annual hydrogen production with E-SMR in Japan Million ton/ 38.6
Investment costs
(Convert all methane to hydrogen) year
Specific cost of reformer M$ 0.48 0.48 0.48 0.48
Annual power accommodation with E-SMR in Japan Billion kWh/ 389
Specific cost of Sulphur M$ 0.33 0.33 0.33 0.33
(Convert all methane to hydrogen) year
removal unit
Annual hydrogen production with E-SMR in Japan Million ton/ 7.4
Cost of PSA unit M$ 0.81 0.81 0.81 0.81
(Convert methane to hydrogen-rich gas mixed with 20% year
Cost of WGS reactor M$ 0.07 0.07 0.07 0.07
hydrogen)
Cost of steam compressor M$ / / 0.01 0.01
Annual power accommodation with E-SMR in Japan Billion kWh/ 74.2
Electric boiler M$ 0.03 0.03 / /
(Convert methane to hydrogen-rich gas mixed with 20% year
Cost of heat pump M$ / / 0.05 0.05
hydrogen)
Cost of CO2 compressor M$ 0.15 / 0.15 /
Photovoltaic power installations in Japan [63] GW 67
Design and engineering M$ 0.37 0.34 0.35 0.35
Wind power installations in Japan [63] GW 4.2
Contractor’s fee M$ 0.09 0.09 0.09 0.09
Annual supply of wind and photovoltaic energy in Japan Billion kWh 105
Contingency allowance M$ 0.09 0.09 0.09 0.09
Annual natural gas consumption in USA [63] Billion Nm3 754
Total capital costs M$ 2.34 2.21 2.41 2.28
Annual hydrogen production with E-SMR in the USA Million ton/ 269.9
Fuel costs
(Convert all methane to hydrogen) year
Natural gas price M$/a 1.76 1.76 1.76 1.76
Annual power accommodation with E-SMR in the USA Billion kWh/ 2722
Electricity price M$/a 1.17 1.14 0.95 0.92
(Convert all methane to hydrogen) year
Operating and maintenance costs
Annual hydrogen production with E-SMR in the USA Million ton/ 51.4
Process water (Including M$/a 0.06 0.06 0.06 0.06
(Convert methane to hydrogen-rich gas mixed with 20% year
waste water treatment)
hydrogen)
Cost of CO2 storage M$/a 0.19 / 0.19 /
Annual power accommodation with E-SMR in the USA Billion kWh/ 518.5
Operating labor cost M$/a 0.28 0.28 0.27 0.26
(Convert methane to hydrogen-rich gas mixed with 20% year
Direct supervisory and M$/a 0.03 0.03 0.03 0.03
hydrogen)
clerical labor costs
Photovoltaic power installations in USA [63] GW 73.8
Utilities M$/a 0.28 0.28 0.27 0.26
Wind power installations in USA [63] GW 117.7
Maintenance and repair M$/a 0.12 0.11 0.12 0.11
Annual supply of wind and photovoltaic energy in USA Billion kWh 228.4
costs
[63]
Operating supplies M$/a 0.01 0.01 0.01 0.01
Annual natural gas consumption in Europe [63] Billion Nm3 490
Laboratory charges M$/a 0.03 0.03 0.03 0.03
Annual hydrogen production with E-SMR in Europe Million ton/ 175.5
Plant-overhead M$/a 0.21 0.21 0.21 0.20
(Convert all methane to hydrogen) year
Administrative costs M$/a 0.06 0.06 0.06 0.06
Annual power accommodation with E-SMR in Europe Billion kWh/ 1770
Distribution and selling M$/a 0.06 0.06 0.05 0.05
(Convert all methane to hydrogen) year
costs
Annual hydrogen production with E-SMR in Europe Million ton/ 33.4
Research and M$/a 0.06 0.06 0.05 0.05
(Convert methane to hydrogen-rich gas mixed with 20% year
development costs
hydrogen)
Total operating costs M$/a 1.20 1.18 1.16 1.13
Annual power accommodation with E-SMR in Europe Billion kWh/ 371.5
LCOH $ /kg 2.82 2.65 2.65 2.47
(Convert methane to hydrogen-rich gas mixed with 20% year
H2
hydrogen)
Photovoltaic power installations in Europe [63] GW 167.8
Wind power installations in Europe [63] GW 216.6
As illustrated in Fig. 11 (a), the lowest LCOH of E-SMR is 2.7 $/kg H2 Annual supply of wind and photovoltaic energy in Europe Billion kWh 468.3
under the current electricity price in China (0.084 $/kWh). While the [63]
application of this system is to accommodate surplus renewable electric
energy, in which the price of electricity can be regarded as zero.
Accordingly, the LCOH of Case 2 (without CCS) is as low as 1.89 $/kg H2. reach 12.28 M$ in 30 years.
Fig. 11 (b) shows the sensitivity analysis of LCOH to natural gas
price. It is evident that current natural gas price in China is relatively 5. Application prospects
high (0.373 $/Nm3), therefore, this process is more economical in areas
with a lower natural gas price. The influence of carbon tax on the LCOH, 5.1. Application in gas supply chain
shown in Fig. 11 (c), manifests that systems with CCS are immune to by
carbon taxes by reason of the characteristic of their zero CO2 emission. The excellent performances in energy, environmental, and economic
When carbon tax exceeds 32.4 $/ton CO2, Case2 (with CCS) costs is less aspects of the E-SMR process are verified in the above discussion.
than that of Case 2 (without CCS) and becomes the most economical Therefore, this process may play an important role in gas production and
hydrogen production process. supply.
Discounted cash flow analysis is an important technique to convert Fig. 13 shows the possible application scenarios of E-SMR equipment
the net future cash flows of the project into NPV, which indicates the in both gas supply end and gas consumption areas. Generally, areas with
resources required and the time to give a profit. Fig. 12 displays the rich natural gas resources are far from gas-consuming areas in most
cumulative discounted cash flow of proposed E-SMR processes with the cases. Therefore, E-SMR equipment can be used in gas supply areas to
hydrogen selling price of 2.8, 3.0, and 3.2 $/kg H2. Case 1 (with CCS) is reform part of natural gas into hydrogen, and hydrogen can be mixed
difficult to achieve profit with 2.8 $/kg H2, while Case 2 (with CCS) has into natural gas pipelines to produce the H2-rich gas. Several advantages
a payback period of 7.5 years. Case 2 (without CCS) has the shortest of this method of hydrogen transport could be summarized as follows.
payback period due to low fuel costs, as shown in Fig. 12. Fig. 12 (b) First, the reuse of natural gas infrastructure can reduce the initial capital
shows that all E-SMR processes are profitable with a payback period of investment and facilitate the transformation of large and medium-sized
within 10 years at the hydrogen price of 3.0 $/kg H2. Fig. 12 (c) shows oil and gas companies. Second, the natural gas pipeline network is
that all the cases proposed have considerable economic benefits when installed in a wide range, which facilitates long-distance hydrogen
the hydrogen price is 3.2 $/kg H2, especially Case 2 (without CCS), transportation and significantly reduces transportation costs. At the
which can realize investment recovery in 2.6 years and whose NPV can same time, the natural gas pipeline allows fluctuations in the proportion

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H. Song et al. Energy Conversion and Management 258 (2022) 115513

of hydrogen mixing, which perfectly fits the characteristics of the 3) Sensitivity analysis shows that electricity and methane as fuel greatly
volatility of renewable energy power generation. Many countries have influence the cost of the E-SMR process. The price of electricity can
tried mixing hydrogen in natural gas pipelines and implemented several be regarded as zero when the application of E-SMR is to accommo­
pilot demonstration projects mentioned before. This process can date the surplus renewable electric energy. The LCOH of Case 2
accommodate renewable energy from the area and inject captured CO2 (without CCS) is as low as 1.89 $/kg H2. Configurations with CCS are
into the oil well to enhance oil recovery. The hydrogen-rich gas reaches more economical when the carbon tax is higher than 32.4 $/ton CO2.
the urban gas station through the natural gas pipelines. The E-SMR When the hydrogen price is 3.2 $/kg, Case 2 (without CCS) invest­
equipment can be arranged in the gas station to convert part of the H2- ment can be recovered within 2.6 years. In the lifespan of 30 years,
rich gas to hydrogen. Then the produced hydrogen can be sent to the the net present value of this design is 12.28 M$.
hydrogenation station, or ammonia plant, or mixed into the urban gas 4) This paper proposed the application scenarios of the E-SMR process
pipelines to supply high hydrogen-rich gas. The CO2 produced during in the natural gas supply chain. First, E-SMR uses natural gas and
the process can be stored in CO2 tanks and geological reservoirs or used surplus renewable electricity to generate hydrogen and passes it into
for industrial CO2 utilization. E-SMR equipment helps decarbonize the natural gas pipeline in the gas supply area, which can realize
natural gas while achieving large-scale accommodation of renewable large-scale renewable energy storage and hydrogen transportation.
energy and large-scale transmission of hydrogen, providing a solution E-SMR at the gas consumption area can provide hydrogen for gas
for global green energy transition and carbon neutrality. users, reduce the carbon emission of gas and accommodate renew­
able electricity.

5.2. Capacity estimation of application


CRediT authorship contribution statement
The popularization of this technology could contribute to hydrogen
supply, transportation, and renewable energy consumption. The Huchao Song: Writing – original draft, Data curation, Investigation,
renewable energy accommodation capacity and hydrogen production Validation, Methodology, Software. Yinhe Liu: Writing – review &
capacity can be achieved in China with E-SMR is displayed in Table 8, editing, Conceptualization, Methodology, Resources, Supervision. Hao
and that of Japan, the United States, and Europe are estimated in Bian: Writing – review & editing, Visualization. Mengfei Shen: Writing
Table 12 (in Appendix C). The annual wind power generation is calcu­ – review & editing, Software. Xiaolong Lin: Writing – review & editing,
lated according to the installed capacity of 1500 h, and photovoltaic Investigation.
power generation is calculated according to the installed capacity of
1000 h. The results show that this technology can achieve large-scale Declaration of Competing Interest
renewable energy accommodation and produce considerable hydrogen
in various countries and regions. The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
6. Conclusions the work reported in this paper.

In this paper, a novel hydrogen production system called E-SMR was Acknowledgements
proposed by combining PTG technology with SMR. Renewable electric
energy was introduced into SMR process through the electric reformer, This work was supported by the Key Research and Development Plan
electric evaporator, and high temperature heat pump. Two E-SMR of Shaanxi Province (No. 2021GXLH-Z-088).
configurations (Case1 and Case2) were put forward and analyzed. Case 1
is integrated with an electric evaporator, and Case 2 is combined with a Appendix A
high temperature heat pump and a steam compressor. Energy analysis
was performed in this paper to evaluate and optimize the performance of
the proposed processes. The techno-economic and sensitivity analyses
were carried out to assess the economic performance of the E-SMR Appendix B
processes. Simulation results highlighted that the high temperature heat
pump in Case 2 could recover more waste heat of production and
evaporate water efficiently, making the energy consumption of Case 2
lower and the efficiency higher than Case 1. Meanwhile, economic Appendix C
analysis shows that Case 2 has a shorter payback period and higher NPV.
The following conclusions have been drawn:

1) In Case 2, the optimal thermal efficiency is 97.27 % (S/C = 3, Tref = References


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