Accepted Manuscript

Simultaneous optimization and heat integration of the coal-to-SNG

process with a branched heat recovery steam cycle

Bo Huang , Yang Li , Rui Gao , Yongfei Zuo , Zhenghua Dai ,

Fuchen Wang

PII: S0098-1354(18)30070-X
DOI: 10.1016/j.compchemeng.2018.02.008
Reference: CACE 6022

To appear in: Computers and Chemical Engineering

Received date: 9 October 2017

Revised date: 28 January 2018
Accepted date: 9 February 2018

Please cite this article as: Bo Huang , Yang Li , Rui Gao , Yongfei Zuo , Zhenghua Dai ,
Fuchen Wang , Simultaneous optimization and heat integration of the coal-to-SNG process with
a branched heat recovery steam cycle, Computers and Chemical Engineering (2018), doi:
10.1016/j.compchemeng.2018.02.008

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 ACCEPTED MANUSCRIPT

Highlights

 A branched heat recovery steam cycle (HRSC) superstructure is proposed.

 Heat integration in the coal-to-SNG process is conducted through the HRSC
superstructure and Duran-Grossmann model.
 Operating conditions of the coal-to-SNG process and HRSC system are optimized
simultaneously.

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 Compared with industrial data, the exergy efficiency is improved by 1.28% for

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the coal-to-SNG process.

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 ACCEPTED MANUSCRIPT

Simultaneous optimization and heat integration of the coal-to-SNG process with a branched heat
recovery steam cycle

Bo Huang1, Yang Li1, Rui Gao1, Yongfei Zuo2, Zhenghua Dai1,, Fuchen Wang1,

1
Key Laboratory of Coal Gasification and Energy Chemical Engineering of Ministry of Education, East

China University of Science and Technology, Shanghai 200237, China

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2
SEDIN Engineering CO., Ltd., Taiyuan 030032, China

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Abstract

The coal-to-SNG process is an energy-intensive process, and optimizing the heat recovery network can improve the

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economy and energy efficiency. This study proposes a branched, triple pressure level heat recovery steam cycle

(HRSC) to recover waste heat, in which one branch is responsible for recovering the waste heat from the water gas
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shift (WGS) unit, and the other branch is responsible for the methanation (METH) unit. The extended Duran-

Grossmann model is used to optimize two heat exchanger networks to match the branched HRSC superstructure.

The temperature/pressure/flow rates of the HRSC streams and the operating temperature of the WGS and METH
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units are optimized. The optimal bypass ratio of the WGS unit as well as the recycle ratio and split ratio of the
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METH unit, are 0.506, 0.681 and 0.456, respectively. The exergy efficiency of the coal-to-SNG plant is improved

by 1.28% compared with the industrial plant, which can reach 54.17%.
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1. Introduction
Natural gas (NG) is cleaner and more energy-efficient compared with other fossil fuels. NG
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demand has increased at an annual rate of 16.4% over the last five years (Li et al., 2016) due to
increased urbanization and industrialization in China. In 2014, the annual demand of NG in
China was 185.5 billion m3, and 30% of the demand relied on importation (Shaikh et al., 2017),
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which indicates that the energy security situation is dire. Producing coal-based synthetic natural
gas (SNG) is a potential way to mitigate this energy security problem due to the relatively rich
coal reserves in China.


Corresponding author: Zhenghua Dai chinadai@ecust.edu.cn

Corresponding author: Fuchen Wang wfch@ecust.edu.cn
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The coal-to-SNG process consists of an air separation unit (ASU), a gasification (GSF) unit, a
water gas shift (WGS) unit, a sour gas removal (SGR) unit, and a methanation (METH) unit,
among which, the GSF unit, WGS unit, and METH unit are strong exothermic processes. Take
the METH unit as an example: 20% of the energy in the syngas is transformed into waste heat
(Topsoe, 2009). Considering the large amount of waste heat, heat recovery has an important
impact on the energy efficiency of the total plant. The waste heat in the chemical plant is usually

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recovered by raising steam or preheating boiler feed water (BFW) through a heat recovery steam

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cycle (HRSC).

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One way to improve the waste heat utilization efficiency is to conduct heat integration and
optimize the heat recovery network. There are generally two kinds of heat integration models.
One model is based on temperature intervals (heat cascade/problem table algorithms), and it is

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represented by the transshipment model (Papoulias & Grossmann, 1983). The original
transshipment model requires the temperature intervals to be fixed, namely, the interactions
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between the chemical process and the heat recovery network can only be realized by using
discrete operating temperatures for chemical processes and heat recovery streams. Elia et al.
(2010) have used this transshipment model to recover heat from a hybrid coal, biomass, and
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natural gas to liquid (CBGTL) process through steam cycles. Martelli et al. (2011) developed a
heat integration model that is based on the problem table algorithm (Linnhoff & Flower, 1978).
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This model has been used to optimize the operating conditions of the HRSC in a coal-to-SNG
plant (Martelli et al., 2011) and a coal to Fischer–Tropsch fuels plant (Martelli et al., 2013).
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Although the operating conditions (pressures, temperatures, and flow rates) of the HRSC streams
are optimized, the coal-to-SNG or coal to Fischer–Tropsch fuels process cannot be optimized. To
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exploit the heat recovery potential, Navarro-Amorós et al (2013) proposed dynamic temperature
intervals to take variable temperature into consideration, which has the potential to investigate
the synergy between operating conditions of process streams and heat recovery steam/water
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streams. Kong et al. (2017) used dynamic temperature intervals to simultaneously realize the
chemical process synthesis and heat integration.

Another heat integration model that can account for the interactions between a chemical process
and a heat recovery network is the Duran-Grossmann model (Duran & Grossmann, 1986), which
is based on the pinch location method (PLM). This model is widely used in the field of
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simultaneous process optimization and heat integration. Baliban et al. (2011) conducted several
investigations on heat and power integration for CBGTL process (Baliban et al., 2011, 2012,
2013). Recently, Yu et al. (2017) also applied the Duran-Grossmann model to an Organic
Rankine Cycles (ORC) system recovering low-temperature waste heat in a refinery.
The aim of this paper is to exploit the synergy between operating conditions of the coal-to-SNG
process and the HRSC system, and the most relevant work was done in the abovementioned

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Duran-Grossmann model-based papers. However, heat integration in these papers occurred

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between all the cold/hot streams from the total site, which is not reasonable because the location
of each subsystem is relatively far from one another. Dowling & Biegler (2015) extended the

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Duran-Grossmann model to conduct heat integration of different groups of process units
separately.

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In this paper, we will use the extended Duran-Grossmann model to simultaneously realize
separated heat integration within the WGS unit and METH unit and heat integration between the
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WGS unit and METH unit through water/steam integration. A branched, triple pressure level
HRSC is also proposed to recover waste heat from a coal-to-SNG process, with one branch
corresponding to heat recovery of the WGS unit, and the other branch corresponding to heat
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recovery of the METH unit. The operating conditions of the WGS unit and METH unit, as well
as HRSC system, are optimized simultaneously. This paper is presented in the following order:
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the second section describes the coal-to-SNG process, the third section provides the
mathematical model, the fourth section presents the results, and the last section summarizes the
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conclusions.

2. Process description and research methods

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The flowsheet of the coal-to-SNG process is shown in Fig. 1 and can be generally described as
follows: The ASU separates air into nitrogen and oxygen. The steam, oxygen, and coal are then
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fed to a gasification unit to produce syngas (CO+H2). The formed syngas is conditioned in the
WGS unit to undergo the water gas shift reaction, thereby meeting the H2/CO ratio requirement.
After removing H2S and CO2 in the SGR unit, the conditioned syngas is finally converted to CH4
rich gas in the METH unit. The HRSC is used to recover waste heat and provide electricity (blue
dashed line in Fig. 1). Apart from electricity, the HRSC also provides medium pressure (MP)
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steam (red line in Fig. 1) for steam users and provides preheated BFW for the gasifier jacket and
the waste heat boiler (WHB) in the gasification unit.

Coal
GSF
Condensate
Condensate CO2,H2S Condensate
WHB

Gasifier
Air MPS Water Sour gas
Air Methanation
separtion gas shift removal
Waste water
Quench treatment
O2
SNG

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LPS

BFW S2 S3 L1 E3 S4 E4 E5
E1 S1 E2

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L1
BFW
Q Label
E1 L LP steam

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S1 E2
S2 S MP steam
S3
MPS HRSC power E3
E4 E Electricity
S4 E5

Fig. 1 Flowsheet of the coal-to-SNG process

2.1 Coal-to-SNG process US

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2.1.1 Air separation unit (ASU)
Cryogenic air separation is widely used to produce high purity oxygen, which is proven to be a
cost-effective technology (Ebrahimi et al., 2015). This process separates N2 and O2 by using their
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different liquefaction temperatures. The ASU is driven by electricity in this study, and the purity
of O2 is 99.6 vol%.
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2.1.2 Gasification unit

The product gas from the fixed-bed gasifier contains approximately 8 vol% (wet basis) CH4, so
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the fixed-bed gasifier is one of the most suitable technologies to produce coal-based SNG. The
schematic diagram of a Lurgi gasifier is depicted in Fig. 2. Lignite coal is fed from the top of the
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gasifier through a lock hopper, and oxygen and steam enter the gasifier from the bottom of the
gasifier. The MP steam generated from the water jacket is used as the gasification agent, but this
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amount of steam is not enough for gasification, which accounts for approximately 10% of the
steam demand for gasification (He et al., 2013). Extra MP steam is extracted from the steam
pipeline, and in this paper, this extra MP steam is provided by extraction from the high pressure
(HP) turbine or MP turbine in the HRSC. The syngas exiting the gasifier enters the quench
cooler, in which the syngas is saturated with steam and enters the waste heat boiler (WHB).
Saturated low pressure (LP) steam is raised in the WHB, and this LP steam is used to treat
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wastewater from the GSF unit and provide heat for the SGR unit. The rest of LP steam is
directed into the LP steam pipeline. In this paper, the surplus LP steam is superheated and used
to generate power in the HRSC.

Coal

Lock
syngas

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hopper
Quench liquor
LP steam

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Gasifier Quench Waste heat
boiler
steam

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BFW
BFW

Steam&O2

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Ash Lock
Gas liquor
Ash
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Fig. 2 Schematic diagram of a Lurgi gasifier

2.1.3 Water gas shift (WGS) unit

The WGS unit adjusts the CO/H2 mole ratio by converting a portion of CO to H2 through the
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water gas shift reaction (1) to satisfy the H2/CO ratio requirement for the methanation reaction,
in which the favorable H2/CO ratio is approximately 3.1. The water gas shift reaction is an
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exothermic and reversible reaction; thus, low temperature is favored for the forward direction.
CO  H 2O  CO2  H 2 ΔH 298
0
 -41.1kJ  mol 1 (1)
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The flowsheet of the WGS unit without heat recovery is shown in Fig. 3. There are two serial
reactors. R-100 is used to burn out O2 in the raw gas, and raw gas from R-100 is split in S-101 so
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that one stream is fed to the main WGS reactor (R-101), while the other part is bypassed. The
bypass ratio is a key parameter for the WGS unit and its definition is shown in equation (2),
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wherein FTSout
101
is the total molar flow rate at splitter S-101 outlet ‘out’ (see Fig. 3). The
operating temperature of the main WGS reactor is 473.15~773.15 K (Boll et al., 2011), and a
sulfur-tolerant catalyst is used due to the existence of H2S. The units E-101 to E-104 perform as
coolers or heaters to adjust the gas temperature to meet the operating requirements. In E-103 and
E-104, part of the water vapor in the syngas is condensed and removed. Finally, the syngas is
cooled to approximately 313.15 K and fed to SGR unit to remove H2S and CO2.
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Gas cooler
E-104 E-103 E-102

Syngas

out
M-102
Condensate

S-101
out2
E-101
R-100 M-101 R-101

Raw gas Steam

Main reactor
Pre-reactor

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Fig. 3 Flowsheet of the water gas shift unit

FTSout

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RB  101
(2)
FTSin101

2.1.4 Sour gas removal (SGR) unit

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The production of a large quantity of CO2 in the shifted syngas from the WGS unit will affect the
methanation reaction; simultaneously, H2S will poison the methanation catalyst. As a result, the
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SGR unit is necessary for the normal operation of the METH unit. The Rectisol process is widely
used in chemical plants (Yu et al., 2012), in which chilled methanol is used to absorb H2S and
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CO2. The energy consumption of the SGR consists of the electricity consumption for methanol
refrigeration and the heat requirement for the reboiler in the regeneration tower.
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2.1.5 Methanation (METH) unit

The function of the METH unit is to convert syngas into the CH4 rich gas via CO methanation (3)
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and CO2 methanation reactions (4). In the METH unit, reactions (1), (3) and (4) are considered.
CO  3H 2  CH 4  H 2O ΔH 298
0
 -206kJ  mol 1 (3)
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CO2 +4H 2  CH 4 +2H 2O ΔH 298

0
 -165kJ  mol 1 (4)
The TREMP (Topsoe, 2009) methanation process is employed for the methanation unit in this
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model. The normal operating temperature range of methanation reactors is 523.15 to 973.15 K,
and the catalyst can operate below its sintering temperature (approximately 1023.15 K)
(Blumberg et al., 2015). The flowsheet of the METH unit in the base plant is shown in Fig. 4.
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Gas cooler
E-211 E-210 E-209 E-208 E-207 E-206 E-205

SNG R-205 R-204 R-203

Condensate Condensate
5th Methanator 4th Methanator 3rd Methanator E-204
P-201
E-202
Steam
out
E-200 E-201 E-203
out2
M-201 R-200 M-202 R-201 S-202
R-202
Sweet gas out2
M-203

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S-201
Sulfur guard st 2nd Methanator
out Steam1 Methanator

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Fig. 4 Flowsheet of the methanation unit

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In the METH unit, six reactors in a series are used. R-200 is the sulfur guard, and R-201 and R-
202 are the main reactors. R-203, R-204, and R-205 are gas cleaners to convert residual CO and

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H2 to CH4. To control the temperature of the reactors, part of the effluent gas from R-201 is
recycled to the inlet of R-201. Equations (5) and (6) show the recycle ratio and the split ratio,
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respectively, as vital operating parameters in the METH unit. The effluent of R-204 is cooled to
remove excess water, thus promoting the forward methanation reaction. Finally, the effluent of
R-205 is cooled to 313.15 K via 3 serial coolers and knocks out condensate water.
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FTSout
RR   202
in
(5)
FTS 202
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FTSout
RS   201
in
FTS 201 (6)
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2.2 Superstructure of the heat recovery steam cycles (HRSC)

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2.2.1 Separated heat integration and water/steam integration

In this paper, we propose a branched HRSC to recover waste heat from the WGS and METH
units in an integral manner. Further, we will conduct ‘separated heat integration’ within each
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subsystem (Dowling & Biegler, 2015) and simultaneously realize heat integration between
different subsystems through water/steam integration. As shown in Fig. 5, the ‘separated heat
integration’ means that the cold streams exchange heat with hot streams in the same unit, namely,
streams in the WGS unit do not exchange heat with streams in the METH unit, and this
configuration is reasonable as the WGS and METH units are relatively far from one another. The
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heat integration between the WGS and METH units is realized by water/steam integration
through the branched HRSC.

The unique feature of the HRSC is that it has two branches. The upper branch is responsible for
recovering the waste heat from the WGS unit, and the lower branch is responsible for recovering
the waste heat from the METH unit. Therefore, two separate heat exchanger networks (HENs)
can be derived, namely, the WGS-HEN and the METH-HEN. It is worth noting that to simplify

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the model, the mixing of branches in the HRSC is isothermal and isobaric. It is important that the

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split ratios between the upper and lower branches are optimization variables and can be different

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at each splitter; this is how the water/steam integration between the WGS and METH units is
realized.

WGS-HEN
USWGS Process streams
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Economizer Evaporator superheater

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METH-HEN METH Process streams

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Condenser

Fig. 5 Schematic of heat integration

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2.2.2 Branched HRSC with a captive power plant (HRSC-CPP)

In the coal-to-SNG process, the largest steam consumer is the Lurgi gasifier, which consumes a
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large amount of MP steam (5 MPa, 723 K). However, the steam is insufficient, even if all the
waste heat is used to generate the MP steam; therefore, a captive power plant (CPP) is applied to
provide extra steam. In this paper, HRSC and CPP are integrated to provide electricity and steam.
The superstructure of the integrated HRSC-CPP is shown in Fig. 6, the HP steam from the CPP
boiler is fed into the HP turbine of the HRSC. We assume that the temperature and pressure of
HP steam generated by the CPP boiler are the same as those generated by the HRSC.
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In this paper, a triple pressure level branched HRSC system is used to exploit the heat recovery
potential. Water from the deaerator is pumped by the LP/MP/HP water pumps, and water/steam
absorbs heat in the corresponding economizers/evaporators/superheaters. Finally, superheated
steams enter the corresponding turbines to generate electricity. The exhausted steam from the LP
turbine then enters the condenser. Part of the LP steam is extracted from the LP turbine and
mixes with the condensed water in the deaerator, thus meeting the operating temperature of the

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deaerator (377 K). In addition, the MP steam is extracted from the HP turbine or the MP turbine

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for MP steam users (including the GSF unit, WGS unit, and METH unit). The GSF unit produces
saturated LP steam in the WHB, and part of the LP steam is consumed by wastewater treatment

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and SGR units. The remaining steam is superheated and injected into the MP turbine or LP
turbine.

E-301 E-302
US E-303
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HP
P-301
Turbine T-301
E-402 E-403
E-401
HP Economizer HP Evaporator HP Superheater
Reheater
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E-305 E-306 E-307 E-304 E-404

MP steam
user
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P-302

E-406 E-407
E-405
MP
MP Economizer MP Evaporator MP Superheater T-302
Turbine
LP steam from
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WHB

E-308 E-309 E-310

E-311 Boiler
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P-303
E-411
E-409 E-410
E-408
LP Economizer LP Evaporator LP Superheater LP
T-303
Turbine
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Deaerator coal
E-312

P-304 air
Demineralized water
E-412 Condenser
BFW

E-313
To water jacket

E-413

Fig. 6 Superstructure of branched heat recovery steam cycle (HRSC)

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2.3 Research methods

The overall model is formulated in the General Algebraic Modeling System (GAMS). This
model is a highly nonconvex NLP problem. There are 3000+ constraints and 3000+ variables, in
which 2000+ constraints and 2000+ variables are nonlinear. The state-of-the-art global solvers,
such as GAMS/BARON, GAMS/ANTIGONE, and GAMS/Lindoglobal, failed to get to the
global optimal solution within a reasonable time (100 hr) for this model; therefore, a local NLP

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solver, GAMS/CONOPT (Drud, 1994), is used to solve it, namely the solution is a local optimal

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solution. In this paper, we will obtain the initial solution with initial values provided by an Aspen
Plus simulation, and the initial solution will be tuned in the tuning procedure. The recycle ratio

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of the METH unit (Li et al., 2014) and the pressures of HP/MP/LP steam are key manipulated
variables that have a relatively large influence on the efficiency of the coal-to-SNG process.

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Each key manipulated variable has been discretized into equally spaced values according to its
bounds. In the tuning procedure, the model has been solved iteratively. In each iteration, only
one key manipulated variable is fixed at a discretized value and other variables are free, and the
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best-known solution is kept and used as the initial value for the next iteration. Finally, the best-
known solution is used as the initial value for the model without fixed key variables, and the
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final solution (best known) is reported in this paper. Each iteration of the model takes about two
CUP seconds (Intel Core i7-4790 3.60 GHz).
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3.1 Thermodynamic property model

In this paper, steam is treated as a real gas, while other gases are treated as ideal gases, and the
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gas mixture is treated as an ideal gas mixture.

ALAMO (Cozad et al., 2014) and Aspen Plus are used to fit the enthalpy-temperature correlation
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for steam in the pressure range of 0.1-125 bar and in the temperature range of 298.15~1000 K. In
the proposed method, ALAMO generates 10000 or more sampling points (T, P) and calls the
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Aspen Plus model (which uses the IAPWS-95 property package) via Python to simulate and
retrieve simulation results (enthalpy values), thus building an enthalpy-temperature correlation.
The R2 can reach 0.999, and the maximum error is less than 2%.

The steam enthalpy-temperature correlation generated by ALAMO is shown below. The units of
enthalpy, T, and P are kJ·kmol-1, K, and MPa, respectively.
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6.44  107
hH 2O   585T  0.176(T ) 2  3.53  105 ln(T )  4.43  103 PH2O 
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37.72( PH2O ) 2 -6.17  10-3 (T ) 2 PH2O  4.23  10-2T(PH2O )2 -2.02  106 (7)

3.2 Coal-to-SNG process model

An operating coal-to-SNG plant in northwest China is used as the base plant in this paper. The

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operating conditions of the WGS unit, METH unit, and HRSC system are optimized to exploit

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the heat recovery potential, while the operating conditions of the ASU, GSF unit, and SGR unit
are fixed due to their relatively narrow operating windows. The mass balance and energy balance

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model for the WGS unit, METH unit, and HRSC are built rigorously, while the operating data
used for the ASU, GSF unit, and SGR unit are retrieved from the base plant in northwest China.

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In the following paper, the WGS unit and the METH unit are combined into the WGS-METH
section.
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3.2.1 The operating data of ASU, GSF unit, and SGR unit
In this paper, only the electricity consumption of the ASU is considered, which is 0.6 kWh/Nm3
O2 at a pressure of 5 MPa (Li et al., 2014).
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As for the gasifier in the GSF unit, Yining coal is used as feedstock, for which the mass flow
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rates is 1081 kg·h-1. Tables 1 and 2 list the properties of coal and the consumption amounts of
oxygen and steam, respectively. The conditions of syngas exiting the gasification battery limit, or
the source gas of the WGS unit, are listed in Table 3. The saturated LP steam (0.6 MPa)
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generated in the WHB is approximately 0.494 t steam/ t coal, of which 36.5% is used in the
wastewater treatment unit, and 35.5% is used in the SGR unit. The remaining LP steam is
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superheated in E-311/E-411 in Fig. 6 and then injected into the MP/LP turbines.

Table 1 Properties of raw coal

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Coal proximate analysis (wt %) HHV (ad) Ultimate analysis (wt %)

Mad Aad Vad FCad MJ/kg C H O N S
13.10 10.33 28.08 48.49 23.01 60.10 3.00 12.43 0.62 0.42
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Table 2 Gasification agent consumption

Gasification agent Value Quality

Oxygen 207.57 Nm3 O2/t coal Purity 99.6 vol%
①
MP steam 1.482 t steam/t coal 5.0 MPa, 723 K
②
MP steam 0.282 t steam/t coal 4.1 MPa, 520 K

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① This extra steam is from the HRSC

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② This steam is from water jacket

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Table 3 Gas composition at the gasification battery limit
Term Value
T/K 446.6
P/MPa(A)
Flow rates / kmol·h -1 US 4
100
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H2O 23.61
CO 13.28
CO2 24.46
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H2S 0.18
Composition
H2 30.05
/vol%
N2 0.10
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CH4 7.88
O2 0.23
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C2H6 0.21
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For the SGR unit, a simple input-output relation is used to simulate this process. The gas
recovery ratio taken from the base plant is shown in Table 4, namely, 100% H2S and 97.55%
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CO2 is removed in the SGR unit.

Table 4 Performance of the SGR unit

Components CO H2 CO2 CH4 H 2S
Recovery ratio/% 99.59 99.97 2.45 100 0
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3.2.2 Models of the WGS-METH section

The mass balance and energy balance model of the WGS-METH section is built to optimize the
operating conditions. In the WGS-METH section, there are mixers, splitters, coolers, heaters,
flash tankers and reactors. The models of the mixers, splitters, coolers, and heaters are
straightforward and are therefore neglected here, following are models of the reactor and flash
tanker.

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In the WGS unit, the water gas shift reaction (1) is considered. This reaction is equilibrium

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restricted, and the approach temperature is 48 K in the WGS unit, which is determined by

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regressing the base plant operating data.

In the METH unit, reactions (1), (3), and (4) are considered, and only 2 of these 3 reactions are

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independent. Therefore, reactions (1) and (3) are modeled in the METH reactors, and the gas
compositions at the reactor outlet are close to an equilibrium state. The approach temperature is
specified as 0.8 K in this paper, and the heat loss is approximately 2.2% of the reaction heat,
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which are also determined by regressing the base plant operating data.

Equilibrium constant correlations for reactions (1) and (3) are shown in equations (8) and (9)
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(Chein et al., 2016); P denotes the total pressure and Fg,iout stands for the molar flow rates of

species i at the outlet of equipment g. The set of reactors that are restricted by the water gas shift
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reaction is defined as SRW={R-101, R-201, R-202, R-203, R-204, R-205}, and the set of
reactors that are restricted by the CO methanation reaction is defined as SRM={R-201, R-202,
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R-203, R-204, R-205}. The composition at the outlet of the reactors is governed by equations (10)
and (11).
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4400
K gWGS  1.767  102 exp( ) g  SRM (8)
Tgout
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26830 FTg 2
out

K gMETH  1.198  1023 exp( )  ( out ) g  SRM (9)

Tgout Tg

Fgout
,CO
 Fgout
, H2O
- K gWGS  Fgout
,CO2
 Fgout
, H2
0 g  SRM (10)

( Fgout
, H2
)3  Fgout
,CO
 K gMETH  Fgout
,CH4
 Fgout
, H2O
0 g  SRM (11)
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The effluent of the WGS reactor (R-101) and the 4th and 5th METH reactors (R-204 and R-205)
need to be cooled to a low temperature so that water vapor in the syngas is condensed. In the
flash model, we assume dry gas does not dissolve in the condensate, the gas stream at the flash
tanker outlet is saturated with water vapor, and excess water vapor is condensed.

3.3 Heat integration model

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3.3.1 HRSC thermodynamic model

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The electricity consumed by the LP/MP/HP water pump can be calculated by equation (12),
where  pump is isentropic efficiency, which is assumed to be 0.8 (Ensinas et al., 2007), hg,H2O
in
stands

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iso
for the specific enthalpy of water/steam at the inlet of equipment g, hg,H2O is the outlet enthalpy

when the compression process is isentropic, and the set of pumps is defined as SP={P-301, P-
302, P-303, P-304}.

FTgin
US
AN
Wpump   iso
(hg,H2O in
- hg,H2O ) (12)
gSP  pump

The power output of the steam turbine is calculated by equation (13), turbine and generator are the
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isentropic efficiencies of the turbine and generator, which are assumed to be 0.8 and 0.96,
respectively (Ensinas et al., 2007), and the set of turbines is defined as ST={T-301, T-302, T-
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303}. The HP and MP turbines are backpressure turbines, while the LP turbine is a condensing
turbine, and the steam dryness at the outlet of the LP turbine is greater than 0.9.
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Wturbine   FTgin  turbine  generator  (hg,H2O

in iso
- hg,H2O ) (13)
gST

DNST 303  0.9 (14)

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Heat absorbed by economizers, evaporators, superheaters and reheaters is calculated by equation

(15), and the set of heat absorbers in the HRSC is defined as SQA={E-301,…, E-313}∪{E-
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410,…, E413}.

QAg  FTgin (hg,H2O

out
 hg,H2O
in
) g  SQA (15)

Heat released by the condenser is calculated by equation (16), and the set of heat coolers in the
HRSC is defined as SQR={condenser}.
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QRg  FTgin (hg,H2O

in out
- hg,H2O ) g  SQR (16)

The pressure drop between two pressure levels is restricted by equation (17).

PHP  PMP  0.5MPa and PMP  PLP  0.5MPa (17)

The temperature change in the evaporator and condenser is assumed to be 1 K so as to avoid the
infinite heat capacity of streams under phase change.

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3.3.2 Boiler of the captive power plant (CPP)

The heat absorbed by the boiler is calculated by equation (18), in which boiler is the boiler

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efficiency, which is fixed at 0.85 (Ensinas et al., 2007) in this paper, M fuel is the mass flowrate of

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coal fed into the boiler, and LHV represents the lower heating value of fuel coal. The amount of
HP steam generated in the boiler is calculated by equation (19).
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Qboiler  boiler  M fuel  LHV (18)

Qboiler  FTboiler   hboiler,H2O

out
 hboiler,H2O
in
 (19)
M

3.3.3 Extended Duran-Grossmann model

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Pinch analysis (Linnhoff, 1982) is a powerful tool to perform heat integration and target the
heating/cooling utility. The analysis requires fixed inlet/outlet temperature and flow rates;
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therefore, it is difficult to use this method to simultaneously optimize the process with variable
temperature and flow rates. However, Duran and Grossmann (Duran & Grossmann, 1986) had
proposed a mathematical model that used floating pinch temperatures so as to optimize the
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process and heat integration simultaneously. Hence, the Duran-Grossmann model has been
adopted.
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As the Duran-Grossmann model is based on pinch methods, it obeys the rule that the pinch point
always appears at the inlet of streams when the heat capacity flowrate (FCp) is fixed; thus, the
Duran-Grossmann model treats each of the inlet temperatures of the hot and cold streams as
pinch candidates. Duran and Grossmann had observed that the true pinch temperature exhibits
the largest heating and cooling utilities among all pinch candidates. The key point of Duran-
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Grossmann model is therefore to calculate the heating utility (the same as heat deficit ( ZH Pch ))

of each pinch candidate, where QSIAPch / QSOAPch are the total heat loads of the cold/hot streams

above each candidate. The set of pinch temperature candidates is defined as PC={ Tgin | g∈

coolers or heaters in the HEN}. The maximum heating utility ( QH ) is determined by equation
(21). The actual minimum cooling utility is determined by the heat balance equation (22),
where ( x ) is the difference between the total heat contents of the cold and hot streams.

T
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Constraint (23) is suitable for the coal-to-SNG process as it has surplus heat to recover. To use
NLP algorithms, max operators in equation (21) should be smoothed by equation (24), where  is

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a small number such as 10-4. For a detailed description, the reader can refer to the original paper
(Duran & Grossmann, 1986).

ZH Pch ( x)  QSIAPch ( x)  QSOAPch ( x)

QH  max{ZH Pch ( x)}

USPch  PC (20)

(21)
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QC  ( x)  QH (22)
QH  0 (23)
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max{0,  }  0.5(  ( 2   )0.5 ) (24)

In the original Duran-Grossmann model, there is only one set of cold and hot streams that
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exchange heat with each other. In this paper, the extended Duran-Grossmann model (Dowling &
Biegler, 2015) is used with two sets of cold and hot streams. One set of cold and hot streams
corresponds to streams in the WGS-HEN (see Fig. 5); the other set corresponds to streams in the
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METH-HEN (see Fig. 5). So there are two sets of constraints (20)-(24).
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3.4 Electricity balance

The electricity generated by HP/MP/LP turbines is used to meet the electricity demand of all the
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auxiliary devices; the power consumption of auxiliary devices is denoted as Wauxiliary, and the
specific power consumption of the ASU, GSF unit and SGR unit are listed in Table 5. The total
power consumption of auxiliary devices is calculated by equation (25), in which
Wpump , Wrecycle , WASU , WGSF , WSGR , Wcompression are values of electricity consumption of the pumps in the

HRSC, syngas recycle compressor in the METH unit, ASU, GSF unit and SNG compressor,
respectively. The electricity balance is constrained by equation (26).
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Table 5 Specific power consumption of auxiliary devices

Devices Specific consumption References

ASU 0.6 kWh/Nm3 O2 (Li et al., 2014)

GSF 0.003 kWh/kg coal (He et al., 2013)
SGR 0.024 kWh/Nm3 syngas (Yin & He, 2011)

T
Wauxiliary  Wpump  Wrecycle  WASU  WGSF  WSGR  Wcompression (25)

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Wturbine  Wauxiliary  0 (26)

3.5 Overall models and objective

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The overall NLP model can be formulated as shown in P1:

Max OBJ 
ESNG
Ecoal
s.t. m(x)  Wturbine  Wauxiliary  0
US
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( x)  0 (P1)
 (x)  0
( x)  0
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The objective is maximizing the total exergy efficiency: ESNG represents the exergy of SNG, and
Ecoal stands for the exergy of gasification coal and the fuel coal. Fuel coal is used to fire the
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captive power plant boiler. The function m(x) represents the electricity balance of this process:
the electricity consumption by auxiliary devices is provided by the steam turbines with no
surplus electricity to the power grid. The function ( x ) represents the energy and material
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balance of the WGS-METH section and the HRSC system. The function (x) is the design
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specification of this process, such as the molar fraction of CH4 in SNG, which is set to 97.6%
(the same as the base plant) and the molar fraction of steam at the METH reactors inlet, which is
set to be greater than 14% to avoid carbon deposition. The function ( x ) represents the
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constraints of the extended Duran-Grossmann model (equations (20)-(24)).

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4. Results and discussion

4.1 Model validation

A set of base plant data is used to verify the thermodynamic property model and WGS-METH
model. The gas conditions are the same as the data in Table 3; the feed gas entering the WGS
unit is 100 kmol·h-1.

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In this paper, the operating conditions of the base plant are used to conduct a simulation with an

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optimization model (formulated in GAMS) to verify the thermodynamic property model and
WGS-METH model. Table 6 compares some key parameters.

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Table 6 Comparison between the base plant data and GAMS model results
①
R-201 inlet R-201 outlet
Base
Plant US Optimization
Model
Base
Plant
Optimization
Model
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T/K 528.2 528.5 948.2 948.9
P/MPa 3.22 3.22 3.17 3.17
H2O 14.16 13.98 24.41 24.19
CO 10.73 10.73 2.95 2.92
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CO2 3.13 3.12 4.61 4.62

Composition
H2 45.11 45.26 27.58 27.76
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/ vol%
N2 0.22 0.22 0.26 0.26
CH4 26.50 26.53 40.18 40.25
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C2H6 0.15 0.15 0.01 0.00

① R-201 is the first main methanation reactor

The temperature and compositions of the base plant and GAMS model agree very well, which
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indicates that the optimization model is reliable.

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4.2 Optimization results

In the following paper, the optimal operating conditions for the WGS-METH section and the
HRSC are described.

4.2.1 Optimal operating conditions for the WGS-METH section

Table 7 shows the optimal operating conditions of the main reactors in the WGS unit and METH
unit, and apart from the temperature, pressure, and compositions in Table 7, the bypass ratio of
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the WGS unit is 0.506, namely, 50.6% of syngas bypasses the WGS reactor R-101. In this case,
steam in the raw gas is sufficient for the water gas shift reaction and no extra steam is needed.
For the METH unit, the optimal recycle ratio is 0.681, which is relatively low compared to the
ratio of 0.85 reported in the literature (Li et al., 2014). Such a low recycle ratio leads to a high
operating temperature in the methanation reactors. The temperature at the R-201 and R-202
outlets is 897.7 K and 973.1 K, respectively, and high temperature is advantageous for the

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cogeneration of electricity (Gassner et al., 2011). The optimal split ratio is 0.456, namely, 54.4%

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of the syngas enters R-201, and 45.6% of the syngas enters R-202. Fig. 7 shows the influence of
the bypass ratio, recycle ratio, and split ratio on the exergy efficiency. When the bypass ratio of

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the WGS unit is between 0~0.6, it has a weak influence on the exergy efficiency; however, when
it exceeds 0.6, the exergy efficiency decreases sharply. The influence of the recycle ratio on

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exergy efficiency is relatively straightforward, and the exergy efficiency initially increases and
then decreases with an increase in the recycle ratio. For the split ratio of the METH unit, the
influence on exergy efficiency is weak when it is between 0~0.5; however, the exergy efficiency
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decreases gradually when it exceeds 0.5.

Table 7. Operating conditions of the WGS-METH section

M

R-101 R-101 R-201 R-201 R-202 R-202 R-203 R-203 SNG

inlet Outlet inlet outlet inlet outlet inlet outlet Product
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P/MPa(A) 3.92 3.87 3.22 3.17 3.14 3.09 3.06 3.01 7.00
T/K 638.7 683.9 524.9 897.7 610.3 973.1 513.2 792.8 313.2

H2O 23.40 18.70 14.00 23.70 10.60 18.70 18.70 29.50 0.30
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CO 12.60 7.90 9.00 1.70 11.50 4.40 4.40 0.30 0.00

Composition CO2 25.30 30.00 3.30 4.50 2.90 4.60 4.60 3.30 1.10
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/vol% H2S 0.20 0.20 0.00 0.00 0.00 0.00 0.00 0.00 0.00
H2 30.50 35.20 38.30 20.70 44.50 29.20 29.20 11.60 0.40
N2 0.10 0.10 0.30 0.30 0.20 0.30 0.30 0.30 0.50
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CH4 7.90 7.90 35.10 49.10 30.20 42.90 42.90 55.00 97.60
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0.544

0.542

0.540

0.538
Exergy efficiency
0.536 Split ratio
Bypass ratio
0.534
Recycle ratio
0.532

T
0.530

0.528

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0.526

0.524

CR
0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Ratio

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Fig. 7 Influence of bypass ratio, recycle ratio and split ratio on exergy efficiency

Fig. 8 depicts the grand composite curves (GCC) of the process streams within the WGS and
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METH units. There is approximately 412 kW/716 kW of waste heat that could be recovered or
removed in the WGS/METH units, respectively, when the heat recovery approach temperature
(HRAT) is fixed at 10 K. It is obvious that the waste heat of the METH unit concentrates in the
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high-temperature region, while it concentrates in the low-temperature region for the WGS unit;
for this reason, we integrate the heat of these two units to realize cascaded utilization of energy.
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1000 Grand Composite Curve of the METH unit

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Grand Composite Curve of the WGS unit

900

800
Temperature /K
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700

600
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500

400

300

0 100 200 300 400 500 600 700 800

Enthalpy/kW

Fig. 8 Grand composite curves of the WGS unit and METH unit without stream generation
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4.2.2 Optimal operating conditions for the HRSC

The electricity balance of the HRSC-CPP is shown in Fig. 9, from which we can see that the
electricity generated by the turbines is 202.9 kW, 66.36% of which is consumed by the ASU
(including O2 compression). The second largest electricity consumer is SGR, which accounts for
20.76% of total electricity consumption. The electricity consumption proportion is similar to that
of (Li et al., 2014).

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Apart from the electricity balance, Fig. 9 also depicts the water balance of the HRSC-CPP. It is

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important to note that the flow rates of the MP steam evaporated in the HRSC is 0, although the
superstructure of the HRSC has 3 pressure levels. A CPP boiler with a capacity of 61.89 kmol·h-1

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HP steam is installed to meet the electricity demand and MP steam demand of the system. To
satisfy the MP steam demand of steam users, 102.54 kmol·h-1 MP steam (5.0 MPa, 723.15 K) is

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extracted from the MP turbine, in which 89.00 kmol·h-1, 0.21 kmol·h-1, and 13.34 kmol·h-1 steam
are sent to the gasifier, METH unit, and wastewater treatment unit, respectively. To maintain the
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operation of the deaerator, 3.94 kmol·h-1 of LP steam (0.126 MPa, 379.53 K) extracted from the
LP turbine is fed to the deaerator. 142.01 kmol·h-1 of demineralized water is heated from 318 K
to the deaerator temperature so as to maintain the water balance of the HRSC-CPP, and 16.94
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kmol·h-1 BFW is heated to 423.15 K and fed to the water jacket of the gasifier.
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AC
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61.89 kmol·h-1
86.80%
GSF
47.19 kmol·h-1 0.00%
WGS
102.54 METH
kmol·h-1 0.20%
WWT
13.00%
-4.58 kW HP Turbine T-301

MPS 66.36%
ASU
0 kmol·h-1 17.9 kW
20.76%

T
SGR

0.00 kW 7.13% SNG

Boiler

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MP Turbine T-302 131.2 kW compr
8.77 1.60%
From WHB GSF
kmol·h-1
14.43 kmol·h-1 4.15%
53.8 kW Pumps

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-0.02 kW coal
LP Turbine T-303

US
air
3.94 kmol·h-1

142.01kmol·h-1
Deaerator
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25.79 kmol·h-1
Demineralized water
-0.10 kW

16.94 kmol·h-1
Condenser
61.89 kmol·h-1
BFW
To water jacket
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31.3 kmol·h-1

To WHB

Fig. 9 Water and electricity balance of the HRSC-CPP

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The pressure, temperature, total flow rates and relative amounts of steam/water generated by the
WGS/METH unit are shown in Table 8. The data of the 6th and 7th columns in Table 8 show the
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distribution of water/steam in the WGS-HEN and METH-HEN. It can be observed that waste
heat from the WGS unit is used to generate LP steam and preheat the demineralized water as
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well as the BFW for the water jacket of the gasifier, while the main function of the waste heat of
the METH unit is to generate HP steam. The difference between this configuration and the
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conventional configuration is that a portion of the saturated HP steam (13.00%) is generated in

the WGS unit and not generated in a conventional WGS unit, and this portion of the HP saturated
steam together with other HP steam generated from the METH unit is superheated in the METH
unit.
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Table 8. Operating conditions of the HRSC

Pressure/MPa Tin/K Tout/K Total/kmol·h-1 WGS/% METH/%

HP Economizer 12.50 377.15 600.72 47.19 9.50 90.50
HP Evaporator 12.50 600.72 601.72 47.19 13.00 87.00
HP Superheater 12.50 601.72 833.15 47.19 0.00 100.00
Reheater 11.07 814.65 832.72 109.07 0.00 100.00

T
LP Economizer 0.30 377.15 406.49 14.43 100.00 0.00
LP Evaporator 0.30 406.49 407.49 14.43 81.40 18.60

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①
LP Superheater 0.30 407.49 446.61 14.43 100.00 0.00
②

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LP Superheater 0.60 432.15 491.88 8.77 100.00 0.00
Demineralized water 0.20 318.15 373.16 142.01 100.00 0.00
BFW for jacket 4.50 377.15 423.15 16.94 100.00 0.00
①Refer to the LP superheater (E-310/E-410 in Fig. 6)

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②Refer to the superheater (E-311/E-411 in Fig. 6) that heats the LP steam from waste heat boiler
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4.2.3 Composite curves
To illustrate the heat recovery effect, composite curves of the WGS-HEN (see Fig. 10) and
METH-HEN (see Fig. 11) are shown. From these two graphs, it is obvious that the cold and hot
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stream composite curves are very close, indicating that waste heat is recovered efficiently.
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700 Hot Composite Curve of the WGS-HEN

Cold Composite Curve of the WGS-HEN
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600
Temperature /K
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500

400
AC

300

0 100 200 300 400 500 600

Enthalpy/kW

Fig. 10 Composite curves of the WGS-HEN

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1000
Hot Composite Curve of the METH-HEN
Cold Composite Curve of the METH-HEN
900

Temperature /K 800

700

600

T
500

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400

300

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0 100 200 300 400 500 600 700 800 900
Enthalpy/kW

Fig. 11 Composite curves of the METH-HEN

4.3 Comparison with the base plant US

To show the superiority of the proposed method, the heat recovery performance of the WGS-
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METH section between the base plant and the optimized plant is compared. Table 9 lists the
operating conditions of the HRSC streams in the base plant and optimized plant. Syngas entering
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the WGS-METH section is the same in these two plants, and SNG exiting the WGS-METH
section of the base plant and optimized plant is the same in terms of exergy (4392.5 kW). The
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base plant recovers 352.62 kW of waste heat in terms of exergy, while the optimized plant
recovers 437.36 kW. The heat recovery amount (in terms of exergy) can be improved by 24.03%
by optimizing the operating conditions of the WGS-METH section and the HRSC
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simultaneously. The exergy efficiency of the coal-to-SNG process is 52.89% for the base plant,
while it’s 54.17% for the optimized plant. The exergy efficiency of the total plant has been
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improved by 1.28%. The main difference of the HRSC between the base plant and the optimized
plant is that HP steam is not generated in the base plant (see Table 9), and the highest
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temperature of the steam is 736 K in the base plant, while it is 833 K in the optimized plant.

Table 10 compares the operating conditions of the main reactors in the WGS-METH section.
The main reactor of the WGS unit (R-101) has been operated at a higher temperature in the
optimized plant than that in the base plant, which gives the WGS unit the ability to generate HP
steam. The relatively lower bypass ratio of the WGS unit ensures that the effluent of R-101 is
larger (the temperature is also higher), thereby improving the quality of waste heat from the
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WGS unit. The recycle ratio of the METH unit in the optimized plant is larger than that in the
base plant, which eliminates the steam requirements in the optimized plant. The split ratio of the
METH unit in the optimized plant is also larger than that in the base plant, allowing the outlet
temperature of R-202 to reach 973.15 K and with the higher temperature, to generate HP steam.

Table 9 Comparison of heat recovery amount between base plant and optimized plant
Case Streams P Tin~Tout Flow rates Exergy

T
-1
/MPa /K / kmol·hr /kW

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MP steam 5.49 378~736 42.20
LP steam 0.80 378~444 7.00

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Base plant 352.62
LP BFW 1 1.00 313~411 130.00
LP BFW 2 2.10 322~395 47

Optimized
HP steam
Reheat steam
LP steam
①
US 12.50
11.07
0.30
377~833
815~833
377~447
47.19
109.07
14.43
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437.36
②
plant LP steam 0.60 432-492 8.77
Demineralized water 0.20 318~373 142.01
BFW for jacket 4.50 377~423 16.94
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①Refer to the LP steam raised in LP economizer/evaporator/superheater in the HRSC

②Refer to the LP steam from WHB that is superheated in the HRSC
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Table 10 Comparison of operating conditions between base plant and optimized plant
Case Tin Tout Effluent
Bypass ratio Recycle ratio Split ratio
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/K /K /kmol·hr-1
R-101 549.9 618.4 37.48
R-201 528.4 948.9 50.67
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Base plant 0.624 0.550 0.420

R-202 534.9 948.8 37.96
R-203 603.2 809.1 34.59
R-101 638.7 683.9 49.20
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Optimized R-201 524.9 897.7 58.69

0.506 0.681 0.456
plant R-202 610.3 973.1 36.74
R-203 513.2 792.8 32.50
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5 Conclusions
The synergy between operating conditions of the coal-to-SNG process and the HRSC system are
exploited by simultaneously optimizing the operating conditions of the HRSC streams and the
coal-to-SNG process. In this paper, a novel, branched, HRSC superstructure for heat recovery
and power generation is proposed that is designed to avoid the heat exchange between process
streams in different subsystems and to realize heat integration between different subsystems

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through water/steam integration. The extended Duran-Grossmann model is used, and it covers

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two sets of cold and hot streams to match the branched HRSC superstructure; hence, the
operating conditions for the two HENs are determined simultaneously.

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The optimal exergy efficiency of the coal-to-SNG plant is 54.17%, which is improved by 1.28%
compared with the base plant. The optimal bypass ratio of the WGS unit, the recycle ratio of the

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METH unit and the split ratio of the METH unit are 0.506, 0.681 and 0.456, respectively. It is
shown that the recycle ratio of the METH unit and the split ratio of the METH unit have a
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greater influence on the exergy efficiency than the bypass ratio of the WGS unit. By analyzing
the exergy recovered by the HRSC, it is found that the heat recovery amount (in terms of exergy)
is improved by 24.03% compared with the base plant, and this gain makes the major contribution
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for the improvement of exergy efficiency.

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This branched HRSC superstructure, together with the extended Duran-Grossmann model, is
suitable for the determination of operating conditions of the chemical plant and heat recovery
network.
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Acknowledgements
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Financial support from the National Natural Science Foundation of China under Grant No.
21776087, the National Key R&D Plan under Grant No. 2017YFB0602604, and the NSFC–DFG
joint project under Grant No. 2171101208 are gratefully acknowledged.
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Nomenclature
ASU air separation unit

BFW boiler feed water

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CBGTL hybrid coal, biomass, and natural gas to liquid

CCS CO2 capture and storage system

DNS dryness of steam

F molar flow rate of species in the stream

FCp heat capacity flowrate

T
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FT total molar flow rate

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GAMS general algebraic modeling system

GSF gasification

GCC

HENs
grand composite curve

heat exchanger networks

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HP high pressure

HRAT heat recovery approach temperature

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HRSC heat recovery steam cycle

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HRSC-CPP heat recovery steam cycle and captive power plant

h enthalpy
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K chemical equilibrium constant

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QH heating utility

LP low pressure
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LVH low-value heat

M mass flow rates

METH methanation unit

METH-HEN heat exchanger network in the methanation unit

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MP medium pressure

NG natural gas

NLP nonlinear programming

ORC organic Rankine cycle

P pressure

T
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PC pinch candidate set

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QA heat absorbed by cold streams in heat recovery steam cycle

QC cooling utility

QR

QSIA
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heat released by hot streams in heat recovery steam cycle

heat load of cold streams above the pinch candidates

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QSOA heat load of hot streams above the pinch candidates

SGR sour gas removal

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SNG synthetic natural gas

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SRW set of reactors restricted by water gas shift reaction

SRM set of reactors restricted by CO methanation reaction

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SQA set of heat absorbers in heat recovery steam cycle

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SQR set of coolers in heat recovery steam cycle

T temperature
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W power

WHB waste heat boiler

WWT wastewater treatment

WGS water gas shift

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WGS-HEN heat exchanger network in the water gas shift unit

WGS-METH water gas shift and methanation unit

ZH heat deficit

Subscripts

g equipment

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pump pumps in heat recovery steam cycle

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turbine turbines in heat recovery steam cycle

recycle recycle in methanation unit

Superscripts

in inlet
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iso isentropic

out outlet
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Pch pinch candidate

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