Energy Conversion and Management 198 (2019) 111927

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Energy Conversion and Management

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

Thermodynamic and environmental analysis of integrated supercritical T

water gasification of coal for power and hydrogen production
Jingwei Chena,c, Wenwen Xua, Feng Zhanga,c, Hongyan Zuob, , Jiaqiang Ea,c, , Kexiang Weib,
⁎ ⁎

Gaoliang Liaoa,c, Yi Fana

a
College of Mechanical and Vehicle Engineering, Hunan University, Changsha 410082, China
b
Hunan Provincial Key Laboratory of Vehicle Power and Transmission System, Hunan Institute of Engineering, Xiangtan 411104, China
c
Institute of New Energy and Energy-Saving & Emission-Reduction Technology, Hunan University, Changsha 410082, China

ARTICLE INFO ABSTRACT

Keywords: Coal combustion for thermal power generation causes serious environmental problems. Relatively efficient and
Coal clean coal utilization technologies need to be developed to alleviate the growing energy crisis and environmental
Supercritical water gasification pollution pressure. A novel integrated supercritical water gasification of coal system with 40 t/h throughput of
Power and hydrogen production coal and water was designed. A thermodynamic analysis and a life cycle environmental assessment under dif-
Thermodynamic analysis
ferent conditions were performed using Aspen Plus 8.4 and SimaPro 9.0 based on the Ecoinvent 3 database,
Life cycle assessment
respectively. Results show that the maximum energy loss is induced by the waste heat of the effluent from the
heat exchanger. By using organic Rankine cycle, the energy efficiency of the system could reach 53.3% when the
temperature and coal concentration are 700 °C and 15 wt%, respectively. The global warming potential, acid-
ification potential and nitrogen oxides are 0.058 kg carbon dioxide eq/(kW·h), 3.63 × 10−4 kg sulfur dioxide eq/
(kW·h) and 7.04 × 10−5 nitrogen oxides eq/(kW·h), respectively, for the process combined with carbon dioxide
capture and storage under the temperature of 700 °C and the coal concentration of 15 wt%. The comparison of
the thermodynamic and environmental performance among different systems shows that the exergy and energy
efficiencies of integrated supercritical water gasification of coal system combined with organic Rankine cycle are
higher than those of integrated gasification combined cycle, and the environmental emissions of the integrated
supercritical water gasification of coal system are less than those of integrated gasification combined cycle
system. This study reveals that the integrated supercritical water gasification of coal is a relatively clean and
efficient coal utilization technology with good industrialization prospects.

1. Introduction resources, environmental pollution is becoming more and more serious

Coal is currently an important fuel for thermal power generation
[1]. During the operation of the conventional coal-fired power plant,
large amounts of nitrogen oxides (NOx), sulfur dioxide (SO2), carbon
dioxide (CO2), heavy metals and particulate matter 2.5 (PM 2.5)
emissions are released [2]. This situation causes serious environmental
problems including acid deposition, air pollution and global climate
change [3]. Approximately half of carbon dioxide emissions, 90% of
SO2 emissions, 70% of dust emissions and 67% of NOx emissions in the
world are caused by coal combustion [4]. However, coal demand is
expected to rise over the next 10 years [5]. In 2012, the global coal
consumption was 3.8 billion tons and it is expected to reach 4.6 billion
tons by 2030, of which 2.8 billion tons will be used for power gen-
eration [6]. With the extensive exploitation and utilization of coal
[7]. Therefore, it is urgent to develop relatively clean and efficient coal
conversion and utilization technologies.
A promising option for coal conversion and utilization is the
emerging supercritical water gasification (SCWG) technology, which
has some advantages over traditional thermochemical pathways. Based
on the previous studies, the advantages of SCWG can be concluded as
follows: (1) Sulfur (S), nitrogen (N), phosphorus (P), mercury (Hg),
arsenic (As) and other elements in supercritical water deposit as in-
organic salts. Therefore, almost no NOx and sulfur oxides (SOx) are
released during gasification process [8]. (2) Complete gasification can
be achieved at lower temperatures (approximately 500–700 °C), com-
pared with the coal gasification technology (approximately 1200 °C)
[9]. (3) Supercritical water acts as the reactant, solvent, and catalyst,
which can inhibit the formation of the tar and coke. Therefore, the

⁎
Corresponding authors at: College of Mechanical and Vehicle Engineering, Hunan University, Changsha 410082, China (J. Jiaqiang).
E-mail addresses: zuohongyan18@126.com (H. Zuo), ejiaqiang@hnu.edu.cn (J. E).

https://doi.org/10.1016/j.enconman.2019.111927
Received 30 June 2019; Received in revised form 5 August 2019; Accepted 7 August 2019
Available online 27 August 2019
0196-8904/ © 2019 Elsevier Ltd. All rights reserved.
J. Chen, et al.
Nomenclature
Abbreviations
SCWG supercritical water gasification
ISCWGC-HPP integrated supercritical water gasification of coal for
power and hydrogen production
CCS carbon dioxide capture and storage
PSA pressure swing adsorption
LCA life cycle assessment
FU functional unit
GWP global warming potential
carbon conversion efficiency can be greatly increased [10]. (4) CO2 can
be separated from the gaseous products by using high-pressure gas-li-
quid separator [11] to obtain a hydrogen-rich combustible gas which
can be used to provide heat for the SCWG reaction and gas turbine for
electricity generation. In addition, supercritical water from the SCWG
reactor can be used to drive the steam turbine to generate electricity.
On the basis of the abovementioned considerations, Guo et al. [12]
proposed a hydrogen production and power generation system based on
coal gasification in supercritical water. The integrated supercritical
water gasification of coal for power and hydrogen production
(ISCWGC-HPP) is a high-efficiency multi-generation coal conversion
system that can produce clean hydrogen-rich syngas, electricity and
high temperature steam simultaneously. However, the thermodynamic
and environmental analysis on the ISCWGC-HPP, which is the first step
to evaluate the prospects of a new technology, has not been reported
yet.
The thermodynamic analysis provides a chance for system optimi-
zation from the energy aspects [13]. Many researchers have conducted
thermodynamic analysis on SCWG technology [14]. Guo et al. [12]
analyzed the thermodynamic performance of coal SCWG under dif-
ferent concentrations, pressures and temperatures. Aziz [15] proposed
an innovative integration system of SCWG and power generation for
microalgae utilization. Simulations revealed that the total energy effi-
ciency of the proposed integrated processes exceeded 40%. Rahbari
et al. [16] performed an energy and exergy analysis of concentrated
Fig. 1. Flow sheet of the ISCWGC-HPP system in Aspen Plus.
2
Energy Conversion and Management 198 (2019) 111927
ADP non-bio-effective potential
AP acidification potential
EP eutrophication potential
CGE carbon gasification efficiency
LHV low heating value
IGCC Integrated gasification combined cycle
NGCC natural gas combined cycle
Symbols
ηen energy efficiency, %
ηex exergy efficiency, %
solar supercritical water gasification of algal biomass by using Aspen
Plus. The results showed that the optimal exergy efficiency (45%) fa-
vored high pumped algae concentration of nearly 25%. Gutiérrez et al.
[17] conducted an energy and exergy analysis of the supercritical water
reforming of glycerol for power production with the aid of Aspen Plus.
A sensitivity analysis was carried out to identify optimal conditions for
maximizing power production.
The analysis of potential environmental impacts is another im-
portant approach to evaluate the future of ISCWGC-HPP technology.
Detailed quantitative analysis of environmental impacts can be con-
ducted through life cycle assessment (LCA) [18]. LCA is a tool for as-
sessing potential environmental impacts throughout the life cycle [19].
LCA can quantify the impact of products or services on different en-
vironmental categories and identify product opportunities to improve
environmental impacts in their life cycle [20]. Kikuchi et al. [21] elu-
cidated the environmental aspects of spray incineration and super-
critical water oxidation processes by LCA. Chen et al. [22] conducted an
LCA of a pilot plant of SCWG heated by concentrated energy to evaluate
the environmental performance of the system. Galera and Gutiérrez
[23] used LCA to investigate the environmental emissions of a system of
supercritical water reforming of glycerol for hydrogen and electricity
production. The research showed that supercritical water reforming is a
good option to produce hydrogen with a global warming potential
(GWP) of only 3.77 kg CO2-eq/kg H2. However, the LCA of ISCWGC-
HPP system has not been studied to date.
J. Chen, et al.
This study aims to investigate the thermodynamic performance with
Aspen Plus and the life cycle environmental impacts of a novel
ISCWGC-HPP system with Simapro to determine the practical prospects
and challenges of the ISCWGC-HPP technology. Nowadays, the eva-
luation and optimization analysis of the ISCWGC-HPP system has not
been conducted in terms of thermodynamic and environmental per-
formance. Thus, this work aims to fill in the research gaps mentioned
above. The novelties and objectives of this study are listed as follows:
(1) A novel ISCWGC-HPP system is designed and modeled with Aspen
Plus.
(2) The thermodynamic performance of ISCWGC-HPP system is eval-
uated through Aspen Plus. Organic Rankine cycle (ORC) is used as a
bottoming cycle to enhance the thermodynamic efficiency of the
system.
(3) The life cycle environmental impacts of the ISCWGC-HPP system
are evaluated to determine the primary environmental burden.
(4) The thermodynamic and environmental performance of ISCWGC-
HPP process is compared with those of other coal conversion
technologies, and the practical application prospects and challenges
of ISCWGC-HPP technology are put forward.
2. Methods
In this section, a novel pilot-scale ISCWGC-HPP system is designed,
and the ISCWGC-HPP system is modelled with Aspen Plus 8.4.
Additionally, the thermodynamic analysis and LCA process are de-
scribed.
2.1. Engineering design
Fig. 1 shows the basic flowchart of ISCWGC-HPP system, including
equipment, raw materials and energy inputs, output products and
production processes. Firstly, the coal (S2) and water are mixed into a
coal slurry. Secondly, pure water (S1) and the coal slurry are pumped to
heat exchanger (HX1) by PUMP1 and PUMP2, respectively. Then the
water and coal slurry are preheated in HX1 and sent to the heat ex-
changer (HX2) and SCWG reactor, respectively. The water is further
heated in the HX2 by the hot flue gas from the furnace, and then heated
by a preheater in the furnace. Thirdly, the coal slurry is mixed with
preheated supercritical water in the SCWG reactor which is heated by
the natural gas furnace. The temperature and pressure of SCWG reactor
and preheater are designed to 600–700 °C and 25 MPa. The designed
total flow rate of the coal slurry and the preheated water are 10 and
30 t/h, respectively. Fourthly, the coal is gasified in the SCWG reactor,
and hydrogen-rich syngas is produced. The solid residues (ash) are se-
parated from the reactor. Fifthly, the effluent from the SCWG reactor
drives the turbine to generate power. The pressure of the exhausted
steam is reduced to 1.5 MPa after power generation, and the heat of the
exhausted steam from the turbine is successively transferred to the
preheated water and coal slurry through the heat exchanger (HX1).
Sixthly, the effluent from HX1 is cooled by the cooler and entered to the
separators. In the high-pressure separator, most of the hydrogen is se-
parated from the fluid and hydrogen-rich syngas is further purified by
pressure swing adsorption (PSA) to collect hydrogen with a purity of
Table 1
Analysis data of coal feedstock being used.
Coal type Elemental Analysis (wt%)
a
C H N O S M
Yimin Lignite 40.5 3.25 0.57 21.43 0.19
a
Difference.
3
Energy Conversion and Management 198 (2019) 111927
over 99%. The remaining combustible gas is fed into the gas furnace to
heat the preheater and SCWG reactor together with natural gas. The
compressed air is used as the oxidant in the furnace. Finally, the liquid
from the high-pressure separator is transferred to the low-pressure gas-
liquid separator. The CO2 rich gas is separated from water and CO2 is
collected and trapped by CCS. Water is recycled to the ISCWGC-HPP
system.
2.2. Process modeling method
The kind of coal used in this study is Yimin lignite, and Table 1
shows the properties of this coal [12]. Coal is not a standard material in
the material database of Aspen Plus, thus the simulation of SCWG
cannot be conducted in a single reactor. A virtual process is introduced
to simulate the SCWG reactor for solving the aforementioned problem
[24]. As shown in Fig. 1, a RYIELD module is used to simulate the
pyrolysis process of coal, and the coal is converted to simple com-
pounds (carbon (C), S, nitrogen (N2), hydrogen (H2), oxygen (O2) and
ash) in the RYIELD reactor (shown as Decomp in Fig. 1). A separator
(SEP-P) is then used to separate the ash produced in the RYIELD re-
actor. The other compounds are transported to a RGIBBS reactor, where
supercritical water is used as a gasification medium to react with pyr-
olysis products. The thermodynamic equilibrium of coal SCWG is si-
mulated by RGIBBS module based on Gibbs free energy minimization
method together with the Peng-Robinson equation of state with Boston-
Mathias alpha function (PR-BM) attribute method. The PR-BM method
has been proven by several researchers to be reliable in the thermo-
dynamic simulation of organic waste [24] and biomass gasification in
supercritical water [25]. The gaseous products are assumed to be H2,
CO2, methane (CH4), and carbon monoxide (CO), which are the main
gaseous products in the experiments [12]. In addition, system power
consumption is completely self-sufficient. The properties of water come
from the database created by IAPWS in 1997 [26]. An Aspen flash re-
actor mode based on the UNIF-DMD method is applied to model the
phase equilibrium in the gas liquid separator (SEP). Furthermore, the
activity coefficient and fugacity of the gas and liquid phases are cal-
culated by the Soavee-Redliche-Kwong equation of state and the
UNIFAC model, respectively. Table 2 summarizes the method and as-
sumptions for the main units of the ISCWGC-HPP system.
2.3. Thermodynamic analysis method
Energy and exergy analyses are conducted to evaluate the thermo-
dynamic efficiency of the ISCWGC-HPP system and find the system
optimization method from the energy aspects.
2.3.1. Energy analysis
The energy conversion efficiency ηen is used to evaluate the energy
performance of the ISCWGC-HPP system. ηen is calculated using Eqs.
(1)–(6). Natural gas is used in this study as the furnace fuel. The main
component of natural gas is methane. Therefore, the natural gas is
treated as methane for calculating natural gas energy.
Eout
= × 100%
en
Ein (1)
Proximate analysis (wt%) Calorific Value (MJ/kg)
A V FC
18.42 15.64 32.21 33.73 16.607
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

Table 2
Modeling method and assumptions of the main units.
Unit Type Methods and Assumptions

Pump Mechanical efficiency: 0.9; Outlet pressure: 25 MPa

Heat Exchanger HX1, HX2, HX3 Minimum temperature approach: 10 °C
SCWG Reactor RYIELD and RGIBBS Thermodynamic equilibrium, Operating temperature: 600 °C/650 °C/700 °C
Turbine Mechanical and isentropic efficiencies: 0.9 and 0.9
Furnace RSTOIC Combustion of combustible gaseous products and natural gas; Operating temperature: 1000 °C
PSA Pressure swing adsorption Recovery ratio of hydrogen: 95%
Compressor COMP1, COMP2 Isentropic efficiency: 0.72
Separator SEP Phase equilibrium

Eout = E H2 + Eelec (2) H

= 1.0438 + 0.0158 C + 0.0813 C ,
O O
for C 0.5;
Ein = Ecoal + ENG + EP (3) =
1.0414 + 0.0177(H / C ) 0.3328(O / C )[1 + 0.0537(H / C )]
, for 0.5<
O
2.0
1 0.4021(O / C ) C (12)
E H2 = MH2 × Q H2 (4) The exergy conversion efficiency ηex is used to evaluate the exergy
performance of ISCWGC-HPP. The ηex is calculated by the Eqs.
Ecoal = Mcoal × Qcoal (5)
(13)–(18):
ENG = MNG × QNG (6) Ex, out
ex = × 100%
−1 −1
where Ein (kJ·h ) and Eout (kJ·h ) are the energy input and energy
Ex , in (13)
output, respectively; ΕH2 (kJ·h−1), Εcoal (kJ·h−1) and ΕNG (kJ·h−1) re- Ex, out = Ex, H2 + Eelec (14)
present the lower heating value of hydrogen produced, coal and natural
gas, respectively; ΕP is the power consumed by the system (kJ·h−1); Ex, in = Ex , coal + Ex , NG + EP (15)
Εelec is the power generated by the system (kJ·h−1); MH2, Mcoal and MNG
Ex, H2 = MH2 × ex, H2 (16)
are the mass flow of H2, coal and natural gas (kg·h−1), respectively; QH2
and Qcoal and QNG are the low calorific value per kilogram of 120.8 kJ/ Ex , coal = Mcoal × ex , coal (17)
kg, 16607 kJ/kg and 50.12 kJ/kg for hydrogen, coal and natural gas,
respectively. Ex, NG = MNG × ex, NG (18)
−1 −1
where Ex,in (kJ·h ) and Ex,out (kJ·h ) are the exergy input and exergy
2.3.2. Exergy analysis output; Εx,H2 (kJ·h−1), Εx,coal (kJ·h−1) and Εx,NG (kJ·h−1) represent the
The exergy of hydrogen and methane is calculated by Eq. (7). The exergy hydrogen produced, coal and natural gas, respectively; MH2,
exergy of methane and hydrogen covers four exergy types [27]. Mcoal and MNG are the mass flow of H2, coal and natural gas (kg·h−1),
respectively; ex,H2, ex,coal and ex,NG is the exergy per kilogram of hy-
ex , gas = ex, gas ki + ex, gas po + ex, gas ph + ex, gas ch (7)
drogen, coal and natural gas (kJ·kg−1).
where ex,gas is exergy of gas (CH4 or H2), kJ/kg; ex,gaski
is kinetic exergy
of gas (CH4 or H2), kJ/kg; ex,gaspo is potential exergy of gas (CH4 or H2), 2.4. Life cycle assessment method
kJ/kg; ex,gasph is physical exergy of gas (CH4 or H2), kJ/kg; ex,gasch is
chemical exergy of gas (CH4 or H2), kJ/kg. The LCA method is a powerful internationally recognized tool for
Potential exergy and kinetic exergy are so small that they can be studying the environmental and potential impacts of a product or ser-
neglected [28]. Eq. (7) results in: vice system throughout its life cycle [33]. In this study, the LCA method
is applied to analyze the environmental emissions during the operation
ex , gas = ex, gas ph + ex, gas ch (8) phase of the ISCWGC-HPP system. The goal of LCA is to examine the net
The physical exergy of gas (CH4 or H2) is calculated by Eq. (9) [29]: emissions of greenhouse gases and other major environmental con-
sequences. The LCA includes three steps. Firstly, the system boundary is
ex , gas ph = n [(h h0) T0 (s s0 )] (9) defined. Secondly, data on the input and output of materials and energy
within the system boundaries are collected as a detailed life cycle in-
where n is molar yield of gas (CH4 or H2), kmol/kg; h is specific en- ventory. Thirdly, the environmental impacts related to mass and energy
thalpy of gas (CH4 or H2) at arbitrary temperatures (kJ/kmol); h0 is flows are assessed on the basis of the inventory data.
specific enthalpy of gas (CH4 or H2) in the environment (8121 kJ/kmol
or 8468 kJ/kmol [30]); T0 is environmental temperature (298.15 K); s is
2.4.1. Goal and scope definition
specific entropy of gas (CH4 or H2) at arbitrary temperatures (kJ/
Fig. 2 defines the system boundary, which is to specify the pro-
(kmol·K)); s0 is specific entropy of gas (CH4 or H2) in the environment
duction process as well as the inputs and outputs within the selected
(186.251 kJ/(kmol·K) or 130.574 kJ/(kmol·K) [30]).
boundaries. Notably, only the system operation phase is considered,
The chemical exergy of gas (CH4 or H2) is expressed as follow [29]:
whereas the impact of the construction and demolition phases is ne-
ex , gas ch = nex, n, gas ch (10) glected. The operation of the ISCWGC-HPP system includes the mining,
collection and transport of coal; hydrogen production through SCWG of
where ex,n,gasch
is standard chemical exergy of gas (CH4 or H2) coal; high-pressure transport of coal and water; power generation; gas
(831,650 kJ/kmol for CH4 and 236,100 kJ/kmol for H2 [31]). furnace heating; and separation and purification of gas products.
The statistical correlation of Szargut and Styrylska [32] is applied to The basic functional unit (FU) in this study is 1 kW·h of net power
calculate the chemical exergy of the coal ex,coal (kJ/kg): output. All emissions, materials, energy consumption and transporta-
tion are based on this FU to provide a common basis for comparing the
ex , coal = LHVcoal (11)
systems studied in this paper. The system consists of the coal slurry
With preparation unit, gasification unit, power generation unit, separation

4
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

System boundary
Physical plant boundary
Recycled wastewater
V3 Direct CO 2
Electric Power Sep 2 emission
Make-up V1
deionized water Cooler Sep 1 Electric
Power CCS
Selective
Water V2 H2
PSA
(99.9%)
Electric
Power Flue gas
Heat exchanger By-product
Water Electric
Pump 1 for water CO\CH 4 )
Heat exchanger Power
Coal for Coal slurry Qp
Coal Mixer Pump 2 Preheater Natural gas
transportion Furnace
Heat exchanger Comp2

Qg
for furnace
Electric Gasifier Comp1 Air
Electric
Power Exhaust
Power
Electric
Power CCS Power
Turbine production
Selective

CO2 Other Net

Emissions Emissions Power

Fig. 2. System boundary for life cycle assessment of the ISCWGC-HPP system.

unit, gas furnace unit, and other subsystems. The raw material is lignite, Table 3
and the raw materials are assumed to be transported by trucks. The Operation conditions of different investigated processes.
environmental information of transportation is taken from the SimaPro Process code Temperature of SCWG Coal concentration in With/
database model as “Truck 10–20 t”. reactor and preheater SCWG reactor (wt%) without CCS
The LCA of processes with different conditions are conducted to find (°C)
a method for system optimization. The reaction temperature and the
A 600 2 without
coal concentration in the SCWG reactor are selected as the important B 650 2 without
operation conditions. The investigated temperature range is C 700 2 without
600–700 °C, and the processes with 2 wt% and 15 wt% of concentra- D 700 2 with
tions are investigated. The processes with different conditions are E 600 15 without
F 650 15 without
shown in Table 3.
G 700 15 without
H 700 15 with
2.4.2. Life cycle inventory analysis
Table 4 shows the detailed life cycle inventory data for the opera-
tion phase of the ISCWGC-HPP system, which includes material con-
sumption, energy consumption, and transportation. The total coal and eutrophication potential (EP) and photochemical oxidation potential
water throughput of the ISCWGC-HPP system is 40 t/h. The coal is (POFP). The ECO-Indicator 99 method is used to estimate emissions of
transported by road from 10 km away. The raw coal and water are NOx.
firstly mixed into a coal slurry with a concentration of 8 wt% or 60 wt%
and are then fed to a heat exchanger with a piston pump. The main gas 3. Results and discussions
products of ISCWGC-HPP are H2, CO2, CH4 and CO. The SCWG gasifi-
cation results are calculated using the Aspen Plus software. The mass In this section, the process simulation results from Aspen Plus are
and energy balance are achieved with Aspen Plus. Notably, all power presented, including the simulation results of mass flow, energy flow
consumption is from electricity produced by turbine in the ISCWGC- and exergy flow. On the basis of the simulation results, the optimization
HPP system. In the process combined with the CCS unit, 0.6588 MJ of method of energy efficiency is proposed and the life cycle environ-
electricity was required for capturing and storing 1 kg of CO2 [34]. PSA mental performance and the emissions are assessed. Finally, a com-
consumes 1.647 MJ of electricity to separate 1 kg of hydrogen [35]. parison of thermodynamic and environmental performance was con-
ducted to clarify the prospects and challenges of the ISCWGC-HPP
2.4.3. Life cycle impact assessment technology.
SimaPro 9.0.0.30 and the Ecoinvent 3.0 database within the soft-
ware are used to conduct LCA. In the life cycle impact assessment, each 3.1. Simulation results of mass flow
input and output in the inventory is classified as a specific environ-
mental impact. Therefore, all emissions to the impact categories are Table 5 shows the simulation results of coal gasification in super-
assessed using their characteristic factors and are expressed as affecting critical water performed using Aspen Plus 8.4. It indicates that the gas
specific equivalents. Two life cycle impact assessment methods, in- yield and gas fraction change slightly as the temperature increases from
cluding CML and ECO-Indicator 99, are used to assess different cate- 600 °C to 700 °C at the concentration of coal in the SCWG reactor being
gories of environmental impacts associated with the processes of the 2 wt%. In the process C, the hydrogen yield is 55.4 kmol/h. The reason
ISCWGC-HPP system. The impact categories in the CML method con- is that complete gasification has been achieved when the temperature
sidered in this study includes GWP, acidification potential (AP), non- exceeds 600 °C at the coal concentration of 2 wt%. Therefore, from the
bio-effective potential (ADP), ozone depletion Potential (ODP), viewpoint of thermodynamics, further increase in temperature is

5
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

Table 4
Main inventory data for the operation of the ISCWGC-HPP system.
Parameters Value Comment

Coal Yimin lignite

Maximum flow rate of coal slurry 10 t/h
Maximum flow rate of preheated water 30 t/h
Operation pressure of the SCWG reactor 25 MPa
Operation temperature of the SCWG reactor and preheater 600 °C/650 °C/700 °C
Coal powder concentration in the SCWG reactor 2 wt% and 15 wt% The feed concentration of coal slurry was 8 wt% and 60 wt%
Temperature of coal slurry at the reactor inlet 220 °C
Temperature of the preheated water at the preheater inlet 350 °C
The source of preheated water Internal recirculation from effluent
Power input to the cooler 24 kW·h
Hydrogen purity at the PSA outlet 95%
Transportation distance of the chemicals 10 km Road transportation
Functional unit 1 kW·h power

unnecessary for hydrogen production. When the coal concentration is
15 wt%, the gas yield increases sharply with an increase in the tem-
perature. The hydrogen yield increases from 96.5 kmol/h to
181.6 kmol/h and the CH4 yield decreases by 28.6% as the temperature
increases from 600 °C to 700 °C. The results imply that a high tem-
perature is not conducive to the methanation reaction. However, the
water-gas shift reaction is promoted at high temperatures. As the con-
centration increases from 2 wt% to 15 wt%, the CH4 fraction sig-
nificantly increases and the H2 fraction in the gaseous products de-
creases evidently. A high feed concentration means less water in the
reaction process. This behavior can be confirmed due to the lack of
water that inhibits the steam methane reforming reaction and water gas
shift reaction [36].
3.2. Simulation results of energy and exergy flow
In this section, the energy and exergy input and output of the system
were analyzed and the optimization of the system by using an ORC as a
bottoming cycle is carried out.
3.2.1. Energy and exergy flow
In the ISCWGC-HPP system, both hydrogen and electricity are the
products. The electricity of the electrical units, such as high-pressure
pumps, PSA, CCS, and compressor, is from the ISCWGC-HPP system
itself. The reactor and preheater are heated by the combustion of nat-
ural gas and combustible gases other than hydrogen produced by
ISCWGC-HPP system. In the furnace, compressed air consisting of 21%
oxygen and 79% nitrogen, is used as the oxidant. Fig. 3 shows that
consumed natural gas increases drastically as the coal concentration
decreases and the temperature increases. However, the generated and
consumed electricity varies slightly for different processes. The reason
is that the electricity generated and consumed by the system is decided
by the capacity of the system. Notably, the variation in total calorific
value and exergy of hydrogen is negligible with the increase in the
temperature when the concentration is as low as 2 wt%. However, the
total calorific value and exergy of hydrogen increase sharply with the
increase in the temperature when the concentration is as high as 15 wt
%. As shown in Fig. 4, the energy and exergy efficiencies increase with
the increase in the concentration and temperature. The energy and
exergy of process G are 46.6% and 42.6%, respectively. In the ISCWGC-
HPP process, higher concentrations lead to higher increase rates of
energy and exergy efficiency with the increase in the temperature. For
example, the energy efficiency increases by 14.9% from process E to
process F, and the energy efficiency increases by 6.7% from process A to
process B. The reason is that the gas yield increases dramatically as the
temperature increases when the concentration of coal is 15 wt%, as
shown in Table 5. Therefore, the total low heating value (LHV) of hy-
drogen and other combustible gases increase with the increase in the
temperature. Meanwhile, the power consumed and produced by the
system changes slightly when the capacity of the system stays the same.
The abovementioned factors lead to the rapid growth of energy and
exergy efficiencies.
3.2.2. Optimization of energy efficiency
The energy input and output of the different units of the system
need to be investigated to enhance its energy conversion efficiency.
Fig. 5 shows the energy input (+) and output (−) of the different units
in the process G. The maximum energy output is the enthalpy difference
of the effluent between the inlet and outlet of the cooler. The inlet fluid
of the cooler, which is the effluent of HX1, contains a large amount of

Table 5
Detailed mass flow in the simulation of supercritical water gasification of coal.
Items Value

Process A B C E F G
Output stream
H2 (kmol/h) 51.8 54.7 55.4 96.5 136.3 181.6
CH4 (kmol/h) 1.0 0.3 0.1 80.4 69.8 57.4
CO (kmol/h) 0.3 0.4 0.5 2.9 5.6 9.8
CO2 (kmol/h) 25.7 26.3 26.4 119.0 126.9 135.1
Ash from reactor (kg/h) 131.2 131.2 131.2 984.3 984.3 984.3
Effluent from low-pressure gas-liquid separator (kg/h) 38607.2 38581.3 38575.9 32176.3 31836.0 31458.8
Flue gas from furnace (kmol/h) 1514.4 1517.4 1545.4 1333.4 1377.5 1464.8
Input stream
Coal (kg/h) 800 800 800 6000 6000 6000
Water (kg/h) 39,200 39,200 39,200 34,000 34,000 34,000
Natural gas (kmol/h) 137 140 143 30 45.0 64
Air (kmol/h) 1345 1355 1375 1100 1130 1200

6
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

a b
3x104 LHV of coal LHV of natural gas 3x104 Exergy of coal Exergy of natural gas
Consumed electricity LHV of hydrogen Consumed electricity Exergy of hydrogen
2x10 4 Produced electricity 2x104 Produced electricity

1x104 1x104

Exergy (kW)
Energy (kW)
0 0

-1x10 4 -1x104
-2x104
-2x104
-3x104
-3x104
-4x104
-4x104
-5x104
A B C E F G A B C E F G
Process code Process code

(a) Energy consumption and production (b) Exergy consumption and production
Fig. 3. Energy and exergy consumption (−) and production (+) in the ISCWGC-HPP process.

latent heat. If the effluent is cooled directly, then a huge loss of energy
will occur. In process G, the temperature of the effluent in the inlet and
outlet of the cooler are 183 °C and 50 °C, respectively. The effluent in
the inlet of the cooler can be classified as low-temperature heat source,
which is valuable to be recycled. The main methods on recycling the
low-temperature waste heat include ORC [37], thermoelectrical tech-
nology [38], and low-temperature steam production [24]. In this study,
ORC is chosen to recycle the waste heat and generate electricity for
exploring the energy optimization potential of the ISCWGC-HPP
system. Fig. 6 shows the simple schematic of a basic ORC for use as a
bottoming cycle. In the ORC system, R11 was used as an efficient ORC
working medium [39]. In the evaporator, the waste heat of the effluent
from HX1 is transferred to the working medium R11. Supercooled R11
in point 2 is heated to the superheated R11 in point 3. Then, the su-
perheated R11 enters the turbine and the electricity is generated. The
steam exhaust of R11 in point 4 flows to the condenser and is cooled to
the supercooled R11 in point 1. Finally, the supercooled R11 is com-
pressed by the pump to form a thermodynamic cycle.
The operation parameters and simulation results from Aspen Plus
are shown in Table 6. Minimum gas pinch point temperature and en-
ergy balance are considered to determine the mass flow of R11 [40]. In
accordance with the energy balance, the temperature and pressure in
the different points represented by T1–T4 and P1–P4, are calculated. The
results show that the net power of ORC based on process G is 2879 kW,
and the energy efficiency of ORC is 17.3%. The net power of ORC
system combined with process F is 2920 kW, and the energy efficiency
of ORC system is 17.4%. On the basis of the data in Fig. 5, the in-
tegration of ORC results in the increase in total energy efficiency of
process F from 42.2% to 49.7% and in the increase in total energy ef-
ficiency of process G from 46.6% to 53.3%, respectively. Therefore, it is
valuable to apply ORC system in the ISCWGC-HPP system.
than those of the processes with a concentration of 2 wt%. When the coal
concentration is 2 wt%, the AP, ADP, EP, ODP and POFP decrease slightly
as the temperature increases. By contrast, AP, ADP, EP, ODP and POFP
increase slightly as the temperature increases in the processes with con-
centration of 15 wt%. The usage of CCS leads to an increase in the AP,
ADP, EP, ODP and POFP in all processes, which is attributed to the fact
that the AP, ADP, EP, ODP and POFP mainly come from the mining and
transportation of coal and natural gas. Therefore, the low natural gas and
coal consumed by the FU cause the low emissions of AP, ADP, EP, ODP
and POFP. Specially, the trend of GWP is different from that of other
impact categories. When the temperature increases, the GWP decreases
evidently. Moreover, the GWP decreases as the concentration increases,
and the GWP decrease rate increases as the temperature increases. The
CCS is beneficial to decrease the GWP effectively. For example, the GWP
of process G is 0.66 kg CO2 eq/FU, and the GWP of process H decreases to
0.058 kg CO2 eq/FU which is nearly one tenth of GWP of process G. This
finding indicates that the global warming emissions are mainly caused by
the CO2 produced by the SCWG of coal and combustion of natural gas.
Therefore, the GWP can be decreased sharply using CCS. Additionally, CO2
is soluble in high-pressure water. This property can be used to separate
CO2 from the gaseous products of coal SCWG [24]. Therefore, CCS is
useful for considerably reducing GWP, but increases in the overall en-
vironmental impact because of consuming electricity while collecting CO2.
As shown in Fig. 7(g), the NOx decreases slightly as the temperature in-
creases, whereas it decreases sharply as the concentration increases. The
application of CCS results in the increase in NOx emissions. In processes G
and H, the NOx emissions are 6.31 × 10−5 and 7.04 × 10−5 kg NOx-eq/
FU, respectively. In accordance with the ECO-Indicator 99 database, the
50
Energy and exergy efficiency (%)

3.3. Life cycle assessment results 45 Energy efficiency

Exergy efficiency
Hydrogen and electricity were both the products in this study. When 40
evaluating such multi-functional systems, the allocation method must
be followed to assign life cycle inventory data and environmental
burdens [41]. This study uses an allocation based on economic value of
35
the product (8.0 €/kg H2 and 0.21 €/(kW·h) [42]) due to the nature of
the commercial nature of the system and the product (material/energy). 30
For example, the environmental impacts of 1 kg H2 produced can be
equivalent to environmental impacts of 38.1 kW·h of electricity pro- 25
duced by the system. Therefore, the overall environmental impacts of
the system can be calculated using a unified FU (1 kW·h of net power). 20
The set of environmental impact potentials considered by this study A B C E F G
are GWP, AP, ADP, EP, ODP and POFP based on the CML approach. Fig. 7 Process code
shows the LCA results of different processes. The AP, ADP, EP, ODP and
POFP of processes with concentration of 15 wt% are considerably smaller Fig. 4. Energy and exergy efficiencies of the ISCWGC-HPP system.

7
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

a 30000 b 350

25000 300

Power consumed (kW)

Energy input (kW) 20000
250

200
15000
150
10000
100
5000 50

0 0
ral gas d 1 2
Coal Natu onsume p 1 ump 2 ooler sor sor
LHV of LHV of Power c Pum P C PSA o m p r e s o m p r e s
C C
Types of energy input Unit

(a) Energy input (+) (b) Power consumed (+) of different units

c 0

-4000
Enengy output (kW)

-8000

-12000
1-LHV of Hydrogen from PSA
2-LHV of other combustible gas
-16000 3-Power produced by steam turbine
4-Energy loss from furnace
-20000 5-Enthalpy difference of effluent in the cooler
6-Enthalpy of ash from SCWG reactor
1 2 3 4 5 6
Type code of energy output

(c) Energy output (-)

Fig. 5. Energy input (+) and output (−) of the different units in process G of the ISCWGC-HPP system.

Exhaust Waste Heat Table 6

Stream Stream Operation parameters and results of the bottoming organic Rankine
cycle.
Evaporator 3
Items Value

Turbine Pressure of waste heat stream (MPa) 1.5

Temperature of waste heat stream (°C) 183
4
Pressure of exhaust stream (MPa) 1.5
Temperature of exhaust stream (°C) 50
Mass flow of waste heat stream (kg/h) 39,016
Condensation Mass flow of R11 (kg/h) 235,000
Condenser
Cycle T1 of R11 (°C) 20
Pump
2 1 P1 of R11 (MPa) 0.15
T2 of R11 (°C) 21
P2 of R11 (MPa) 2.5
T3 of R11 (°C) 179
Fig. 6. A simple schematic of an organic Rankine cycle for use as a bottoming P3 of R11 (MPa) 2.5
cycle. T4 of R11 (°C) 61.6
P4 of R11 (MPa) 0.15
Net power of ORC system (kW) 2879
main source of NOx in this study is the combustion of natural gas. Efficiency of ORC system (%) 17.3
Therefore, NOx emissions can be decreased by reducing the use of natural
gas and increasing the production of combustible gases.
3.4.1. Comparison on thermodynamic performance of experimental results
3.4. Comparison of thermodynamic and environmental performance and simulation results
Fig. 8 shows the comparison on the thermodynamic performance of
A comparison on thermodynamic performance of experimental and experimental results and simulation results. The carbon gasification
simulation results is conducted. A comparison of thermodynamic and efficiency (CGE) and H2 yield of the experiments are much lower than
environmental performance with other technologies is also performed those of simulation results in terms of the thermodynamic equilibrium,
to explore the prospects and challenges of the ISCWGC-HPP system. which results in less energy and exergy efficiencies of the system based

8
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

a 1.0 b 0.0012

0.0010
0.8

0.0008

GWP (kg CO 2-eq)

AP (kg SO2-eq)
0.6
0.0006
0.4
0.0004

0.2
0.0002

0.0 0.0000
A B C D E F G H A B C D E F G H
Process code Process code

(a) GWP (b) AP

c 0.00016 d 0.00012

0.00014
0.00010
0.00012

POFP (kg C2H 4-eq)

0.00008
EP (kg PO 4 -eq)

0.00010
-3

0.00008 0.00006

0.00006
0.00004
0.00004
0.00002
0.00002

0.00000 0.00000
A B C D E F G H A B C D E F G H
Process code Process code

(c) EP (d) POFP

e 1.0x10
-7
f
-7
1.2x10
-8
8.0x10 -7
1.0x10
ODP (kg CFC -eq)
ADP (kg Sb -eq)

-8
6.0x10
-8
8.0x10
-11

-8
6.0x10
-8
4.0x10
-8
4.0x10
-8
2.0x10 -8
2.0x10

0.0 0.0
A B C D E F G H A B C D E F G H
Process code Process code

(e) ADP (f) ODP

g 0.00025

0.00020

0.00015
NOx (kg eq)

0.00010

0.00005

0.00000
A B C D E F G H
Porcess code

(g) NOx
Fig. 7. Life cycle assessment results.

9
J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

a 90 b 120 e e 40
H2 e COe CH4e CO2e H2 yielde CGEe en ex

H2 yield(mol/kg) or CGE (%)

80 H2 s
CO s
CH4 s
CO2 s H2 yields CGEs en
s
ex
s

70 100 35

(%)
Gas fraction(%)
60
80 30

ex
50

(%) or
40
60 25
30

en
20 40 20
10
0 20 15
600 650 700 600 650 700
Temperature ( ) Temperature ( )

(a) Gas fraction (b) Hydrogen yield, CGE, ηen and ηex
Fig. 8. Comparison of experimental gasification results (2 wt% Yimin lignite + 2 wt% K2CO3, 22.5–25 MPa [12]) with simulation results (2 wt% Yimin lignite,
25 MPa).

on the experimental results. In order to achieve the goal of system in- need to be conducted to overcome the challenges, as detailed as fol-
dustrialization, it is necessary to enhance H2 yield and gasification ef- lows:
ficiency with high coal concentration by using effective catalysts and
optimizing SCWG process. (1) Industrial scale-up of the ISCWGC-HPP system. ISCWGC-HPP
system is a very complex system that consists of the SCWG reactor,
high-temperature heat exchangers, high-pressure coal feeding
3.4.2. Comparison of thermodynamic and environmental performance with
system, steam turbine, furnace, PSA. Integrating these complex
other technologies
components is a difficult task.
In many previous studies, the energy efficiency was represented by
(2) Continuous feeding and gasification of coal slurry are of high con-
net electricity efficiency or gross electricity efficiency [43]. To facilitate
centration. This study suggests that 15 wt% of coal concentration in
the comparison, the energy efficiency of different systems is re-calcu-
the SCWG reactor is needed from the energy and environmental
lated based on the equations of energy and exergy efficiency defined in
perspective. Therefore, the feed concentration of coal should be
this study. Fig. 9 shows the comparison on the thermodynamic effi-
60 wt% when the mass flow ratio of preheated water and coal slurry
ciencies of different systems. It indicates that the energy and exergy
is 3. The continuous feeding of coal slurry with 60 wt% of con-
efficiencies of process G are slightly higher than those of other SCWG
centration without plugging is a major challenge. In addition, the
processes, conventional coal gasification system, and coal power plant.
complete gasification of 15 wt% coal in the reactor is necessary but
However, the thermodynamic efficiencies of process G are lower than
those of the IGCC system. After the ISCWGC-HPP system is optimized,
the energy efficiency of the ISCWGC-HPP system combined with ORC is
higher than that of IGCC. Therefore, system optimization, such as 60 energy efficiency This study
combining the ISCWGC-HPP system with an efficient waste heat re- exergy efficiency
covery system and taking advantage of a combined cycle power gen-
eration system, is important. From the prospect of energy efficiency, the 50
(%)

operation conditions of process G (15 wt%, 700 °C and 25 MPa) are

necessary for the industrialization of the ISCWGC-HPP system. 40
ex

Fig. 10 shows the comparison on environmental emissions of dif-

ferent technologies. Equivalent CO2 (GWP), SO2 (AP) and NOx, which
30
and

are the emissions mainly from coal utilization, are chosen as re-
presentative emissions in comparing the environmental performance of
en

the different technologies [44]. Fig. 10 shows that the environmental 20

performance of the ISCWGC-HPP system is better than that of tradi-
tional thermal power plants. Notably, the GWP of process G is lower
than that of the IGCC system but higher than that of the NGCC system.
By using CCS, the GWP of process G decreases to 0.58 kg CO2 eq/
(kW·h), which is considerably lower than that of IGCC with CCS.
Equivalent SO2 emission of the ISCWGC-HPP system (process G) is close
to that of IGCC and NGCC. NOx emission of the ISCWGC-HPP system
(process G) is 6.31 × 10−5 kg NOx eq/(kW·h), which is one order of
magnitude less than that of IGCC and NGCC. The abovementioned re-
sults reveal that ISCWGC-HPP with efficient gasification of coal at a
concentration as high as 15 wt% is a relatively clean coal utilization
technology compared with other technologies.
3.5. Future work in terms of challenges and chances
The ISCWGC-HPP technology is a comparatively clean technology
with good industrial application prospects. However, several studies
10
0
1 2 3 4 5 6 7 8 9 10 11 12 13
Code of system
Fig. 9. Comparison of thermodynamic efficiencies. 1- Conventional power
plant of circulating fluidized bed [45]; 2- Integrated solid oxide fuel cell and
coal gasification system [46] (averaged efficiency); 3- Coal pyrolysis with cir-
culating fluidized bed power plant [45]; 4- SCWG of biomass (30 wt% biomass,
873 K) [47]; 5- Integrated SCWG of microalgal [15] (averaged efficiency);
6–253 MW IGCC in Buggenum [48]; 7- Oxygen-blown IGCC [43]; 8- Air-blown
IGCC [43]; 9- ISCWGC-HHP (process G, this study); 10- ISCWGC-HHP (process
G, this study) combined with ORC; 11- Concentrated solar SCWG of algal bio-
mass [16]; 12- SCWG of Microalga [49]; 13- Supercritical water reforming of
glycerol [17]

10
 J. Chen, et al. Energy Conversion and Management 198 (2019) 111927

a Fig. 10. Comparison of environmental

1.2 b emissions. 1- Thermal power plant with
Equivalent CO2 (kg CO2 eq/kWh)

CO2-eq 0.0040 SO2-eq 0.0040

lignite [50] (averaged value); 2- Thermal
1.0

Equivalent SO2 (kg SO2 eq/kWh)

NOx
0.0035 0.0035 power plant with natural gas [50] (averaged
value); 3- Supercritical power plant without

NOX (kg NOX/kWh)

0.8 0.0030 0.0030
This study
CCS (CO2 [51], SO2 and NOx [52]); 4- Su-
0.0025 0.0025
0.6 percritical power plant with CCS (CO2 [51],
0.0020 0.0020 SO2 and NOx [52]); 5- NGCC [52] (averaged
0.4 0.0015 0.0015 NOx); 6- NGCC with CCS [52] (averaged
0.0010 0.0010 NOx); 7- IGCC [53]; 8- IGCC with CCS (CO2
0.2 This study [51], averaged SO2 and NOx [54]); 9-
0.0005 0.0005
ISCWGC-HHP (process G, this study);
0.0 0.0000 0.0000 ISCWGC-HHP with CCS (process H, this
1 2 3 4 5 6 7 8 9 10 1 2 3 4 5 6 7 8 9 10
study).
Code of system Code of system

(a) Equivalent CO2 emissions (b) Equivalent SO2 and NOx emissions

difficult. Using preheated water to enhance heating rate of the coal NOx emissions of the ISCWGC-HHP system are lower than those of
slurry is an effective method to achieve complete gasification of the integrated gasification combined cycle. This study indicates that
coal slurry with high concentration. However, this method results ISCWGC-HHP is a relatively clean and efficient coal utilization
in a high feeding concentration of coal slurry and a decrease in technology when the coal can be efficiently gasified under specific
energy efficiency. Therefore, exploring an alternative method to conditions (the coal concentration of 15 wt% and the reaction
promote SCWG that meets the energy and environmental require- temperature of 700 °C). Nevertheless, many challenges in its ap-
ments is a challenging and valuable work in the future. plication should be overcome in the future.
(3) Evaluating the thermodynamic and environmental performance
based on an actual pilot-scale ISCWGC-HPP system. In this study, Declaration of Competing Interest
the ISCWGC-HPP system is designed theoretically, and the mass and
energy flow of ISCWGC-HPP system are simulated using Aspen Plus. The authors declare that they have no conflict of interests regarding
The results of thermodynamic and environmental analysis based on the publication of this paper.
the actual system are conducive to evaluating the system and pro-
posing optimization methods. Acknowledgements

4. Conclusion This work was financially supported by the National Natural Science
Foundation of China (Contract NO. 51508176 and 71573082),
A novel system of integrated supercritical water gasification of coal Fundamental Research Funds for the Central Universities, Key Projects
for hydrogen and power production with 40 t/h throughput of coal and of Hunan Province Science and Technology Plan (NO. 2018SK2019)
water was designed and simulated by Aspen Plus. The thermodynamic and Open Foundation of State Key Laboratory of Multiphase Flow in
performance was analyzed and life cycle environmental impacts of the Power Engineering of China.
system were evaluated using Simapro software. The main conclusions
were obtained as follows: References

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