Krist V. Gernaey, Jakob K. Huusom and Rafiqul Gani (Eds.

), 12th International Symposium on Process

Systems Engineering and 25th European Symposium on Computer Aided Process Engineering.
31 May – 4 June 2015, Copenhagen, Denmark © 2015 Elsevier B.V. All rights reserved.

Modelling and optimization of a heat integrated

gasification process
Yi Zhu, Adetoyese Olajire Oyedun, Maojian Wang, Ergys Pahija, Chi Wai Hui
Department of Chemical and Biomolecular Engineering, The Hong Kong University of
Science and Technology, Clear Water Bay, Kowloon, Hong Kong

Abstract
In this study, an iteration optimization is performed based on the Gibbs free energy
minimization approach. Further, simultaneous optimization of a heat integrated
gasification process is presented. The study shows how heat integration can improve the
overall efficiency of a gasification process. We formulated a mathematical model which
simultaneously optimizes the operating parameters and its interaction via heat
integration among the hot syngas, steam generation and the feed preheat. This allows
the model to simultaneously maximize the cold gas efficiency and also minimize the
Gibbs free energy. The model also combined gasification model with an energy
targeting model that is able to handle processes with variable stream temperatures and
flow rates.

Keywords: gasification, heat integration, simultaneous optimization.

1. Introduction
The threats of global warming and energy crises urge the need of cleaner conversion
technologies for fossil fuels such as coal. Due to the ability to mitigate the pollutions to
the environment and greenhouse gas emissions, gasification becomes a promising
conversion technology and receives increasing attention worldwide (Clayton et al.,
2007). The production of syngas from gasification, however, is a complex process that
is strongly affected by the composition of feedstock, the gasification temperature and
pressure, the amount of gasification feed water (GFW) and oxygen, etc. (Abuadala et al.,
2010).

To evaluate how these parameters would influence the gasification performance, several
equilibrium models based on Gibbs free energy have been developed to effectively
study the process in measurement of cold gas efficiency (CGE). However, most of
efforts are placed on the parametric studies through control variant methods rather than
find the optimum operating condition considering feed flow rates along with
gasification temperature. Additionally, in gasification, quite a lot of feedstock is fully or
partly oxidized to provide heat for raising the reaction temperature to a very high level,
often over one thousand degree Celsius. The recovery of the sensible heat from the hot
syngas plays a key factor in the overall energy efficiency and has seldom been taken
into account in previous studies.

In this work, the iteration algorithm is first utilized to identify the operating condition of
a gasification process corresponding to the highest CGE. Further, a heat integrated
gasification model is developed that maximizes CGE of a gasification process with
considerations of the amount of feed as well as heat integration simultaneously. A heat
integration model is established to ensure the feasibility of heat exchange among the hot
402 Y. Zhu et al.

syngas, feed streams and steam boiler. The model will be illustrated through case
studies of carbon gasification.

2. Equilibrium modelling
The gasification modelling approach is based on the theory that chemical equilibrium is
achieved when the total Gibbs free energy for a set of considered gasification products
is minimized. The total Gibbs free energy is calculated as:
‫ܩ‬௦௬௦ ൌ σே ଴ ே ே
௜ୀ௣௥௢ௗ ݊௜ ߂‫ܩ‬௙ǡ௜ ൅ σ௜ୀ௣௥௢ௗ ݊௜ ܴܶ ݈݊ ܲ ൅ σ௜ୀ௣௥௢ௗ ݊௜ ܴܶ ݈݊ ‫ݕ‬௜ (1)
Besides, the function, ‫ܩ‬௦௬௦ , also needs to satisfy the elemental and heat balance. The
energy balance for the gasification process is calculated using Eq. (9).
݊‫ܪ‬௙ǡ௙௨௘௟ ൅ ‫ܪ‬௣ ሺܶ௜௡ ሻ ൅ σே ே
௜ୀ௥௘௔௖௧ ݊௜ ‫ܪ‬௙ǡ௜ ሺܶ଴ ሻ ൌ σ௜ୀ௣௥௢ௗ ݊௜ ‫ܪ‬௙௔ǡ௜ ሺܶ௢௨௧ ሻ (2)
As suggested by de Souza-Santos, the enthalpy of formation for the solid fuel reactant
can be calculated as shown in Eq. (10) (de Souza-Santos, 2004).
‫ܪ‬௙ǡ௙௨௘௟ ൌ ‫ ܸܪܮ‬൅ σே
௜ୀ௣௥௢ௗ ‫ܪ‬௙ǡ௜ ሺܶ଴ ሻ (3)
where ‫ ܸܪܮ‬is the lower heat value in kJ/kmol and ‫ܪ‬௙ǡ௜ is the enthalpy of formation of
ith gas under complete combustion of the solid fuel. In the calculation, the outlet
temperature of syngas is taken as the gasification temperature. The initial temperature of
reactants ሺܶ଴ ሻ is assumed to be 298.15 K. Thus, preheating heat represents the enthalpy
change from 298.15 K of all reactants.

In addition, the minimization of Gibbs free energy is subject to elemental balance by:
σே ே
௞ୀ௥௘௔௖௧ ݊௞ ܽ௞ ൌ σ௞ୀ௣௥௢ௗ ݊௞ ܽ௞ (4)
The constrain now is to find a set of ݊௜ and a gasification temperature (ܶ) in Eq. (1)
which can minimize the total Gibbs free energy of the system while satisfying heat
balance (Eq. (2)) and elemental balance (Eq. (4)). The direct minimization is
accomplished by generalized reduced gradient nonlinear method. The reaction pressure
is pre-specified. Providing initial values, the minimization of Gibbs free energy
generates a set of ݊௜ and determines the reaction temperature simultaneously.

3. Optimization through iteration

Based on the developed equilibrium model based on Gibbs free energy minimization,
the iteration algorithm is utilized to identify the optimum operating condition. The
details of calculation procedure are illustrated in Figure 1.

Figure 1. Calculation procedure of iteration

Modelling and optimization of a heat integrated gasification process 403

The upper limit of O2 feed can be set as the stoichiometric amount for complete
combustion. The value of OH2O/C at 1 is considered as the upper limit for GFW feed.
Although the approach is direct, we should also notice that the iteration process will be
exponentially increased if the heat integration is also included or the high fidelity is
required.

4. Simultaneous optimization of a heat integrated gasification process

To improve the optimization process, an approximation model which can consider the
heat integration along with the gasification process parameters is developed.

Assuming that coal contains only carbon, gasification of coal consists of several major
reactions (Li et al., 2001): partial and complete combustion, carbon-steam, boudouard,
methanation and water-gas shift reactions.

Table 1. The major reactions and equilibrium constants at different temperatures

1,000 K 1,200 K 1,400 K 1,600 K
C + 0.5O2 = CO 2.89E+10 3.04E+09 5.94E+08 1.72E+08
CO + 0.5O2 = CO2 1.65E+10 57,535,774 1,023,261 50,350
C + H2O = CO + H2 2.52 38.43 267.56 1,141.03
C + CO2 = 2CO 1.75 52.75 580.46 3,423.81
C + 2H2 = CH4 0.10 0.02 0.00 0.00
CO + H2O = CO2 + H2 1.44 0.73 0.46 0.33

As shown in Table 1, the calculated equilibrium constants indicate that:

(1) Gasification is in favour of high temperature to promote complete conversion of
carbon. High temperature facilitates the production of H2 and CO instead of CO2.
(2) With sufficient supply of oxygen, the reactions tend to produce more CO than CO2.
The CO2 formation is only subject to the energy balance.
(3) At reaction temperature above 1,200K, CH4 production can be eliminated.

Based on the above analysis, the question is whether the Gibbs free energy of the
product gas can be simultaneously minimized while maximizing CGE. In order to
ascertain this, Eq. (1) is removed from the developed equilibrium model to form a
“simultaneous model”. The simultaneous model is used to maximize CGE at a specific
reaction temperature between 1,000K to 1,800K by varying oxygen and steam feed at 1
bar pressure. The reaction pressure is fixed since it should not have a strong influence to
the product yield or composition. The elevated pressure in commercial gasifiers was
mainly for reducing equipment size (Phillips, 2006).

At each reaction temperature, the optimized feed rates from the simultaneous model are
used as inputs to the equilibrium model that minimizes Gibbs free energy. Reaction
temperature is recalculated from the equilibrium model and compared to that from the
simultaneous model. As shown in Figure 2, results (reaction temperature) from both
models are identical when reaction temperature above 1,400K. These results are verified
by Aspen Plus Gibbs reaction model.

The tests indicate that when the reaction temperature is above 1,400K, maximizing CGE
will simultaneously minimize the Gibbs free energy of the product gas. This observation
greatly simplifys the solution procedure. Having the reaction temperature at above
404 Y. Zhu et al.

1,400K also coincide with the latest commercial entrained-flow coal gasifiers that are
operated at 1,473 K-1,873 K (Collot, 2006).

1800

1600
Temperature (Aspen results)

1400

1200

1000
1000 1200 1400 1600 1800
Temperature (simultaneity pre-specified)
Figure 2. Temperature profile of simultaneous model and equilibrium model.

On the other hand, sensible heat utilization is evaluated between feed preheating and
steam generation. Ensuring feasible heat integration imposed new constraints to the
problem. The model of heat integration ensures the feasibility of heat transfer. In this
work, the simultaneous optimization model proposed by Duran and Grossmann (Duran
and Grossmann, 1986) is applied to simultaneously optimize the gasification process
and the amount of energy recovery. The model is modified to accommodate process
streams with phase change.

5. Case study
The feeding rate of coal (with 100% carbon) is fixed at 10,000 kg/h and reacts with
oxygen and GFW at 1 bar. HP steam is produced at (832 K, 125 bar) for export and the
cooled syngas is utilized for electricity generation in combined cycle. Minimum
approach temperature of heat exchange is set at 10K. Two cases are presented in the
following sections. Case 1 shows the approach to identify optimum feed flow rates and
reaction temperature by iteration. In Case 2, flow rates as well as stream temperatures
are optimized simultaneously with consideration of heat integration. The heat
integration model is considered in Case 2 to ensure the feasible heat recovery.

5.1. Case 1
In this case, the optimization is conducted with gasification temperature ranging from
1,273 K to 1,873 K. An iterative approach is applied to maximize CGE by varying the
feed flow rates while Gibbs free energy is minimized. Reaction temperature is
converged at 1,273 K with feeding 3,909 kg/h GFW and 10,009 kg/h O2. The highest
CGE reaches 87.11%. Since require iteration, the solution process is slow and easily
trapped at local optimum.
Modelling and optimization of a heat integrated gasification process 405

To further study the gasification, OH2O/C vs CGE in two typical temperatures are plotted
in the Figure 3. As shown in it, the highest CGE for each operating temperature appears
at the carbon conversion turning point where the carbon happens to be completely
converted. Before or after it, CGE has a lower value due to the negative effects brought
by the wasted carbon residue or the excessive GFW respectively. Because in the
equilibrium model, the higher operating temperature means the more energy is wasted
on raising the temperature. Therefore, the optimizations converged at the allowed
lowest temperature, 1,273 K, which saves the most heat.

Figure 3. CGE and carbon conversion efficiency at 1,273 K and 1,873 K

5.2. Case 2
The flow rates of gasification process are optimized directly through simultaneous
model while the sensible heat recovery through feed preheating as well as HP steam
generation is also considered. The gasification temperature is allowed to be varied
between 1,673 K and 1,873 K. Considering reasonable endurance of heat exchanger
(Gupta et al., 1999), we set the related temperature limits as shown in Table 2.

Table 2. Parameters of the heat integrated gasification process.

Parameters Lower temperature limit (K) Upper temperature limit (K)
O2 298 700
GFW 298 700
Gasification temperature 1673 1873

Optimum solution of Case 2 is shown in Figure 4 where 9,863.73 kg/h O2 and 3,903.29
kg/h GFW are fed and preheated to 700 K. Reaction temperature is converged to 1,673
K with CGE reaches 87.95%. The difference comes from the higher feed temperatures
which are both optimized at 700 K. As a result, O2 supply is reduced dramatically to
9,863.73 kg/h. Meanwhile, due to the lower oxygen feed, more GFW is fed that resulted
in more H2.
406 Y. Zhu et al.

298 K
Carbon 10000 kg/h
700 K Gasifier Hot Syngas 1673 K
298 K 9863.73 kg/h 23767.02 kg/h
O2 9863.73 kg/h Q= 1070.14 kW H2 20.65%
700 K CO 79.35%
298 K 3903.29 kg/h CO2 0.00%
Heat
H2O 3903.29 kg/h recovery Q= 3502.16 kW H2O 0.00%
network 832 K, 125 bar CGE 87.95%
HP steam 298 K 7372.08 kg/h
generation 7372.08 kg/h Q= 6952.71 kW HP steam
Cooled 464 K generation
syngas 23767.02 kg/h Electricity
generation
Figure 4. Process flowsheet of Case 2.

6. Conclusion
Effectively utilize the sensible heat from the syngas for feed preheating or steam
generation can reduce oxygen demand and improve the overall gasification
performance. In this study, a novel model is formulated to simultaneously optimize the
gasification conditions, flow rates and preheating levels of the feeds and the utilization
of the hot syngas. When reaction is at temperatures above 1,400K, maximizing CGE
automatically results gas products with minimum Gibbs free energy. This observation
reduces the complexity in solving the bi-level optimization problem and reduces the
chances of being trapped at local optimum. The gasification model is integrated with a
heat integration model that guarantee feasible reaction on one hand and optimize the
feed flow rates and preheating levels on the other. Case studies have demonstrated the
effectiveness of the integrated model.

Acknowledgements
The authors gratefully acknowledge the support from Hong Kong RGC -GRF grant
(613513) and the UGC-Infra-Structure grant (FSGRF13EG03).

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