Chemical Engineering Journal 429 (2022) 132442

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Chemical Engineering Journal

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

Speeding up turbulent reactive flow simulation via a deep artificial neural

network: A methodology study
Yi Ouyang a, Laurien A. Vandewalle a, Lin Chen b, Pieter P. Plehiers a, Maarten R. Dobbelaere a,
Geraldine J. Heynderickx a, Guy B. Marin a, Kevin M. Van Geem a, *
a
Ghent University, Laboratory for Chemical Technology, Technologiepark 125, 9052 Gent, Belgium
b
AVGI, Technologiepark Zwijnaarde 122, 9052 Gent, Belgium

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

Keywords: Turbulent reactive flow simulation often requires accounting for turbulence-chemistry interactions and the sub-
Turbulent Reactive Flow Simulation grid phenomena. Their complexity leads to a trade-off between computational efficiency on one hand and
Artificial Neural Network computational accuracy on the other. We attempt to bridge this gap by coupling the power of machine learning
Lagrangian PDF Method
with the turbulent reactive flow simulation, specifically in the form of a deep artificial neural network. The
Turbulence-Chemistry Interaction
Lagrangian Monte Carlo method is chosen as a demonstration case as it is one of the most accurate models for
Sub-Grid Effect
turbulent reactive flow simulation, but also one of the most time-consuming. The workflow consists of training
data generation, deep neural network construction, and implementation in ANSYS-Fluent, followed by an
evaluation of model accuracy and efficiency, which results in an order of magnitude faster simulation without
loss of accuracy thanks to our data-driven deep neural network. This approach can be of universal relevance in
speeding up time-consuming models in the field of reactive flow simulation.

closure can be reduced to that of the scalar covariance [2,12]. Two

1. Introduction
Turbulent reactive flows are an interdisciplinary and multiscale topic
in chemical reactor technology and combustion engineering, in which
the interaction of turbulent flow, turbulent mixing, and chemistry is a
complicating factor [1–3]. For the purpose of computational fluid dy­
namics (CFD) simulation of turbulent reactive flow, one has to carefully
consider the closures for the chemical source term as both chemical time
scale and flow time scales should be taken into account. A spectrum can
be found in Fox’s pioneering work [2], roughly dividing the reaction
into three categories: slow chemistry, finite-rate chemistry and fast
chemistry, and in that order, the dominating factor for the reaction
process shifts from intrinsic kinetics to the turbulence-chemistry inter­
action (TCI). Essential in this respect is the TCI based model for an ac­
curate simulation. Typical examples of reaction processes affected by
TCI are combustion [4,5], mostly in gas phase, and micromixing [6–9],
mostly in liquid phase.
In general, TCI refers to the interaction between the turbulence
enhanced mixing of the species and the reaction process affecting the
flow [10,11], the key for TCI models being the closure of the chemical
source term in the transport equations. Based on Reynolds averaging,
representative approaches have been widely adopted for that purpose:
(1) moment closure schemes and (2) probability density function (PDF)
closure schemes. As far as the first-order moment closure is concerned,
the Finite-Rate Model (FRM) can be classified into this category as the
reaction source term is calculated based on the Arrhenius equation and
mean scalar values, but it ignores TCI. In 1977, Magnussen and Hjert­
ager [13] proposed the Eddy-Dissipation Model (EDM). Combing FRM
and EDM, most CFD codes employ EDM as an upper limit for fast
chemistry simulation to slow down the reaction rate. As turbulent-
characteristic properties are included in EDM to calculate the reaction
rate, TCI is taken into account. The Eddy-Dissipation Concept Model
(EDCM) was subsequently proposed as an extension of EDM. It assumes
reactions occur within the turbulent fine scales [14]. EDM and EDCM are
widely used in turbulent reactive flow simulation owing to their high
computational efficiency. As mean scalar values (such as the Reynolds
averaging based mean species concentration) are used, they can be
considered as belonging to the first-order moment closure category.
Higher-order moment closures can be found in Fox’s work [2], one latest
example of which relates the covariances of species concentration to the
variance of the mixture fraction [15], as will be discussed in the sub­
sequent section.

* Corresponding author at: Technologiepark 125, 9052 Gent, Belgium.

E-mail address: Kevin.VanGeem@UGent.be (K.M. Van Geem).

https://doi.org/10.1016/j.cej.2021.132442

Available online 14 September 2021

1385-8947/© 2021 Elsevier B.V. All rights reserved.
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

Nomenclature Sct turbulent Schmidt number,Sct = μt

ρDt
U Favre mean fluid velocity vector, m/s
A& B empirical constants in the EDM, respectively equal to 4.0 ν kinematic viscosity, m2/s
and 0.5 vi stoichiometric coefficient of speciesi
Cconv , Cdiff &Cmix convection, diffusion and mixing local time step 〈⋯〉 mean value
constants, 0.5 is adopted for all of them 〈⋯|⋯〉 conditional probability
CD1 & CD2 model constants in the EDC model, respectively equal to
0.134 and 0.5 Greek letters
Cj molar concentration of reactant species j, kmol/m3 Δt local time step in the Lagrangian PDF method
C*i molar concentration of reactant species j determined by Δtconv , Δtdiff andΔtmix convection, diffusion and mixing local time
Arrhenius rate in the EDC model, kmol/m3 steps
Cμ turbulence model constant, equals to 0.09 ε turbulent kinetic energy dissipation rate, m2/s3
Dt turbulent diffusivity, m2/s μt turbulent viscosity, Pa⋅s
F Favre joint PDF of composition ξ characteristic length fraction of the fine structure in the
f mixture fraction EDC model
Jk,i molecular diffusion flux vector, kg/(m2⋅s) ρ density, kg/m3
( )12
k turbulent kinetic energy, m2/s2 τη Kolmogorov time scale, τη = ∊ν , s
kr reaction rate constant, m3/(kmol⋅s)
Φ(f) beta distribution of the mixture fraction
L characteristic length of computational cell, square root of
ψi composition space vector for speciesi
cell area for 2D cells, m
Mi molecular weight of speciesi Abbreviations
n rate exponent of speciesj ANN Artificial Neural Network
N number of reactant species CFD Computational Fluid Dynamics
Ri net rate of species i production of the Lagrangian PDF DQMOM-IEM Direct quadrature method of moments combined with
method, kg/(m3⋅s) the interaction-by-exchange-with-the-mean model
2
Ret turbulence Reynolds number,Ret = kν∊ EDM Eddy-Dissipation Model
Ri,EDC net rate of species i production of the EDC model, kg/(m3⋅s) EDCM Eddy-Dissipation Concept Model
Ri,EDM net rate of species i production of the EDM, kg/(m3⋅s) FRM Finite-Rate Model
Ri,FR net rate of species i production of the Finite-rate model, kg/ PDF Probability Density Function
(m3⋅s) RANS Reynolds-averaged Navier–Stokes
Ri,β− PDF net rate of species i production of the β-PDF model, kg/ TCI Turbulence-Chemistry Interaction
(m3⋅s) SGE Sub-Grid Effects

Unlike the moment closure, the Probability Density Function closure
scheme uses distribution functions instead of lumped values to describe
scalars in a computational grid cell, to account for Sub-Grid Effects
(SGE) [16]. Two representative methods can be found: (1) the
presumed-PDF method and (2) the full or transport PDF method. As its
name suggested, the former assumes a distribution shape in advance for
the PDF, such as β-distribution based models [17–19] and δ-function
based models [8,9]. Although a presumed distribution form is an
effective way to close the scalar covariance term, the shortcoming is the
presumption itself, which leads to different model performance [20].
The transport PDF method, however, requires no presumption of the
distribution shape by introducing the Monte Carlo method to solve the
PDF transport equations [21]. The Monte Carlo algorithm defines
notional particles in computational grids to represent the PDF and take
the SGE into account. Since the turbulent characteristic properties, such
as the turbulent kinetic energy and dissipation rate, are involved when
tracking the Lagrangian notional particles, the TCI eventually plays a
crucial role in the closure of the chemical source term. It is worth
mentioning that solving the transport PDF could also be under the
Eulerian framework, examples being the direct quadrature method of
moments combined with the interaction-by-exchange-with-the-mean
micromixing model (DQMOM-IEM) and stochastic fields method
[2,22,23]. The Lagrangian Monte Carlo PDF method is by far believed to
be one of the most accurate methods for turbulent reactive flow simu­
lation but at the same time one of the most time-consuming ones
[24,25]. In fact, to some extent, the low computational efficiency of the
model limits its broad application [3].
A possible way to tackle this limitation is via machine learning,
especially in the form of an Artificial Neural Network (ANN). Deep
learning, i.e. an ANN containing a certain number of hidden layers, has
shown to be very performant in many diverse fields [26–30]. After
providing relevant variables as inputs and desired variables as outputs,
deep ANN links the two via learning, i.e. credit assignment to weights
and bias when minimizing properly defined loss functions [31]. Deep
ANN exhibits powerful capabilities in data regression and pattern
recognition in general and in chemical (engineering) research in
particular [32]. Examples include transport scalars prediction [33,34],
species properties prediction [35,36], synthetic route design [37,38],
optimization framework construction [39], flow pattern classification
[40] to name a few. In addition, it has also been successfully coupled to
CFD simulations [31,41–47]. Particularly, a deep ANN works quite well
in approximating numerical solutions for underlying partial differential
equations (PDEs) [48–50]. Since the reaction rate in turbulent reactive
flow is always highly nonlinear, it is possible to use a deep ANN to
calculate e.g. the chemical source terms present in the PDEs corre­
sponding to the transport PDF method. In this case, a data-driven
approach is expected to obtain a fast simulation of turbulent reactive
flow based on the accuracy of the full/transport PDF method, which is
also the main motivation of this work. As pointed out in a recent
research of developing a digital twin of a combustion furnace, the
concept of the reduced-order modelling is essential for CFD results being
used in real time prediction owing to the quick response of reduced-
order models compared to CFD simulations [51]. As such, ANN-based
strategies can be considered as an important approach for developing
the reduced-order model.
In this work we will demonstrate a novel approach to build a
framework for coupling a deep ANN and turbulent reactive flow simu­
lations and investigate the maximum speedup of the simulations by the

2
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

generated ANN in respect to the accuracy. Specifically, the Lagrangian fine structure can be expressed based on the turbulent Reynolds number
PDF method is chosen as the target model due to its high accuracy Ret as follows:
combined with a high computational cost. Essential for the success are ( )14 ( )14
the input/output data collection from the TCI model, ANN architecture/ ξ=
3CD2 1
(3)
training, and implementation in the solver framework. The target TCI
2
4CD1 Ret
model is thus replaced by the ANN-based model, and the prediction
Between the fine structures and surroundings, mass transfer occurs to
performance as well as a speedup factor are assessed. Strengths and
supply the reactant species to the reaction region, i.e. the fine structure.
weaknesses are discussed.
The time scale for the mass transfer process is estimated by the Kol­
mogorov time scale τη as follows:
2. Turbulence-chemistry interaction models
( )12
CD2
Simulating turbulent reactive flow requires a proper closure for the τ= τη (4)
3
chemical source term, which usually translates in the need for a model to
calculate the reaction rate for each computational cell in either an And finally, the net source of species i based on EDCM is expressed as:
explicit or implicit manner. In what follows, a summary of how to ξ2 ( )
calculate the reaction rate, expressed in the form of the net rate of Ri,EDC = Mi ( ) Ci* − Ci (5)
τ 1 − ξ3
species production in various TCI models is given.
In the above equations, CD1 and CD2 are model parameters. The
turbulence Reynolds number Ret is defined as kνε , where ν is the kinematic
2
2.1. Finite-Rate Model
( )12 2
viscosity. The Kolmogorov time scale τη is calculated as νε . ξτ repre­
As discussed above, the FRM does not account for TCI, but it is a good
starting point to discuss the reaction rate calculation. The FRM is based sents the intra-cell mass transfer rate between the fine structures and
on the Arrhenius equation and the general reaction rate expression. For surroundings. ξ3 represents the volume fraction of the fine structures
an irreversible elementary reaction, a general form of the net source of that can be used to calculate the average scalars of a cell. Note that the
species i due to reaction is given by: expressions of the intra-cell mass transfer rate and average scalars of a
cell can take different forms [52–54], but Eq. (5) is the form used in this
∏
N
( )n
Ri,FR = vi Mi kr Cj (1) work. C*i is determined by applying the Arrhenius rate at fine structure
j=1 conditions after reacting over the time scale τ. Ci is the mean concen­
tration at the cell level.
where vi is the stoichiometric coefficient of species i, Mi the molecular
weight of species i, kr is the rate coefficient, N represents the number of
2.4. β-PDF model
reactant species, n is the rate exponent of species j, and Cj is the molar
concentration of reactant species j.
The β-PDF model is one of the representative models for the
It’s important to note that the Cj term represents the mean state
presumed-PDF method. The reaction rate can be calculated in the form
concentration if a Reynolds-averaged Navier–Stokes (RANS) equations
of Eq. (1), but the species concentration follows a beta distribution
based turbulence model is applied, hence why it is considered as a first-
instead of a moment closure. However, if multiple variables (e.g. two or
order moment closure. The concentration fluctuation or any turbulent
more species) are involved for chemistry, developing a multi-
characteristic parameter is not accounted for. The mean state concen­
dimensional PDF becomes difficult [3]. One solution is to introduce a
tration is also used in the EDM and EDCM model.
new variable–the mixture fraction to replace the reactant composition
state in each cell. For instance, in Baldyga et al.’s work, the net source of
2.2. Eddy-Dissipation Model species i is given by [17,18]:
∫1
The EDM takes the turbulent characteristic properties into account ∏N
( )n
Ri,β− = vi Mi kr 〈 Cj 〉 = vi Mi kr C(f )Φ(f )df (6)
and assumes the reaction is turbulent mixing-limited [13]: PDF
j=1 0
( )
ε
Ri,EDM = vi Mi A min
C1 C2 Cj Cp
, , ⋯, , B (2) In Eq. (6), the notation of 〈⋯〉 denotes the mean value. f is the
k v1 v2 vj vp mixture fraction, a conserved scalar quantity defined by a linear trans­
formation of the species concentration, representing a local equivalence
where A and B are empirical constants, ε is the turbulent kinetic energy ratio [2]. Φ(f) is the beta distribution of the mixture fraction. Most
dissipation rate, k is the turbulent kinetic energy, and the subscript p importantly, there are two parameters that determine the shape of the
represents the product species. The limiting factors of reactant and beta distribution, which needs closure. Different closure approaches
product species (which generally means the limiting factor of flame have been reported [15,17], but no matter what the closure is, the tur­
spread in combustion simulation) are described by taking the minimum bulent characteristic properties play an important role in determining
values in the equation. According to Eq. (2), the intrinsic kinetics are not the two parameters.
considered in the EDM. The mean reaction rate is only a function of
turbulent characteristic properties and species concentration. Therefore,
a commonly used method is to calculate both Eqs. (1) and (2) and choose 2.5. Lagrangian PDF method
the smaller one as the actual net production rate i.e. chemical source for
the corresponding cell. The transport PDF method does not assume the shape of the PDF a
priori, but derives the PDF transport equation from the Navier-Stokes
equation [55]:
2.3. Eddy-Dissipation Concept Model
( ) ( )
∂ ∂ ∂ ∂ ρμt ∂F ∂ 1 ∂ ∂Jk,i
(ρF) + (ρUk F) + (ρRi F) = + ρ〈 |ψ 〉F
EDCM assumes that a cell contains turbulent fine structures and ∂t ∂xk ∂ψ i ∂xk Sct ∂xk ∂ψ i ρ ∂xk ∂xk
surroundings, and that reactions take place in the region of the fine (7)
structures where the turbulent kinetic energy dissipates [14]. The latter
accounts for the SGE in EDM. The characteristic length fraction of this where Ri is the net source of species i due to reaction, F is the Favre joint

3
Y. Ouyang et al.
PDF of composition, ρ is the mean fluid density, Uk is the Favre mean
fluid velocity vector, ψ i is the composition space vector for species i, Sct
is the turbulent Schmidt number and Jk,i is the molecular diffusion flux
vector. The notation of 〈P|Q〉 represents the conditional probability of
event P. Particularly, μt is the turbulent viscosity, calculated from a
2
RANS model, such as ρCμ k∊ , used in this work (Cμ is a turbulence model
constant which is usually taken to be 0.09 [56]).
Solving Eq. (7) could be under the Eulerian framework, one example
being the DQMOM approach [2,22,23], but a presumption of the PDF
form is still made for in this case. A more accurate way to solve the PDF
transport equation is by employing the Monte Carlo algorithm and
defining a certain number of notational particles in each cell, which is
known as the Lagrangian PDF method. The particles have mass,
depending on the cell mass in which the particles are located. Generally,
the principal steps in the Lagrangian PDF method are summarized as
follows [2]: (1) advancing the Finite-volume code, i.e. solving the mo­
mentum transport equation and turbulence model (such as a RANS
model) to get the velocity and turbulent scalars (such as turbulent vis­
cosity in Eq. (7)) at each cell; (2) interpolating the scalars to the intra-
cell particle based on the particle’s location; (3) advancing the PDF
code based on the Monte Carlo algorithm. For the step 3, the particles
move through the computational domain due to convection, mixing and
reaction. Several models were proposed to adjust the particle composi­
tion to account for particle mixing, such as the Modified Curl Model [57]
and the Euclidean Minimum Spanning Tree Model [58]. The latter is
used in this work. The Arrhenius rate is applied at the particle level. The
PDF is thus described by the intra-cell particle information, similar to
constructing a histogram to estimate the PDF. As a result, the Lagrangian
PDF method simulates the reaction in an indirect way, i.e. through re­
action within each of the notional particles. The mean reaction rate at
the cell level can then be calculated by the mass-weighted average
scalars of the intra-cell particles. The Lagrangian PDF method is theo­
retically by far the most accurate model to take into account the SGE and
TCI, but the intra-cell particle tracking makes the model extremely time-
consuming.
For a proper numerical efficiency two important choices need to be
made in the Lagrangian PDF method: the particle number per cell and
the particle local time step [59]. Note that increasing the particle
number per cell or decreasing the particle local time step will reduce
statistical errors but will always increase computational cost. To obtain a
reliable prediction, one should increase the particle number per cell to
make sure the simulation results are independent of the particle number
[2]. In general, the particle number is roughly in the range of 20–200
[24,59–61]. In this work, the number of particles per cell is set to 50. As
for the local time step, it is determined by:
( )
Δt = min Δtconv , Δtdiff , Δtmix (8)
where:
L structing and training the deep ANN based on the input layer of the cell
Δtconv = Cconv (9)
U data and the output layer of the mean reaction rate, (4) compiling the
L2
Δtdiff = Cdiff (10)
Dt
k
Δtmix = Cmix (11)
∊
In Eqs. (9)–(11), L is the characteristic length of a cell, U is the mean
velocity, and Dt is the turbulent diffusivity. Without the constants Cconv ,
Cdiff and Cmix , Eqs. (9)–(11) provide the characteristic time scale of flow
convection, turbulent diffusivity and turbulent mixing. The 3 constants
usually take values of less than 1 to determine the local time step to
advance the intra-cell particle. They are all set as 0.5 in this work, in line
with previous research [59].
To sum up, if no TCI is considered, the mean reaction rate is only a
4
Chemical Engineering Journal 429 (2022) 132442
function of reaction rate coefficient and species concentration. However,
taking TCI into account leads to various approaches, such as direct
closures in the EDM or EDCM, or indirect ways where the PDFs are
determined first, after which they are coupled with the mean reaction
rate calculation. Regardless of which approach is used, the turbulent
characteristic properties are very important in determining the chemical
source term. As the intention of this work is to use ANN to replace and
speed up certain TCI models, understanding the determining factors is
essential for selecting the ANN input features.
3. Methods
3.1. CFD model
The focus of this work is to develop a methodology of using a data-
driven ANN to replace and speed up certain TCI models, specifically
the Lagrangian PDF method. Therefore, a simple example case is built to
demonstrate the workflow and prove its viability. Fig. 1 shows the ge­
ometry of the example case. Inlet a and inlet b, both with a width of 2
mm, introduce species A and B into the reaction domain. Due to the
regular geometry, a structured mesh can be easily created.
The model reaction used in this work is given below:
(12)
k
A+B→C
After the species A and B are injected, the mixing of species A and B
takes place in the computational domain, and the reaction occurs once
the two species contact, generating species C. The rate equation is given
by r = kCA CB , where k = 1000m3 /(kmol∙s).
The FRM, EDCM and the Lagrangian PDF method as well as the
subsequent established ANN-based model are implemented to simulate
the above case. In addition, other numerical models have been kept
identical for different simulations. For instance, given the high Reynolds
number in the computational domain (2.0 × 104 –8.0 × 104), the
standard k-ε turbulence model is adopted for all simulations. For a
straightforward comparison, the direct integration chemistry solver is
applied for all cases. All the species concentrations are monitored during
the calculation and the iteration does not stop until the species profiles
remain steady. The convergence criteria for all equation residuals are set
to 1.0 × 10-6.
3.2. Methodology
Fig. 2 shows the proposed methodology of using a deep ANN to
replace and speed up the Lagrangian PDF method under the ANSYS-
Fluent framework. The procedure briefly consists of (1) performing
simulations of the training cases using the Lagrangian PDF method, (2)
exporting the cell data and particle data of the simulation results and
further linking the cell data, e.g. turbulent characteristic properties and
species concentration, to the particle data of reaction rate, (3) con­
ANN, i.e. the weights, bias and activation functions in Fluent using user-
defined functions and (5) performing simulations using the ANN-based
model to calculate the reaction rate of each cell. The detailed descrip­
tion is as follows:
Fig. 1. 2D geometry of the simulation case.
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

Fig. 2. Schematic of the deep ANN methodology for modeling turbulence chemistry interaction.

1. Prior to an ANN architecture, a training dataset is needed. Hence, the
first step is to perform simulations of several turbulent reactive flow
cases using the Lagrangian PDF method and export the data both at
the cell level and at the particle level.
2. The exported cell data contains the velocity fields, turbulent char­
acteristic properties, species concentration, etc. at locations of all the
computational cells. The exported particle data is similar. Based on
the spatial location of the cells and particles, the cell data can be
linked to intra-cell particle data by employing the ball tree algorithm
[62,63] and the Chebyshev distance [64]. Most importantly, the
mean reaction rate of each cell can be then calculated based on the
corresponding intra-cell particles.
3. The training data is then fed to an ANN, the architecture of which is
shown in Fig. 2. The turbulent kinetic energy, dissipation rate, and
the mass fractions of reactant A & B at the cell level are chosen as the
input layer data. The output layer consists of the mean reaction rate
as discussed in step 2. To obtain a proper prediction accuracy, the
Keras Tuner [65] is applied to search for an optimal set of hyper­
parameters of the ANN architecture, i.e. a proper combination of
various activation functions, the number of hidden layers and neu­
rons. As the number of combinations is huge, the hyperband tuning
algorithm in the Keras Tuner is invoked to search for high-performing
candidate models, which is done by using an adaptive resource
allocation strategy. For example, in the initial stage, only a few
epochs are specified to select the best half candidate models for the
next round, similar to a sports championship style bracket. After a
thorough evaluation 3 hidden layers with respectively 32, 64, 128
neurons are employed. The rectified linear unit (ReLU) and sigmoid
are chosen as the activation functions, which introduces a degree of
nonlinearity into the network. A MinMaxScaler [66] is used to scale
the input and output data to a range of 0 and 1. The python deep
learning library Keras [67] with the backend of Tensorflow [68] is
used to construct the deep ANN.
4. After a deep ANN with acceptable accuracy is obtained, the weights,
bias and activation functions of the deep ANN are translated into
4. Results and discussion
4.1. Training and test set generation
Table 1 gives an overview of the cases that are simulated for
generating the training and test set. Various combinations of inlet ve­
locity, mass fraction and geometry are explored. The specified inlet
velocities in Table 1 correspond to a Reynold number range of 2.0 × 104
–8.0 × 104, which ensures the flow is turbulent. In addition, considering
the rate constant and the specified inlet reactant concentrations, the
reaction characteristic time scale is at least one order smaller than the
turbulence time scale for all the cases in Table 1, which ensures a fast
chemistry [2] and the TCI is the dominating factor for the reaction
process. The Lagrangian PDF method has been implemented for all the
cases, but only the exported data from Cases 1–5 is used for the ANN
training data. In other words, the conditions of Cases 6–11 are our test
set, which will be used to evaluate the performance of the ANN-based
model. In particular, Cases 5–9 are specified to evaluate the prediction
performance for different operating conditions while Cases 10–11
evaluates different geometries. More information on specifying the
training and test set is provided in the Supplementary Information. The
inlet velocity, mass fraction and geometry will have a direct impact on
the turbulence flow and reaction process, and eventually on the con­
centration profile of the product species C.
4.2. Grid independence test
Fig. 3 shows a grid independence test based on the mass fraction
distribution of the product species C along the horizontal axis. The
Table 1
Dataset construction: Training and test set.
Case # Dataset Inlet velocity Mass Mass
type [m/s] fraction of A fraction of B

user-defined functions (UDFs), which is further compiled in Fluent. Case-1 Training 10 0.1 0.1
To be more specific, the UDFs invoke the cell level data of the tur­ Case-2 Training 10 0.2 0.2
Case-3 Training 10 0.05 0.05
bulent kinetic energy, dissipation rate, and the mass fractions of
Case-4 Training 5 0.1 0.1
reactant A & B and return the reaction rate to the corresponding cell. Case-5 Training 20 0.1 0.1
5. When performing a simulation based on the above UDFs, the mean Case-6 Test 10 0.075 0.075
reaction rate of each computational cell is determined by a well- Case-7 Test 10 0.15 0.15
trained deep ANN. Case-8 Test 15 0.075 0.075
Case-9 Test 10 0.15 0.075
Case-10 (different Test 15 0.075 0.075
geometry)
Case-11 (different Test 15 0.075 0.075
geometry)

5
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

4.4. ANN-based model to predict training dataset

Fig. 5 shows the mass fraction distribution of the product species C in

the computational domain based on various models. Once species A and
B mix in the domain, after which reaction occurs and generates species
C. Particularly, the Lagrangian PDF method shows a local feature of
species distribution as it is the intra-cell particle composition that de­
termines the concentration distribution. To further quantitatively
compare the simulation results of various models, Fig. 6 shows a com­
parison based on all the training dataset cases. Note that the discussion
in this section is not about justifying which TCI model gives the best
accuracy, in fact all of them are widely used in literature or practical
engineering simulations, but to prove the ANN-based model can replace
and further speed up the TCI simulations with ideally an order of
magnitude. As shown in Fig. 6, the differences in the models themselves
lead to widely varying results. Only based on the comparison of the
training dataset cases (Cases 1–5), the ANN-based model agrees well
with the Lagrangian PDF method. In other words, the ANN-based model
Fig. 3. Grid independence test based on the mass fraction of product C and can replace the Lagrangian PDF method and shows reasonable accuracy
the FRM.

results are obtained based on the FRM. As the total cell number in­
creases, the distributions tend to converge, especially in the region
where the mixing and reaction initially occur. To quantify the result of
the independence test, the grid convergence index (GCI) is applied [69].
Grid-2/Grid-4 and Grid-4/Grid-5 are chosen as two sets of fine/coarse
grids as both sets of grid spacing ratios are equal to 2. Based on the GCI
approach and the average mass fraction values, the GCI2/4 and GCI4/5
are calculated to be 0.05008% and 0.24427%, respectively, indicating
the solutions are in the asymptotic range of convergence [69]. There­
fore, the grid with 14,364 cells is adopted in this work (Grid-2 in Fig. 3).

4.3. ANN training

Fig. 4 shows the parity plot of the ANN prediction. As discussed in

Table 1, Cases 1–5 are used to generate the training dataset. Each case
has 14,364 cells and in total there are 71,820 data points fed to the ANN.
10% of the data is split off from the training dataset and is used as the
validation dataset to determine the proper number of ANN training
epochs. Therefore, Fig. 4a contains 64,638 data points while Fig. 4b
contains 7182 data points. A root mean square error is calculated as the
loss function for both the training dataset and split validation dataset,
which are 8.70 × 10− 3 and 8.50 × 10− 3, respectively, indicating a
reasonable prediction accuracy is achieved. Given such low loss function
values, Fig. 4 also proves that the selected input layer features give
proper information to predict the mean reaction rate of each cell.
Fig. 5. Mass fraction distribution of the product species C for Case-1: (a) FRM;
(b) EDCM model; (c) Lagrangian PDF method; (d) ANN-based model.

Fig. 4. Parity plot for the reaction rate prediction: (a) training dataset; (b) split dataset for validation.

6
Y. Ouyang et al.
Fig. 6. Comparison of the FRM, EDCM, Lagrangian PDF method and ANN-based model: (a) Case-1; (b) Case-2; (c) Case-3; (d) Case-4; (e) Case-5.
(accuracy here means how close the result of the ANN-based model is to
the result of the Lagrangian PDF method, not validation based on
experimental data), and more importantly, this level of accuracy is not
obtained by the other considered TCI models such as the EDC model.
4.5. ANN-based model to predict testing dataset
A key question that remains is if the model can simulate new con­
ditions next to replicate data that it was trained for. Fig. 7 shows the
results of the ANN-based model simulating Cases 6–9, which are
different from the operating conditions of the training cases. Fig. 8
shows the results of simulating Cases 10–11, which have different ge­
ometries. To evaluate the model performance, Cases 6–11 are simulated
by the Lagrangian PDF method as well. Meanwhile, Fig. 9 summarizes
and compares all the data points of the results when using the
Lagrangian PDF method and the ANN-based model, i.e. the data points
of the two models in Figs. 6, 7 and 8 for all the training and test cases.
Both training cases and testing cases are within ± 10% deviation,
meaning overfitting is avoided and the ANN-based model can predict
7
Chemical Engineering Journal 429 (2022) 132442
unseen data. Results show that the ANN-based model remains in good
agreement with the target model, indicating the ANN-based model is
able to simulate new conditions after training with a limited number of
cases. From a practical point of view, one can use a similar approach to
employ deep ANN(s) to replace the Lagrangian PDF method or even
other time-consuming TCI models for specific application cases.
As long as suitable training data is available, an ANN-based model is
essentially independent of the cases, indicating this methodology can be
applied to other practical simulations. While the methodology itself can
be of universal relevance, the generated ANN in this work is not, as the
selection of training dataset, input parameters and architecture of the
ANN can be case dependent. For instance, in a case with different
reactant species/species number and reactor/burner geometries, the
ANN construction and the training process should be re-run to fit the
specific case. However, the procedure to build this framework, i.e.
generating a training dataset, specifying input parameters, constructing
the deep ANN and compiling the ANN in ANSYS-Fluent, should be the
same as presented in this work. The first step would be choosing a set of
proper training data cases, preferably the cases with representative
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

Fig. 7. ANN-based model to predict turbulent reactive flow under various operating conditions: (a) Case-6; (b) Case-7; (c) Case-8; (d) Case-9.

Fig. 8. ANN-based model to predict turbulent reactive flow for different geometries: (a) Case-10; (b) Case-11.

conditions in the full map of operating conditions. In practical uses of
the methodology in this study, the method of experimental design can be
used for the training cases, e.g., orthogonal experimental design. The
training cases that cover the operating condition range will improve the
prediction performance of the ANN-based method as the necessary in­
formation can be learned by the ANN. Next, after driving a well-trained
ANN model, the fundamental model can be replaced to some extent
while maintaining accuracy. For example this will become very effective
when it comes to parametric analysis and reactor/burner geometry
optimization, as both of them require a large number of similar simu­
lations [70]. Actually, the original motivation of this work is to increase
the computational efficiency of the Lagrangian PDF method when per­
forming parametric analysis in a liquid–liquid micromixing simulation
work [7], in which the TCI is essential for an accurate simulation.
5. Speedup factor assessment
To further quantify the performance of the ANN-based model it is
necessary to evaluate the computational efficiency. The Lagrangian PDF
method is considered as our reference. The procedure for calculating the
speedup factor start with simulating Cases 6–11 via the Lagrangian PDF
method and the ANN-based model. Identical convergence criteria are set
for both models. The calculations are carried out on a serial processor of
Intel core i7-8650U. The calculation time is recorded from the initiali­
zation of the simulation to achieving a steady-state result. The speedup
factors for Cases 6–11 are then calculated by normalizing the efficiency

8
Y. Ouyang et al. Chemical Engineering Journal 429 (2022) 132442

Fig. 9. Comparison of the simulation results based on the Lagrangian PDF method and the ANN-based model: (a) training Cases 1–5; (b) test Cases 6–11.

of the Lagrangian PDF method to 1, meaning the average speedup factor

is calculated by the ratio of the average time consumed when using the
Lagrangian PDF method and the average time consumed when using the
ANN-based model in the simulation of Cases 6–11. Fig. 10 shows the
average speedup factor with an error bar of standard deviation. An
average speedup factor of 14.1 is achieved by using the ANN-based
model.
It should be noted that the computational efficiency of the
Lagrangian PDF method highly depends on the particle number per cell
and the local time step. Nevertheless, the particle number and local time
step adopted in this work should be considered representative, as dis­
cussed in previous sections. On the other hand, the efficiency of the
ANN-based model highly depends on the ANN architecture, i.e. the
number of layers and neurons. For instance, the ANN architecture shown
in Fig. 2 contains 10,721 trainable parameters (weights and biasses).
The efficiency of the ANN model coupled in Fluent is inversely pro­
portional to the number of trainable parameters, which implies that
when the number of parameters is halved, the computational efficiency Fig. 10. Speedup factor of the ANN-based model.
of the ANN-based model will be doubled. However, a certain number of
trainable parameters are needed to maintain the ANN prediction Declaration of Competing Interest
performance.
The authors declare that they have no known competing financial
6. Conclusions interests or personal relationships that could have appeared to influence
the work reported in this paper.
While the Lagrangian PDF method is regarded as one of the most
accurate models for turbulent reactive flow simulation, its low compu­ Acknowledgments
tational efficiency hinders its broad application. Research on the closure
of the chemical source term leads to various approaches to calculate the Yi Ouyang gratefully acknowledges financial support from a post­
mean reaction rate of each computational cell, showing diverse model doctoral fellowship from the Research Foundation – Flanders (FWO)
performance. As machine learning is showing great potential in grant number 1273421N. This work was performed in the framework of
approximating the numerical solutions for underlying partial differen­ the Catalisti clusterSBO project HBC.2019.0109 within the MOONSHOT
tial equations, an approach to accelerate the time-consuming turbulent innovation program. The research leading to these results has received
reactive flow simulation that keeps a reasonable accuracy is a big step funding from the European Research Council under the European
forward. In this work a data-driven deep ANN has been constructed that Union’s Horizon 2020 research and innovation programme /ERC grant
replaces and speeds up the Lagrangian PDF method by an order of agreement n◦ 818607.
magnitude. Based on a limited number of training cases, the ANN-based
model is capable of calculating the mean reaction rate under new Appendix A. Supplementary data
operating conditions and different geometry cases. Results show that
reasonable accuracy is obtained with respect to the target model, which Supplementary data to this article can be found online at https://doi.
could not be realized by the other TCI models considered. Overall, the org/10.1016/j.cej.2021.132442.
data-driven ANN-based model is in this specific case 14 times faster than
the Lagrangian PDF method. It is believed that employing this meth­ References
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