Chemical Engineering and Processing 88 (2015) 29–36

Contents lists available at ScienceDirect

Chemical Engineering and Processing:

Process Intensification
journal homepage: www.elsevier.com/locate/cep

Intensification of a hydrotreating process to produce biojet fuel using

thermally coupled distillation
Claudia Gutiérrez-Antonio a, *, Fernando Israel Gómez-Castro b , Salvador Hernández b ,
Abel Briones-Ramírez c
a
Facultad de Química, Universidad Autónoma de Querétaro, Cerro de las Campanas s/n, Las Campanas, Querétaro 76010, Mexico
b
Departamento de Ingeniería Química, División de Ciencias Naturales y Exactas, Universidad de Guanajuato, Campus Guanajuato, Noria Alta s/n, Guanajuato
36050, Mexico
c
Exxerpro Solutions, Av. del Sol 1B Interior 4B Col. El Sol, El Tintero, Querétaro 76113, Mexico

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

Article history: Aviation sector contributes with 2% of the total CO2 emissions, and predictions estimate that air traffic
Received 21 July 2014 will duplicate in the next 20 years. The development of aviation fuel from renewable feedstocks has been
Received in revised form 4 September 2014 identified as the most promissory strategy to reduce CO2 emissions. Recently, a process to produce
Accepted 6 December 2014
aviation fuel from renewable feedstock has been proposed, which converts vegetable oil through
Available online 10 December 2014
hydrogenating, deoxygenating, isomerization and selective hydrocracking to renewable fuels, which are
purified later.
Keywords:
In this work, we propose the intensification of the hydrotreating production process through the use of
Biojet fuel production process
Renewable aviation fuel production process
thermally coupled distillation for the purification stage; moreover, we incorporate a turbine in order to
Synthetic paraffinic kerosene generate electricity with the energy contained in the outlet stream of the reactor. Also, the purification
Process intensification stage is optimized through a multiobjective genetic algorithm, coupled to a process simulator. Results
show that the use of thermally coupled distillation reduces the energy requirements in the separation
stage. Also, energy can be generated as a result of the conditioning of the stream that is fed to the
distillation train.
ã 2014 Elsevier B.V. All rights reserved.

1. Introduction 1) Technological improvements in engines and aircraft structures.

In the transport sector, the aviation industry is responsible for
2% of the total annual emissions of CO2, about 705 million of tonnes
in 2013 [1]. The overall percentage is small; however, it is
estimated that by 2020 global emissions of international aviation
will be approximately 700% higher than that in 2005, even if the
engine efficiency will increase by 2% per year [2]. The International
Civil Aviation Organization, ICAO, forecasts that air traffic will grow
at a rate of 4.8% per year until 2036 [3], this finding is consistent
with the reports of the International Air Transport Association,
IATA, which estimates that air traffic will double by 2020,
compared to 2005. Therefore, both IATA as ICAO have established
a four-pillar strategy to combat climate change problem [5], which
includes:
* Corresponding author. Tel.: +52 442 192 1200.
E-mail address: claugtez@gmail.com (C. Gutiérrez-Antonio).
2) Operational improvements by on line optimization of flight
paths.
3) Market-based measures, basically emissions trading.
4) Development of alternative fuels.
IATA estimates that this strategy will allow a 50% reduction in
CO2 emissions by 2050, relative to 2005 emissions levels, and, also,
neutral growth in CO2 emissions from 2020 [6]. From the above
alternatives, IATA identifies the development of biofuels as one of
the most promising ways to significantly reduce the greenhouse
gas emissions. The aviation fuel from renewable feedstocks, also
known as biojet fuel, must be drop in, since changes in motor
structures are not desirable; thereby, it has to present the same
properties and chemical composition of the jet fuel [4]. Thereby,
compounds known as synthetic paraffinic kerosene (SPKs) have
been developed, and they are very similar to the jet fuel in
energetic density and physical properties [7]. The SPKs contains
small amounts of sulfur, generating less contaminant emissions in
comparison with the conventional jet fuel. The only inconvenient

http://dx.doi.org/10.1016/j.cep.2014.12.002
0255-2701/ ã 2014 Elsevier B.V. All rights reserved.
30 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36

Fig. 1. Hydrotreating process for production of biojet fuel.

of the SPKs is that they do not contain aromatics, so that they must 2. Modelling and intensification of hydrotreating process:
be used in mixtures up to 50% of biojet fuel with the fossil jet fuel purification
according to standard ASTM D7566 [8].
The SPKs can be produced from biomass in, at least, two ways The hydrotreating process consists of the transformation
[9]. The first one considers the gasification of the biomass, which is of vegetable oil through hydrogenating, deoxygenating, isomer-
introduced to a Fischer–Tropsch process where the SPKs are izing and selective hydrocracking to generate renewable fuels,
generated [10–12]. The second one considers the extraction of which are purified later [13]. Thereby, the process is integrated by
vegetable oils, which are chemically modified to produce the SPKs two consecutive reactors and a conventional distillation
[13]. In both cases, purification of the product stream is required to sequence.
obtain the biojet fuel. The study of hydrotreating reaction of vegetable oils is of recent
In 2009, a process to produce aviation fuel from interest; experimental research has been performed for soybean
renewable feedstocks through hydrotreating was proposed [20,21], rubber seed [22], canola [23], pine [23], sunflower [24],
[13]; the process, developed by UOP Honeywell, considers rapeseed [25,26,27] and cottonseed [28]. With base on the
the transformation of vegetable oil to generate hydrocarbons reported data in the literature, we consider a typical composition
using two consecutive reactors and a distillation column (or a for the stream that is fed to the distillation train. Table 1 shows the
train of distillation columns), as shown in Fig. 1. The hydrotreating composition of the renewable hydrocarbons, which consists in
process to produce biojet fuel has been proved at pilot plant light component, those in the range of the boiling point of fossil jet
level [7], using vegetable oils as renewable feedstocks [14]. fuel, and those in the range of green diesel; it is worth to mention
UOP Honeywell has produced several thousand gallons of that this feed composition is in agreement with the data reported
renewable jet fuel from a variety of feedstocks, including first by McCall et al [13]. The generated hydrocarbon renewable stream,
generation oils such as palm and soybean oils, as well as second which leaves the reactive section at 240
C and 60 bar [20–28], is
generation oils like camelina, jatropha and algae oils [15–17]. fed to a distillation sequence to generate three products: light
Several demonstration flights has been realized [18], proving hydrocarbons (C3–C7), biojet fuel (C8–C16) and green diesel
that the biojet fuel produced through hydrotreating of vegetable (C17 and C18). However, the high pressure of the outlet reaction
oils reaches the specifications of fossil jet fuel; also, the fuel stream must be reduced before it is fed to the distillation sequence.
was approved for commercial passenger-bearing flights by In order to utilize the energy contained in the outlet reaction
ASTM International on July 1st, 2011 [19]. However, it is stream we use a turbine, so that energy can be generated in the
important to mention that there is not so much information process.
available for the kinetic model or type of catalyst involved in the The purification of the renewable fractions of hydrocarbons is
hydrotreating process of UOP Honeywell due to confidential performed in a distillation sequence. We analyze both, a
issues.
In this work, we propose the intensification of the
hydrotreating process to produce biojet fuel through the use of Table 1
thermally coupled distillation columns, for the purification of Composition of the renewable hydrocarbons feed stream.
a typical hydrocarbon stream generated in the reactive section
Component Flow stream
of the process; also, we incorporate a turbine in order to (kg/h)
generate electricity with the energy contained in the stream that
n-Propane to n-heptane 10.1255
leaves the reactor system. To ensure low-energy designs for n-Octane to n-tetradecane 21.6061
the distillation systems, the purification stage is optimized n-Pentadecane 0.2157
through a multiobjective genetic algorithm with constraints, n-Hexadecane 0.2299
which is coupled to Aspen Plus process simulator; so, we generate n-Heptadecane 19.0796
n-Octadecane 20.1919
results considering the complete and rigorous model of i-Pentadecane 0.06901
the process. The use of thermally coupled distillation columns i-Hexadecane 0.0736
allows getting a reduction in energy requirements in the i-Heptadecane 6.1055
separation stage. Also, energy can be generated in the process i-Octadecane 6.4614
as a result of the conditioning of the stream that is fed to the
Total 84.1582
distillation train.
 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36 31

conventional and a thermally coupled distillation sequences in
order to compare the energy consumption and capital costs
associated with these sequences. The conventional sequence is
proposed in the original hydrotreating process, and the thermally
coupled distillation sequences are proposed in this work in order to
decrease the overall energy consumption of the process, making it
more sustainable and reducing costs of utilities.
The analyzed distillation sequences are conventional and
thermally coupled distillation sequences: direct conventional
(DC), indirect conventional (IC), direct thermally coupled (DTC),
indirect thermally coupled (ITC), Petlyuk sequence (PS) and
Dividing Wall Column (DWC). The conventional and thermally
coupled distillation sequences are designed using a multiobjective
genetic algorithm with constraints, coupled to Aspen Plus process
simulator, through the use of the RadFrac module, and accelerated
through neural networks [28].
The optimal design problem for conventional distillation
sequences involves the simultaneous minimization of the number
of stages and the heat duty in each column of the sequence; this
minimization is constrained by the required recoveries and
purities in each product stream:
MinðQ i ; Ni Þ
subject to
y m  xm
where Qi and Ni are the heat duty and the number of stages of
the column i, while ym and xm are vectors of obtained and required
purities for the m components, respectively. For all distillation
sequences the objectives are the heat duty and the number
of stages of each distillation column of the sequence; thereby,
we manage four objectives for DC, IC and ITC, while three
objectives are managed for DTC, PS and DWC. This minimization
implies the manipulation of several variables, both continuous and
integer, which are presented in Table 2. Note that since the product
streams flows are manipulated, the recoveries of the key
components in each product stream must be included as a
restriction; for all sequences we consider recoveries of 99% in the
key components.
The algorithm generates a set of optimal designs that represent
the best trade-off between the selected objectives; it manages
several objectives simultaneously, manipulating integer and
continue variables, and the link to Aspen Plus allows considering
the complete model of the distillation columns. The algorithm
works as follows: the first generation is created from an initial
design, and all individuals are sent to Aspen Plus to simulate them
and get data about objectives and constraints; then, individuals are
ranked in subpopulations, according to the number of satisfied
constraints. The best individuals are selected to be the new parents
of the second generation, and so on; the process ends when the
maximum number of generations has been reached. For the
distillation sequences analyzed, the objectives are the number of
stages (associated with capital costs) and energy consumption
(associated with operating costs) in each column, achieving the
specified recoveries and purities.
From here, we will call conventional processes to those that just
consider the purification through conventional distillation sequen-
ces, Fig. 2. Also, we will call intensified processes to those that
consider the turbine and the thermally coupled distillation
sequences, Fig. 3. Thereby, we compare two conventional hydro-
treating process with four intensified hydrotreating process in
terms of energy consumption (associated with operation costs)
and number of stages (associated with capital costs).
3. Discussion of results
The optimal designs for both conventional and intensified
sequences for the purification stage of the hydrotreating process
(1)
are presented in this section. The results and their discussion are
presented in the following way. First, the results of the
conventional process for purification of biojet fuel are presented,
and later those of the intensified processes.
3.1. Conventional process for production of biojet fuel
As mentioned before, the conventional process for the production
of biojet fuel considers two consecutive reactors followed by a
conventional distillation sequence. This configuration corresponds
to the original process of hydrotreating developed by UOP Honeywell
[13]. Since in the original process of hydrotreating there is not a clear
indication of which type of conventional distillation is used [13], we
analyzed both direct and indirect conventional distillation sequen-
ces in order to find the best sequence in terms of energy consumption
(associated with operation costs) and number of stages (associated
with capital costs). The best sequence is considered as the base case
for comparison with the proposed intensified processes.
Then, we apply the Fenske–Underwood–Gilliland–Kirkbride
shortcut methodology to generate initial designs of both
conventional schemes; these designs are used as initial solutions

Table 2
Manipulated variables to generate the Pareto fronts of conventional and thermally coupled distillation sequences.

Conventional Thermally coupled

DC IC DTC ITC PS DWC

Reflux ratio in column 1, R1 X X X X
Feed stage in column 1, NF,1 X X X X X X
Number of stages in column 1, N1 X X X X X X
Reflux ratio in column 2, R2 X X X X
Feed stage in column 2, NF,2 X X
Number of stages in column 2, N2 X X X X X X
Distillate stream flow of column 1 D1 D D
Distillate stream flow of column 2 D2 D2 S D2 D2
Bottoms stream flow of column 2 B2 S S S
Product stage of liquid interconnection flow FL in column i,NFL,i NFL1,C1 NFL1,C2 NFL1,C2
Feed stage of vapor interconnection flow FV in column i, NFV,i NFV1,C1 NFV1,C2
Vapor interconnection flow, FV FV1 FV2 FV2
Feed stage of liquid interconnection flow FL in column i, NFL1,i NFL1,C1 NFL2,C2
Product stage of vapor interconnection flow FV in column i, NFV,i NFV1,C1 NFV2,C1
Liquid interconnection flow, FL FL1 FL1 FL1

Total 8 8 9 9 12 9
32 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36
Fig. 2. Conventional hydrotreating process for production of biojet fuel considering the reactive section within the conventional distillation sequences: (a) direct (DC); (b)
indirect (IC).
for the multiobjective genetic algorithm with handling constraints,
coupled to Aspen Plus simulator, and accelerated through neuronal
networks [28]. The model used in the simulation is Radfrac, so the
complete set of MESH equations is used to generate the optimal
designs. Also, for the calculation of liquid–vapor phase equilibrium
we use the Chao–Seader correlation [32]. The parameters used for
the optimization of conventional distillation schemes are 1000 in-
dividuals with 60 generations; these parameters were obtained
through a tuning process where the number of individuals and
generations is changed until we found the minimum number of
generations and individuals from which there is no significant
change in the Pareto front.
Fig. 4 shows the Pareto front generated for conventional
distillation schemes, and Table 3 contains three selected designs
for each sequence: minimum energy consumption, minimum
number of stages and similar number of total stages of direct and
indirect scheme. It is worth to mention that all designs that
integrate the Pareto front are optimal including the minimum heat
duty, the minimum number of stages and all designs between
these extremes; also, all designs satisfy the requirements in
purities and recoveries specified in the optimization problem.
From Table 3 we can observe that the minimum heat duty is
presented in the conventional direct sequence, also reached with
fewer stages than those required in the indirect scheme. However,
also from Fig. 4 we can observe that there is a zone where both
Pareto fronts overlap, when heat duties are between 23,500 and
26,000 W. From this zone, we selected two designs of similar total
number of stages in order to analyze the difference in the heat duty
for each sequence. The design of indirect sequence is slightly better
than the design of the direct, since 1.2% less energy is required to
achieve the separation. Therefore, the best sequence in the
conventional process is the indirect one.
Summarizing, in the conventional process to purify biojet fuel,
the energy required to perform the separation is around 23,213 W,
132 being the total number of stages of the indirect conventional
distillation sequence.
3.2. Intensified process for production of biojet fuel
As mentioned before, the intensified process for production of
biojet fuel considers two consecutive reactors followed by a
turbine, which decreases the pressure of the stream leaving the
isomerization reactor before it is fed to the thermally coupled
distillation sequence. We analyzed four thermally coupled
sequences: direct, indirect, Petlyuk sequence and Dividing Wall
Column in order to find the best sequence in terms of energy
consumption (associated with operation costs) and number of
stages (associated with capital costs). These sequences are
 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36 33

Fig. 3. Intensified hydrotreating process for production of biojet fuel considering the implementation of a turbine within the thermally coupled distillation sequences: (a)
direct (DTC); (b) indirect (ITC); (c) Petlyuk (PS); (d) Dividing Wall Column (DWC).

Fig. 4. Pareto front of conventional distillation sequences.

34 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36

Table 3 3.2.2. Purification

Selected designs from Pareto front of conventional distillation sequences.
As it has been mentioned before, we consider direct and
Direct indirect thermally coupled distillation sequences along with the
N1 N2 Q
Petlyuk distillation sequence and the Dividing Wall Column for
(W) the purification of the renewable hydrocarbon stream that leaves
Minor heat duty 35 96 21,971.87
the reactive section. We apply the section rearrangement
Similar number of total stages 51 79 23,493.97 methodology [29] to generate initial designs for direct and indirect
Minor number of stages 33 57 29,746.97 thermally coupled sequences, with base on the designs generated
for conventional distillation sequences with Fenske–Underwood–
Indirect
Gilliland–Kirkbride shortcut methodology. Moreover, the initial
N1 N2 Q solutions for Petlyuk distillation sequence and Dividing
(W)
Wall Column were obtained with a shortcut methodology based
Minor heat duty 190 52 23,208.40 on the concept of minimum distance [30], which involved
Similar number of total stages 106 26 23,213.44
information about the feed composition and the easy separation
Minor number of stages 111 61 26,015.00
index of the mixture, as defined by Tedder and Rudd [31]. These
designs are used as initial solutions for the multiobjective genetic
algorithm with handling constraints, coupled to Aspen Plus
simulator, and accelerated through neuronal networks [28]. The
compared with the best sequence of the conventional process. It is model used in the simulation is Radfrac, so the complete MESH
worth to mention that in the optimization of the Petlyuk sequence equations are used to generate the optimal designs. Also, for the
we consider that each interconnection stream can be located in a calculation of liquid–vapor phase equilibrium we use the
different stage; in other words, it is possible to have four Chao–Seader correlation. The parameters used for the optimiza-
interconnection streams instead of two. tion of conventional distillation schemes are 1000 individuals with
90 generations; these parameters were obtained through a
3.2.1. Turbine tuning process where the number of individuals and generations
As it was mentioned before, the conditions of the renewable is changed until we found the minimum number of generations
hydrocarbon stream that leaves the second reactor must be and individuals from which there is no significant change in the
decreased in order to be fed to the intensified distillation sequence. Pareto front.
Then, in order to feed the hydrocarbon stream to the distillation Fig. 5 shows the Pareto front generated for thermally coupled
sequence in adequate conditions, we propose a turbine to take distillation schemes, and Table 4 contains three selected designs
advantage of the pressure on the stream. In the simulation, we for each sequence: minimum energy consumption, minimum
choose a hydraulic turbine from the pressure changers models number of stages and similar number of total stages of direct and
available in Aspen Plus. Such equipment allows using the kinetic indirect scheme. It is worth to mention that all designs that
energy contained in the high-pressure stream in order to produce integrate the Pareto front are optimal including the minimum heat
electricity. Simulations show that 74.5 W are generated during the duty, the minimum number of stages and all designs between
process; which can contribute to decrease the overall operating these extremes; also, all designs satisfy the requirements in
costs of the process. purities and recoveries specified in the optimization problem.

Fig. 5. Pareto front of thermally coupled distillation sequences.

 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36 35

Table 4 optimal intensified designs, we choose from each Pareto front

Selected designs from Pareto front of thermally coupled distillation sequences.
designs with around 130 total stages, which are already presented
Direct in Table 4. The direct thermally coupled sequence presents the
N1 N2 Q
minimum heat duty (18,358.08 W) with 129 total stages, while the
(W) indirect thermally coupled scheme with 130 stages requires 10.5%
Minor heat duty 116 27 18,354.93
more energy. For the separation of the renewable hydrocarbons,
Similar number of total stages 101 28 18,358.08 both Petlyuk sequence and dividing wall column are not a
Minor number of stages 60 15 19,295.40 promising option, since 69.8% and 147% more energy is required
in comparison with the direct thermally coupled distillation
Indirect
sequence. It seems that the restriction in the location of the
N1 N2 Q interconnection streams in the Dividing Wall Column has a strong
(W)
impact in the energy consumption. If we compare the best
Minor heat duty 119 23 20,294.59 intensified sequence (direct) with the best conventional sequence
Similar number of total stages 102 28 20,295.06
(indirect) we found that for the same number of total stages (130)
Minor number of stages 80 7 22,321.61
the intensified sequence requires 21% less energy than the
Petluyk sequence conventional one.
Summarizing, in the intensified process to produce biojet fuel
N1 N2 Q
(W) the energy required to perform the separation is around 18,358 W,
130 being the total stages of the direct conventional distillation
Minor heat duty 21 215 29,154.20
Similar number of total stages 15 107 31,175.85 sequence. Moreover, 75 W are generated during conditioning of the
Minor number of stages 20 84 53,304.24 stream leaving the reaction section and entering into the
distillation train; although this energy represents only 0.4% of
Dividing wall column
the total energy required for separation it certainly contributes to
N1 N2 Q having a more sustainable process, with a reduced carbon
(W) footprint. Also, the reduction in energy requirements lead to
Minor heat duty 14 140 269,300.80 minor production costs of biojet fuel.
Similar number of total stages 12 124 270,265.30
Minor number of stages 16 82 293,601.46
4. Concluding remarks

We proposed the intensification of a hydrotreating process of

From Table 4 we can observe that the minimum heat duty is
presented in the direct thermally coupled scheme, followed by the
indirect scheme; nevertheless, the minimum energy requirements
are higher in the Petlyuk sequence, but those of the dividing wall
column are in another magnitude order. These data are clearly
showed in Figs. 5 and 6. In order to make a comparison between all
biojet fuel, through the use of thermally coupled distillation
columns for the purification stage; also, we incorporated a turbine
in order to generate electricity with the energy contained in the
stream that leaves the reactor system. Also, as a result of the
modification of conditions of the stream of the reactor that will be
fed to the distillation sequence, about 75 W was generated in the
process. The implementation of thermally coupled distillation

Fig. 6. Pareto front of thermally coupled distillation sequences without Dividing Wall Column.
36 C. Gutiérrez-Antonio et al. / Chemical Engineering and Processing 88 (2015) 29–36
sequences allows getting a reduction of 21% in the energy
consumption of the separation stage, in comparison with the
original process. The reduction in energy requirements lead to a
more sustainable process and minor production costs of biojet fuel.
Acknowledgements
Financial support provided by Universidad Autónoma de
Querétaro and Exxerpro Solutions for the development of this
project is gratefully acknowledged.
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