Chemical Engineering Journal 431 (2022) 133771

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Chemical Engineering Journal

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

Computational fluid dynamics (CFD), artificial neural network (ANN) and

genetic algorithm (GA) as a hybrid method for the analysis and
optimization of micro-photocatalytic reactors: NOx abatement as a
case study
Jéssica O.B. Lira, Humberto G. Riella, Natan Padoin *, Cíntia Soares *
Laboratory of Materials and Scientific Computing (LabMAC), Department of Chemical and Food Engineering, Federal University of Santa Catarina, Campus Universitário
Reitor João David Ferreira Lima, 88040-900 Florianópolis/SC, Brazil

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

Keyword: In this work the hybrid CFD-ANN-GA method is proposed as a tool for the analysis and optimization of micro-
Micro-photocatalytic reactor photocatalytic reactors, taking NOx abatement as a case study. Initially, a 3D CFD model of the microreactor
Gas-phase allowed the investigation of the effects of residence time, light intensity, relative humidity and initial NO con­
Computational fluid dynamics (CFD)
centration on the performance of the photocatalytic reaction. Then, an artificial neural network (ANN) was
Artificial neural network (ANN)
Genetic algorithm (GA)
implemented to predict the overall conversion of NO in the micro device. Different ANN structures were
developed using data from 256 CFD simulations, and the best structure was chosen based on the performance
factors MSE, RMSE and R2. Moreover, a genetic algorithm (GA) was used to find the optimal operating conditions
that maximize the NO conversion. The best ANN model consisted of a feed-forward back-propagation structure
with three layers and 11 neurons in the hidden layer (4:11:1), logsig-logsig transfer function and training
through the Levenberg-Marquardt algorithm. This network presented a high predictivity (R2 = 0.9997), and it
was used for optimization by GA to determine the optimum conditions. Based on the optimization results, full NO
conversion (100%) was achieved when the residence time, light intensity, relative humidity and initial con­
centration were 2.12 s, 10 W⋅m− 2, 10%, and 2.09 × 10− 8 kmol⋅m− 3, respectively. Furthermore, the most
influential variable on the NO conversion prediction was the residence time, with a relative importance of
48.97%. The ANN was then modified to yield two outputs: NO consumption rate and pressure drop. All pa­
rameters were kept the same, except the number of neurons in the hidden layer (17). GA was then applied to a
multi-objective optimization, aiming to maximize the NO consumption rate while minimizing the pressure drop
in the system. The optimal set of operating conditions in this scenario was found based on a Pareto front analysis.

1. Introduction
Recently, the application of microchannel technology has attracted
great attention due to its potential for intensifying chemical processes.
The remarkable characteristics of the microreactors are mainly due to
the compactness of the reaction environment [1,2]. These devices have
advantages over larger-scale reactors such as high surface-to-volume
ratio, short molecular diffusion distances, laminar flow and excellent
heat and mass transfer [3,4].
The combination of microreactors with heterogeneous photo­
catalysis technology translates into greater homogeneity of photon flux
over the entire device compared to conventional reactors [5,6].
Moreover, due to its short diffusion distance, the reagent solution meets
the catalyst film more efficiently, leading to better performance in
immobilized heterogeneous photocatalytic reactions. In fact, extensive
research has been reported on the application of microchannel reactors
in liquid phase photocatalytic processes [7–10].
However, the application of microreactors for the photocatalytic
degradation of the pollutant in the gas phase still receives little atten­
tion, even with a very attractive potential to provide high conversions
due to its small size [11–14]. Versborg et al. [11] investigated the
oxidation of CO and methanol using silicone microreactors sealed with a
Pyrex cap and TiO2 impregnated on the inner walls. Costa Filho et al.
[14] applied heterogeneous photocatalysis technology to a milli-
photoreactor known as NETmix for n-decane degradation. Fernández-

* Corresponding authors.
E-mail addresses: natan.padoin@ufsc.br (N. Padoin), cintia.soares@ufsc.br (C. Soares).

https://doi.org/10.1016/j.cej.2021.133771
Received 3 October 2020; Received in revised form 21 May 2021; Accepted 18 November 2021
Available online 23 November 2021
1385-8947/© 2021 Elsevier B.V. All rights reserved.
J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

Nomenclature p(Ω’ →Ω) Phase function

R Universal gas constant (m2⋅s− 2⋅K− 1)
A⊥ Cross-section area of the channel (m2) R2 Correlation coefficient
ANN Artificial neural network Re Reynolds number (-)
b1 Bias of the hidden layer RH Relative humidity (%)
b2 Bias of the output layer RMSE Root-mean-square error
Cin
i Inlet concentration of species i (kmol⋅m− 3) RI Relative importance (%)
( )
Dij Molecular diffusion coefficient for the pair i - j (m2⋅s− 1) − ri’’ S Reaction rate for species i per unit of area (kmol⋅m− 2⋅s− 1)
Di,m Molecular diffusion coefficient for the specie i in the s Spatial coordinates
mixture (m2⋅s− 1) S Selectivity (%)
E Irradiance (W⋅m− 2) T Temperature (K)
e− Electron T’ Transpose operator
F Generic body forces ub Upper bound
I Identity matrix vin Inlet velocity (m⋅s− 1)
Iλ Intensity of photons (W⋅m− 2⋅μm sr-1) VMR Volume of the microreactor (m3)
IW Weight of the hidden layers Xi Conversion of species i (%)
IF Intensification factor α Kinetic parameter related to irradiance (m2⋅W− 1)
GA Genetic algorithm ΔP Pressure drop (Pa)
h+ Hole κa,λ Volumetric absorption coefficient
Intrinsic kinetics for species i (m⋅s− 1) Wavelength (μm)
’’
ki λ
Ki Intrinsic equilibrium parameters (m3⋅kg− 1) μ Mixture dynamic viscosity (kg⋅m− 1⋅s− 1)
lb Lower bound μ(i,j) Dynamic viscosity of each species in the mixture
LW Weight of the output layers (kg⋅m− 1⋅s− 1)
Mw Mixture molecular weight (kg⋅kmol− 1) ρ Density of the mixture (kg⋅m− 3)
Mw,i Molecular weight of species i (kg⋅kmol− 1) σ ij Lennard-Jones characteristic length of the pair i-j (Å)
MSE Mean squared error Ω Angular coordinates
OF Objective function ΩD Collision integral
Pabs Absolute pressure (kg⋅m− 1⋅s− 2) τ Residence time (s)
pout Outlet pressure (Pa)

Catalá et al. used a capillary microreactor [15] and a commercial
microreactor [16] for the elimination of volatile organic compounds
(VOCs) in low concentrations, with propene being the model compound.
An in-depth investigation of the transport phenomena that occur
within microchannels is necessary to improve the design of photo­
microreactors. Thus, mathematical models based on computational fluid
dynamics (CFD) can stand out because they have advantages of time
saving and high precision, in addition to the ability to calculate physical
quantities that are difficult to measure experimentally [17,18]. There­
fore, once the model has been validated, the prediction of the effect of
different operational configurations and the evaluation of different
geometric configurations can be readily performed with virtual pro­
totypes, before experimentation and construction of any physical
equivalent. However, most studies dealing with photocatalytic micro­
reactors (in liquid and/or gas phase) investigate the effects of individual
parameters on the efficiency of the photocatalytic degradation of the
model compound (i.e., evaluate the process efficiency by varying only
one parameter and keeping the others constant). Thus, the effects of the
interactions between the variables are not observed. However, it is
desirable to have a model to analyze and quantify the performance of
photocatalytic reactors considering the interaction effects of all relevant
operational parameters, converting a real-world problem into an opti­
mization problem.
It is important to develop effective optimization algorithms capable
of providing satisfactory results with robustness and efficiency [19].
Although a variety of optimization methods have already been devel­
oped, some of them can be highlighted as gradient-based optimization
(GBO) and optimization based on metaheuristics [19,20]. Gradient-
based optimization methods have long been used to solve problems of
continuous optimization. These algorithms use the sensitivity (gradi­
ents) of the objective functions and constraints to determine the direc­
tion of the search toward the optimal performance, using an iterative
procedure to find the lowest value [21]. However, the presence of
multiple local optima makes the global optimization difficult for this
type of method because the GBO can get stuck in a local minimum
[22,23]. It can be solved if the search starts sufficiently close to the
global optimum of the objective function or using multiple starting
points [24]. These methods have been used in a wide range of applica­
tions to solve different types of optimization problems. The most popular
gradient-based optimization methods include Newton’s method [25],
the Quasi-Newton method [26], the Levenberg-Marquardt algorithm
[27], and the conjugate direction method [28]. In addition, many of
these optimization methods are already implemented in finite volume
and fine element method-based solvers, e.g., the Optimization Module
available in COMSOL® Multiphysics providing a general interface to
calculate optimal solutions to engineering problems [29]. On the other
hand, in recent decades, different optimization methods based on met­
aheuristics have been developed and used to simulate biological phe­
nomena. Some examples are the genetic algorithms (GA) [30], particle
swarm optimization (PSO) [31], among others. GA was derived from the
Darwin’s theory of evolution [32]. PSO is an evolutionary search algo­
rithm that is similar to the GA technique for optimization considering a
population of individuals (a “swarm”) rather than concentrating on a
single individual implementation [33]. Therefore, the strategy of finding
optimal objective parameters is employed by the evolution of possible
parameters under the influence of the entire population [20]. Optimi­
zation methods based on metaheuristics are typically stochastic in na­
ture, improving a randomly generated set of initial designs in a pseudo-
random way. In addition, these methods have mechanisms that allow
the search to escape local minima [34]. Therefore, currently, some
studies are being conducted to develop hybrid methods in an attempt to
achieve the best combination between robustness and computational
efficiency and local versus global optimization [21,35,36].
In this sense, a hybrid method coupling artificial neural networks

2
J.O.B. Lira et al.
(ANN) and genetic algorithms (GA) has been shown to be an efficient
tool for process simulation and optimization, including heterogeneous
photocatalysis [37,38]. ANN models are a class of nonlinear computa­
tional techniques that attempt to mimic the human neural system
[39,40]. ANN models can properly analyze and predict complex
nonlinear process parameters by approximation functions. ANN have
been used in several fields of science and engineering, and it has been
applied to solve environmental problems such as pollutant degradation,
remediation and problems related to process control [41–44]. Moreover,
a technique of computer-based artificial intelligence, such as the genetic
algorithm (GA), is known as an alternative method to solve nonlinear
optimization problems mimicking the principles of biological evolution
[38,45]. GA can apply ANN models to search for the optimal set of
operational parameters (or geometrical conditions) that result in the
highest efficiency of the process. Based on this, Hassani et al. [23] used
ANN-GA modeling to predict the performance of the antibiotic photo­
catalytic degradation process. Cordero et al. [46] used artificial neural
networks to assess the efficiency of removing NOx from urban photo­
catalytic pavements on a pilot scale. In contrast, Rahimi et al. [45] used
CFD-ANN-GA modeling to estimate the friction factor in serpentine
microchannels with different geometric parameters.
Therefore, the present work explores the application of the hybrid
CFD-ANN-GA method as a tool for the analysis and optimization of
micro-photocatalytic reactors taking the abatement of NOx as a case
study. Nitrogen oxides (NOx), composed of NO and NO2 , were used as
model pollutants, as they negatively affect the environment and the
quality of life of human beings. The microreactor was simulated using
COMSOL Multiphysics 5.3a. The model incorporates the NO and NO2
chemical reaction intrinsic kinetics equation that was previously
implemented and validated [47]. The study firstly explores the indi­
vidual effects of operational parameters (residence time, light intensity,
relative humidity and initial NO concentration) using CFD techniques.
Then, the ANN-GA method is applied for the prediction of NO conver­
sion at the output of the microreactor and optimization of the opera­
tional parameters of the process. The ideal conditions were then
simulated using CFD to assess the performance of the ANN-GA model.
It is worth mentioning that, previously, our research group carried
out an optimization analysis of a flat plate reactor using the combination
of the response surface (RSM) and CFD methodology [48]. The RSM
Fig. 1. Representation of the geometry of the micro-photoreactor investigated in this study and details of the computational domain in some segments of the device.
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Chemical Engineering Journal 431 (2022) 133771
technique has numerous advantages and is already widespread in the
literature for the development and optimization of processes with the
minimum number of experiments. However, its main limitation is that it
can only assume non-linear quadratic correlation and, therefore, re­
quires a narrow search window, being limited to the number of points in
the experimental design. Moreover, many studies have compared the
performance of ANN-GA and RSM tools and have proven that ANN-GA is
a more powerful tool for modelling and optimization than RSM
[41,49,50]. Hence, the hybrid CFD-ANN-GA approach proposed in the
present paper brings great benefits and more promising results due to
the modeling and optimization of complex and non-linear environ­
mental phenomena, which is the case of photocatalytic degradation
reactions.
2. Model description
2.1. Reactor concept and geometry
The microreactor used in this work is a commercial microfluidic
device (Micronit® Microfluidics BV, Enschede, The Netherlands, model
R150.676). This device is assembled with borosilicate glass using the
powder blasting technique and has a total volume of 13 μL, a surface-to-
volume ratio of 3.5 × 104 m2/m3 and a hydraulic diameter of 133.5μm.
The performance of the microreactor was evaluated for environmental
applications in liquid phase in the past [51] and now extended to pho­
tocatalytic NOx abatement (gas phase). The schematic representation of
this device is shown in Fig. 1.
A three-dimensional CFD model was used to represent the main
characteristics of the MR. The feed in the reactor was composed of a
mixture of nitrogen monoxide (NO), water (expressed as relative hu­
midity) and air. The chemical reaction was assumed to occur only on the
outer surface of the catalytic material. It should be noted that the pho­
tocatalytic chemical reactions were implemented in all the internal walls
of the microdevice, considering a homogeneous film of photocatalyst
deposited on these surfaces.
2.2. Chemical kinetics
The kinetic model for the photocatalytic NOx abatement used in this
J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

study was based on the work of Ballari et al. (2010) and modified by Lira [ ( )]
(11)
’
ρ(u⋅∇)u = ∇⋅ pI + μ ∇u + (∇u)T
et al. (2019) in order to obtain the intrinsic parameters necessary for
CFD simulations [47,52]. The photocatalytic oxidation mechanism of
where ρ is the density of the mixture, u is the the velocity vector, p is the
NOx mixtures was reported in several publications [53–55]. All these
pressure, I (dimensionless) is the identity matrix, μ is the mixture dy­
works proposed the decomposition of NO into NO−3 through the pathway
namic viscosity and T’ is the transpose operator [57]. The properties of
NO → HNO2 → NO2 → NO−3 . The generic mechanism can be described in
the mixture such as viscosity and density were obtained by Eqs. (12) to
the following equations [56].
(14).
TiO2 + hν→TiO2 (e− + h+ ) (1) ∑ yi μ
μ= ∑ i (12)
j yi ϕij
O2 + e− →O⋅−2 (2) i

⎡ ( )( ⎤
)
H2 O + h+ →H + + HO⋅ (3) ⎣1 + μi 1 Mw,j 1
⎦2
2 4
μj Mw,i

NO + O⋅−2 →NO−3 (4) ϕij = [ ( )] (13)

M 1
8 1 + Mw,i 2

(5)
w,j
NO + HO⋅ →HNO2

(6) Pabs Mw
HNO2 + HO⋅ →NO2 + H2 O ρ= (14)
RT
NO2 + HO⋅ →NO−3 + H + (7)
where μ(i,j) is the dynamic viscosity of each species in the mixture, Mw is
the mixture molecular weight and R is the universal gas constant.
where TiO2 (titanium dioxide) is the semiconductor (photocatalyst), hν
The chemical species conservation equation is written in Eq. (15),
represents an incident photon with energy equal to or greater than the
assuming diluted concentration (i.e., large excess of air) [57].
band interval of the photocatalyst, e− and h+ are the photogenerated
( )
electron and hole, respectively, O⋅−2 represents the superoxide anion and u⋅∇Ci + ∇⋅ − Di,m ∇Ci = 0 (15)
HO⋅ is the highly oxidative hydroxyl radical.
The rate laws for NO and NO2 degradation are given by Eqs. (8) and where Ci is the species concentration, and Di,m is the species diffusivity in
(9), respectively [52]. the mixture.
’’ The diffusivity coefficient of the gas mixture presented in Eq. (15)
( ) s √̅̅̅̅̅̅̅̅̅̅̅̅̅̅
’’
− rNO s =
kNO CNO
× (− 1 + 1 + αE) (8) was derived from a diffusion model considering a mixture average,
calculated by Eq. (16) [58]. The gas phase binary diffusion coefficients
s s g
1 + K NO CNO + K NO2 CNO2 + KH2 O CH2 O
(Dij ) were calculated through a modified Chapman-Enskog correlation
given by Eq. (17) [58]. It is important to note that the photocatalytic
( ) ’’ ’’ (
’’
s
kNO2 CNO s
− kNO CNO √̅̅̅̅̅̅̅̅̅̅̅̅̅̅)
− rNO = 2
× − 1 + 1 + αE
2 s s s g
1 + K NO CNO + K NO2 CNO2 + KH2 O CH2 O reaction rate was modeled as a boundary condition on the walls (i.e., any
volumetric reaction rate was neglected).
(9)
1
g
where CsNO,NO2 and CH2 O are the concentration of NO and NO2 on the Di,m = ( ) (16)
∑ yj
surface of the photocatalyst and of H2 O in the gas phase, respectively; E j,j∕
=i Dij

is the light intensity that was explicitly considered in these rate laws; ki
’’
[ ( )]
and Ki are intrinsic (i.e., without contributions of mass transfer limita­ T3 1
+ M1w,j
1
2
Mw,i
tions) kinetics and adsorption parameters, respectively. It is worth Dij = 0.0018583 × (17)
noting that different average light intensities were obtained for the top, Pabs σ 2ij ΩD
side and bottom layers of the microreactor (see Supplementary Mate­
rial). Therefore, the reaction rate was applied differently for each layer where Mw(i,j) is the molecular weight of the species, T is the absolute
of the microchannel, taking into account the respective light intensities. temperature, Pabs is the absolute pressure, σij is the “collision diameter”
and ΩD is the collision integral. The parameters in this equation were
2.3. Assumptions and governing equations expressed in our previous work [47].
Rigorous modeling of the radiation field in the microreactor requires
2.3.1. Model assumptions the solution of the radiative transfer equation (RTE) in the appropriate
In this study, the flow regime in the microreactor was assumed to be coordinate system. The general form of the RTE can be written according
steady and laminar. The thickness of the photocatalyst film was to Eq. (18), in which the physical quantity of radiative intensity (Iλ (s,Ω))
neglected since it was assumed to be thin [51]. It was assumed that the is a function of wavelength (λ), transfer direction (Ω) and spatial loca­
gas shows ideal gas behavior. The chemical reactions were assumed to tion (s) [59–61]. However, for systems in which the photocatalyst is
occur only at the surface of the photocatalyst in the microreactor. immobilized on a surface, there is no scattering of light and radiation
Finally, it should be noted that the problem is essentially isothermal. absorption occurs in the TiO2 coating [59]. So, the RTE was simplified
according to Beer-Lambert’s law for the light transmission through a
2.3.2. Governing equations non-scattering medium [59,62], resulting in Eq. (19).
A system of non-linear partial differential equations that describe the dIλ (s, Ω)
∫
σs,λ 4π
single-phase flow and the transport of multicomponent species in steady ds
= − κa,λ Iλ (s, Ω) − σ s,λ Iλ (s, Ω) +
4π 0
p(Ω’ →Ω)Iλ (s, Ω’ )dΩ’
state was solved using the commercial code COMSOL® Multiphysics
(18)
5.3a (Burlington MA, USA). The continuity equation and the momentum
conservation equations are presented in Eqs. (10) and (11), respectively dIλ (s)
[57]. + κa,λ Iλ (s) = 0 (19)
ds
ρ∇⋅u = 0 (10)

4
J.O.B. Lira et al.
2.4. Boundary conditions
The following boundary conditions were applied to the device:
• Inlet: It was assumed that the species that were fed in the micro­
channels are NO, NO2 , water (expressed as relative humidity) and
air, and the inlet average flow velocity of the mixture was specified
by Eq. (20).
in
v = vin , CNO = CNO in
, CNO2 = CNO , CH2 O = CHin2 O (20)
2
• Outlet: At the channel outlet, an atmospheric pressure boundary
condition (null gauge pressure) was applied, and the gradient of
species i concentration was defined as zero, according to Eq. (21).
p = pout , ∇Ci = 0 (21)
• Channel walls: On the channel walls, a Neumann condition was
imposed, considering continuity of fluxes due to mass transport and
chemical reaction. The no-slip boundary condition on the stationary
wall was also specified.
Di,m ∇Ci = ri’’ (22)
Also, it should be noted that the problem was essentially isothermal
because microreactors allow better effective heat management
compared to macroscopic reactors due to their high surface-to-volume
ratio [63,64].
2.5. Computational procedure
The equations presented in section 2.3 were solved using the finite
element method-based commercial code COMSOL Multiphysics®
(version 5.3a, Burlington MA, USA), considering the coupling of the
laminar flow and transport of diluted species. The 3D geometry repro­
duced the main characteristics of the device (see Fig. 1). Complementary
simulation of the radiation field was developed separately in a 2D
domain representing the microchannel’s cross-section using the discrete
ordinate method (DOM) (see Supplementary Material). The same
approach was carried out in our previous work [51] to determine the
different average light intensities in the top, side and bottom layers of
the microreactor.
The 3D computational domain of the microreactor was discretized
into tetrahedral elements with a uniform grid. Additionally, a higher
density of elements was created in the regions close to the wall, where
the photochemical reaction occurs (see Fig. 1). The influence of the
density of the mesh elements on the simulation results was investigated
in a mesh independence study (see Supplementary Material). The in­
dependence regarding the mesh refinement level was confirmed by
refining the domain until the NO and NO2 concentration at the reactor
outlet was affected by less than 1% by an additional refinement step.
Therefore, a mesh with 3.2 × 106 elements was found to be suitable for
this study and was used in all simulations presented in this work.
The model was solved in two stages in steady state. Both steps were
solved fully coupled using the MUMPS direct solver. In the first step, a
solution for the momentum conservation equations was found, while in
the second step the chemical species conservation equations were
solved, considering the velocity field previously calculated. A relative
error of numerical solutions below 10− 10 for each step was assumed as a
convergence criterion.
3. Effect of operational parameters on the performance of the
photocatalytic NOx abatement in the microreactor
To evaluate the performance of the microreactor, a parametric
analysis was performed based on the variation of relevant operational
5
Chemical Engineering Journal 431 (2022) 133771
parameters. The NO conversion (XNO ) was used to characterize the
performance of the microreactor in these different scenarios, expressed
by Eq. (23).
( in avg,out )
CNO − CNO
XNO (%) = in
× 100 (23)
CNO
The effects of the residence time (τ), light intensity (E), initial NO
concentration (Cin
NO ) and relative humidity (RH) were investigated. The
procedure was performed considering a variation of the parameters
analyzed in the range established for different residence times. It is
worth noting that the evaluation of the parameters was carried out
individually so that the other parameters were kept constant. All CFD
simulation conditions are shown in Table S3 of the Supplementary
Material.
Moreover, in order to maximize the NO conversion, it is necessary to
investigate how the four variables interactively affect XNO and deter­
mine the optimal operating conditions. Thus, a model based on artificial
neural networks (ANN) was developed in this study to predict XNO at the
outlet of the microreactor. Then, optimization with genetic algorithm
(GA) was developed to determine the optimal operating condition to
maximize XNO .
Also, the XNO predicted from the ANN allowed to determine the rate
of NO consumption in the microreactor. A complementary optimization
study was then carried out with the GA aiming to maximize the rate of
NO consumption while minimizing the pressure drop in the microfluidic
device.
4. ANN and GA implementation methods
The artificial neural network (ANN) is one of the nonlinear compu­
tational methods that attempt to simulate the human neural system
[39,40]. ANN models can adequately analyze and predict complex
nonlinear process parameters by approximation functions. ANN has
received a lot of interest in the modeling field due to its desirable
characteristics, as a reliable technique able to learn complex and non-
linear processes [41]. In the research, MATLAB 2013a software (Math­
Works Inc, USA) was used for the development of the network archi­
tecture and the optimization of operational parameters. To model the
behavior of the photocatalytic NOx abatement in a microreactor, an
ANN was designed using the three-layer feed-forward backpropagation
network [23,41,65,66], considering the input, hidden and output layers.
Fig. 2a represents the multilayer feed-forward neural network archi­
tecture with multiple inputs and a single output (MISO). While Fig. 2b
illustrates the model for multiple inputs and multiple outputs (MIMO).
The variables used in the parametric analysis (τ, E, Cin
NO and RH) were
fed to the input layer to build the ANN topology. The output variable
was XNO , as the variable used to characterize the performance of the
microreactor (Fig. 2a). All variables were normalized between 0 and 1 to
minimize the deviation. When employing this procedure, all data (Yi )
were scaled to a new value of Yi,norm using Eq. (24) [67].
Yi − Yi,min
Yi,norm = (24)
Yi,max − Yi,min
where Yi,min and Yi,max are the extreme values of the variable Yi . In the
next step, the samples were divided into training (70%), validation
(15%) and test (15%) subsets, respectively [41]. The training, validation
and test sets were randomly selected from the data from the CFD sim­
ulations to investigate the predictive capability of the model. Details of
the parameters used in the ANN model are shown in Table 1. The
network was trained with 185 datasets.
In order to create a robust and accurate model using ANN, it is
necessary to properly consider the architecture of the neural network
[66]. First, the number of neurons in the hidden layer must be opti­
mized, based on a careful selection of hidden neurons to avoid over-
fitting or poor performance of the neural network. Thus, the number
J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

Fig. 2. Schematic diagram of model (a) MISO and (b) MIMO feed-forward backpropagation topology neural network.

of neurons in the hidden layer was optimized by the trial-and-error √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅

√
method between 1 and 20 neurons to reduce the error function. For √1 ∑ Q
( )
the determination of the hidden neurons, Levenberg-Marquart was used RMSE = √ Yi,pred − Yi,CFD 2 (26)
Q i=1
as a backpropagation algorithm with logsig and logsig functions in the
input and output layers, respectively. The performance of the neural ∑Q ( )
network was determined according to the mean square error (MSE), root i=1 Yi,pred − Yi,CFD
R2 = 1 − ∑Q ( ) (27)
mean square error (RMSE) and the correlation coefficient (R2), accord­ i=1 Yi,pred − Ym

ing to Eq. (25), (26) and (27), respectively. When the values of MSE and
RMSE are low, and R2 is close to 1, this indicates that the ANN model has where Q refers to the number of data points, Yi,pred is the forecast of the
good performance and high precision [67]. ANN network, Yi,CFD is the CFD modeling response, Ym is the average of
the values, and i represents the data points.
1 ∑Q
( ) In addition to selecting the number of neurons in the hidden layer,
MSE = Yi,pred − Yi,CFD 2 (25)
Q i=1 the optimal training algorithm for photocatalytic NOx abatement was
also investigated by comparing nine different training algorithms. The
4:11:1 topology was used for the following training algorithms:
Levenberg-Marquardt (LM), BFGS Quasi-Newton (BQN), Resilient

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J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

Table 1 NO conversion. The flowchart of the optimization process using the in­
Model variables and their intervals and the parameters used in the construction tegrated ANN-GA approach is shown in Fig. 3.
of the ANN topology. The program starts with a population of random regimes using a set
Parameters Range Unit of individual coded solutions (operational input parameters) as opti­
Input layer
mization parameters. GA applies the fitness function (the objective
τ* 0.11–6.19 s function given from the best trained ANN model) to classify the indi­
E* 0.3–13 W⋅m− 2 vidual solutions corresponding to their suitability. The objective func­
* 4.48 × 10 − 9
kmol⋅m− 3 tion can be indicated as expressed by Eqs. (29) and (30).
Cin
NO
–4.48
× 10− 8
OF = logsig(LW × logsig(IW × [x(1); x(2); x(3); x(4) ] + b1 ) + b2 ) (29)
RH* 10–100 %
Output layer 1
XNO 0–100 % logsig(x) = (30)
1 + exp(− x)
ANN topology Information Selection mode
Input neurons 4 Based on the number of input
variables where OF is the objective function, IW and b1 are the weights and bias of
Output neurons 1 Based on the number of output the hidden layer and LW and b2 are the weight and bias of the output
variables layer. These values are taken from the best trained ANN. In this opti­
Hidden layer neurons 1–20 Optimization of the number of mization, the classification method is applied to the fitness scale, while
neurons based on the minimum
the stochastic uniform is used for the selection method. It must be noted
MSE
Performance function MSE, RMSE and - that the GA coupled ANN model was also designed using the MATLAB
R2 2013a software, considering the parameters specified in Table 2.
Data splitting function Dividerand Default Furthermore, GA was applied to a multi-objective optimization
Data division(training; 70%;15%;15% Default
considering the ANN with two outputs (NO consumption and pressure
validation; test)
Backpropagation Levenberg- Comparison of 9 backpropagation
drop). In this case, the aim of the optimization problem was to maximize
algorithm Marquart (LM) algorithms the NO consumption while minimizing the pressure drop in the micro­
Input/output layer Logsig/logsig Comparison of 9 combinations of fluidic device.
transfer functions the input/output layer functions

*Range of the parameters taken from the literature [52]. 5. Results and discussion

Backpropagation (RP), Scaled Conjugate Gradient (SCG), Conjugate
Gradient with Powell/Beale Restarts (CGB), Fletcher-Powell Conjugate
Gradient (FCG), Polak-Ribiére Conjugate Gradient (CGP), One Step
Secant (OSS) and Variable Learning Rate Backpropagation (GDX)
[65,68,69]. Moreover, the transfer functions of the input and output
layers have also been optimized by comparing nine combinations of the
transfer functions tansig, logsig and purelin. The selection of the
appropriate training algorithm and the combination of transfer func­
tions were based on the lowest value of MSE and RMSE and the highest
value of R2.
In this research, the relative importance of the input variables (τ, E,
Cin
NO and RH) in ANN was evaluated through the algorithm proposed by
Garson [51], expressed by Eq. (28), which is based on the partitioning of
connection weights, obtained from the ANN training.
∑m=Nh ((⃒⃒ ih ⃒⃒/∑Ni ⃒⃒ ih ⃒⃒ ) ⃒⃒ ho ⃒⃒ )
m=1 ⃒Wjm ⃒ k=1 Wkm × Wmn
RIj = ∑k=Ni {∑m=Nh ( ⃒ ih ⃒/∑Ni ⃒ ih ⃒ ) ⃒ ⃒} (28)
⃒W ⃒ ⃒W ⃒ × ⃒W ho ⃒
k=1 m=1 km k=1 km mn
where RIj is the relative importance of the input variable j; Ni and Nh are
the numbers of inputs and hidden neurons, respectively; W’s are the
connection weights. The superscripts i, h and o refer to input, hidden and
output layers, respectively, and the subscripts k, m and n refer to input,
hidden and output neurons, respectively.
A complementary study was carried out, where the ANN was trained
considering the NO consumption rate and the pressure drop as output
variables based on multi-input multi-output (MIMO) principle (Fig. 2b).
In this case, the ANN retained the same structure described above.
Genetic algorithms (GA) are in a class of evolutionary computational
techniques that are designed to successfully solve non-linear optimiza­
tion problems [23,70]. The integration of the ANN model and an opti­
mization algorithm has been used successfully in several engineering
studies to solve optimization problems. This hybrid ANN-GA technology
is a powerful tool to predict and optimize complex processes and
perform better than the response surface method (RSM) that has been
used as a model replaced in recent decades [50]. Therefore, in this work,
GA is used to optimize the operational parameters of the best network
structure obtained from the ANN model to maximize the photocatalytic
5.1. Model validation
The intrinsic kinetics of NO and NO2 chemical reaction were vali­
dated using experimental data reported in the literature [52]. This
validation was carried out in a previous work in which we had a
comprehensive discussion about obtaining the necessary intrinsic pa­
rameters for CFD simulations [47]. From the validation of the intrinsic
rate, the geometry of the reactor was extrapolated from a flat plate to the
micro-reactor. With the intrinsic reaction rates validated, the reactor’s
geometry was extrapolated from a flat plate to the micro-photoreactor.
Thus, the microreactor CFD model was simulated in the present paper.
The successful validation of the intrinsic kinetics confirms not only the
scientific basis of the model but also supports its applicability for design
purposes, being suitable for application in different configuration of
photocatalytic reactors and scaling of the reactor size [71,72]. There­
fore, the initial geometry of the reactor was extrapolated from a flat
plate to the micro-photoreactor to identify new phenomena and/or
changes in photocatalytic performance using the same validated
intrinsic reactions rate and the same boundary conditions for the pho­
tocatalytic NOx abatement.
5.2. Simulation analysis
In a microreactor, the NO conversion is mainly influenced by τ, E,
Cin
NO and RH . Thus, to examine the performance of the microreactor
(based on XNO ), a parametric analysis was performed based on the
variation of these operational parameters.
First, the effect of τ on MR performance was investigated (0.11 to
6.19 s; CFD simulation conditions reported in Table S3, run 1, keeping
− 8
constant RH = 50%, Cin NO = 4.47 × 10 kmol⋅m− 3 and E = 10 W⋅m− 2).
The τ values were obtained for different inlet velocities from Eq. (31).
VMR VMR
τ= = (31)
Qfeed vin × A⊥
where VMR is the microreactor volume, vin is the initial velocity at the
entrance of the microreactor, and A⊥ is the cross-sectional area of the
channel. Fig. 4 (a) shows that in high residence times (τ > 0.60 s) full

7
J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

Fig. 3. ANN-GA flowchart.

longer time that the molecules pass inside the device as the residence
Table 2
time is increased, prolonging the time for adsorption and oxidation re­
GA main parameters used in the optimization of the process.
actions on the catalyst surface [73]. Similar results were summarized in
Parameters Value the review presented by Das and Srivastava [74] for microfluidic-based
Number of variables 4 photocatalytic microreactor for environmental application in liquid-
Fitness function 4:11:1 trained ANN phase. However, the microreactor exhibited a higher pressure drop,
Population type/size Double vector/100
mainly due to the increase in flow rates (decrease in τ), as shown in
Scaling function Rank
Selection function Stochastic uniform
Fig. 4 (b). It was justified by the fact that, in microreactor systems, the
Crossover function/fraction Scattered/0.80 pressure drop is much greater, as the characteristic diameter of the
Mutation function Constraint dependent microchannels is several times smaller. Therefore, the extremely small
Migration direction/fraction Forward/0.2 dimensions of the microchannels cause greater friction on the walls,
Function tolerance 10− 6
resulting in higher consumption of mechanical energy, which is trans­
lated in the observed pressure drop [75,76]. Similarly, An et al. [77]
conversion of the pollutant was achieved. This analysis showed that XNO evaluated the pressure drop in several types of microreactors for
increased from 79% to 100% with an increase in residence time from monophasic catalytic reactions of methane. The authors observed that
0.11 to 6.19 s (corresponding to flow rates ranging from 7.14 to 0.13 the pressure drop is much higher in geometries where the flow is not
mL⋅m− 1), respectively. This behavior was expected since there will be a divided, as the fluid is forced to flow through much longer passages.
Moreover, simulations were conducted to assess the effect of light

8 3 2
Fig. 4. (a) Effect of residence time on the NO conversion under steady-state conditions, keeping constant RH = 50%, Cin
NO = 4.47 × 10
−
kmol⋅m− and E = 10 W⋅m−
and (b) pressure drop over the flow rate.

8
J.O.B. Lira et al.
intensity in different residence times (Fig. 5) within the range of 1
W⋅m− 2 to 13 W⋅m− 2 (run 2, Table S3, keeping constant Cin NO = 4.47 ×
10− 8 kmol⋅m− 3 and RH = 50%). As expected, high values of light in­
tensities favor XNO , regardless of the residence time, reaching values
above 90% for E = 10 W⋅m− 2. However, when working with lower light
intensities, it took a longer residence time to obtain high XNO . It was
noticeable for E = 1 W⋅m− 2, where XNO 15% and 100% were obtained
for τ = 0.15 s and 5.53 s, respectively.
This behavior can also be seen in Fig. 6, which presents the NO molar
concentration profiles in the microreactor for τ = 5.53 s, 1.20 s and 0.25
s and E = 1 W⋅m− 2 and 10 W⋅m− 2. It was found that for high values of τ
and E = 1 W⋅m− 2 (Fig. 6 (a) and (b)), the molecules were degraded
before half of the reactor domain due to the longer time they pass inside
the microreactor. However, for E = 1 W⋅m− 2 and low τ (Fig. 6 (c)), NO
leaves the reactor without undergoing a reaction because the molecules
will pass through the device very quickly. Thus, for this situation (low E
and different τ), the phenomenon that governed the efficiency in terms
of XNO was the short residence time. On the other hand, when the light
intensity increases to E = 10 W⋅m− 2 (Fig. 6 (d), (e) and (f)), the pho­
tocatalytic NOx abatement occurs even before reaching half of the
microreactor in all cases. Providing a higher light intensity, there will be
a greater availability of the electron-hole pairs, capable of forming
oxidative radicals and hence degrade the pollutant molecules. Conse­
quently, the efficiency of the process is improved at the expense of
higher light intensity (and energy consumption).
Additionally, XNO was evaluated as a function of the initial NO
concentration within the range of Cin NO = 4.47 × 10
− 9
kmol⋅m− 3 to 4.47
× 10 kmol⋅m (run 3, Table S3, keeping constant E = 10 W⋅m− 2 and
− 8 − 3
RH = 50%). Fig. 7 shows that regardless of the NO amount in the gas
stream, full conversion was obtained for high residence times. This
stems from the fact that the microreactors have large surface-to-volume
ratios; therefore, even at higher concentrations, all NO molecules come
into contact with active sites on the surface of the photocatalyst, leading
to full NO conversion. However, as the τ decreases (i.e., when working at
high volumetric flow rates), high XNO was found for low NO concen­
trations at the inlet. This happens because under higher NO concentra­
tions the proportion of active sites in the photocatalyst and reactive
species to NO molecules drops.
Finally, water plays an important role in photocatalytic reactions,
since hydroxyl radicals (OH⋅ ) are generated by the oxidation of the water
molecules adsorbed on the catalyst surface. Therefore, NO conversion
was also evaluated as a function of relative humidity (RH) for the range
Fig. 5. Effect of light intensity on the NO conversion under steady-state con­
ditions for several residence times, keeping constant RH = 50% and Cin
NO = 4.47
× 10− 8 kmol⋅m− 3.
9
Chemical Engineering Journal 431 (2022) 133771
of 10% to 100% (run 4, Table S3, keeping constant E = 10 W⋅m− 2 and
Cin
NO = 4.47 × 10
− 8
kmol⋅m− 3). Clearly, the higher the relative humidity
of the airflow, the greater the generation of hydroxyl radicals. However,
competitive adsorption between water and molecules of the pollutants
can occur at the active sites of the photocatalyst. Fig. 8 shows that full
conversion is obtained for high values of τ (1.20 and 5.53 s), regardless
of the increase in RH . Although for short residence times, τ = 0.15 s for
instance, it can be seen that there was a significant drop in XNO after an
additional increase in RH above 50%. It should occur due to the com­
bination of two effects: i) competition with the water molecules them­
selves and ii) shorter contact time of the molecules for adsorption and
participation in the reaction steps on the surface of the catalyst. More­
over, as it can be seen in Fig. 8, the best XNO was achieved up to RH =
30%. This value was also reported by other researchers as the ideal RH
content for the photocatalytic process of other gas-pollutant abatement
such as toluene [73].
5.3. ANN model
MSE, RMSE and R2 were applied to measure the network perfor­
mance and to select the optimal architecture of the ANN model. The
maximum value of R2, close to 1, and the minimum values of MSE and
RMSE were desirable. 70% of the data is employed to train the network,
whereas the remaining data are for testing and validating the network
(15% of each section). There is generally no theoretical procedure for
assessing the appropriate number of neurons in the hidden layer before
training [45]. The trial-and-error method was used to determine the
appropriate number of neurons in the hidden layer to prevent over­
fitting. Thus, in this study, different number of neurons were considered,
and the best possible number of neurons was selected when reaching the
ideal value (low value of MSE and RMSE and higher value of R2). The
model was trained from 1 to 20 hidden neurons and the MSE and R2 in
each case were evaluated, as shown in Fig. 9 (a). It can be seen that when
11 neurons were used in the hidden layer, the highest R2 value (i.e., R2
= 0.9997) and the minimum MSE and RMSE were found (MSE = 4.75 ×
10− 5 and RMSE = 6.90 × 10− 3). Therefore, a 4:11:1 topology was
selected for these networks. Moreover, the training algorithm was also
optimized based on the evaluation of nine algorithms, and Levenberg-
Marquardt (trainlm) was selected because it had the lowest MSE and
RMSE and the highest R2 value. Additionally, concerning the transfer
functions, the combination of purelin, logsig and tansig was evaluated to
define which function should be used in the input and output layers.
Thus, the transfer functions logsig and logsig were selected for the input
and output layers because they reached an ideal value (lower value of
MSE and RMSE and higher value R2). The same procedure in choosing
the number of neurons in the hidden layer to avoid overfitting was
performed by other works available in the literature [37,78,79], as well
as the procedure for choosing the training algorithm and the combina­
tion of activation functions also [65] (see Table S4, Supplementary
Material). Fig. 9 (b) shows the variation of training, validation, and test
errors with the number of epochs for the optimal ANN model. The graph
shows the MSE of the network decreasing after more epochs of training,
i.e., the network is learning. The training stopped when the validation
error started to increase after 91 epochs. The best performance was
obtained from the epoch with the smallest validation error (MSEvalidation
= 1.05 × 10− 4 and MSEtrainng = 4.75 × 10− 5), as shown in Fig. 9 (b).
A common option to assess any correlation between the simulated
data and predicted data by the ANN model is through a scatter plot. If
the dots on the graph lies on a straight line on a scatter plot, the cor­
relation of the two variables is high, with a coefficient close to 1, and the
model’s accuracy is high as well. Fig. 10 shows the comparison of the
results obtained through the CFD simulations with the training, vali­
dation and test data set using the ANN model. As it can be seen in Fig. 10,
the developed network could predict the outcomes extracted from CFD
successfully, i.e., the results indicate that the neural network estimated
J.O.B. Lira et al.
Fig. 6. NO molar concentration (mol⋅m− 3) profile. (a) E = 1 W⋅m− 2 and τ = 5.53 s, (b) E = 1 W⋅m−
and τ = 5.53 s, (e) E = 10 W⋅m− 2 and τ = 1.20 s and (f) E = 10 W⋅m− 2 and τ = 0.25 s.
Fig. 7. Effect of the normalized initial NO concentration on the NO conversion
under steady-state conditions for various residence times, keeping constant RH
= 50% and E = 10 W⋅m− 2.
values for all data points are close to the CFD-validated data. Correlation
coefficients (R2) close to 1 indicate the reliability of the model, i.e., the
trained neural network predicts NO conversion values very well, and it
can be used to estimate the reactor’s performance. Moreover, the ac­
curacy of the testing data proves the validity of the model. The devel­
oped four-layered neural network (4:11:1) in this study provides the
weights and biases, which are listed in Table S5 in the Supplementary
Material. Thus, ANN’s bias and weight were used to calculate the rela­
tive importance from Eq. (28) and to create the metamodel used in the
optimization step applying a genetic algorithm.
5.4. Relative importance of the operating parameters
The ANN used in this work provided the weights and bias, and they
were listed in Table S5 in the Supplementary Material. From the neural
network weight matrix, the relative importance of the input variables in
the NO conversion was calculated by the Garson method (Eq. (28)). As
10
Chemical Engineering Journal 431 (2022) 133771
2
and τ = 1.20 s, (c) E = 1 W⋅m− 2
and τ = 0.25 s, (d) E = 10 W⋅m− 2
Fig. 8. Effect of relative humidity on the NO conversion under steady-state
conditions for several residence times, keeping constant E = 10 W⋅m− 2 and
− 8
Cin
NO = 4.47 × 10 kmol⋅m− 3.
can be seen in Fig. 11, all variables affected the NO conversion. Thus, no
operational parameter studied in this work could be neglected. How­
ever, it was observed that a higher value of relative importance implies
that the variable most significantly affects the performance of the sys­
tem. Thus, the residence time is the parameter that has the greatest in­
fluence on the process under analysis, with RI = 48.97%.
5.5. GA optimization
After reaching the best trained ANN, the research proceeds with the
optimization process using a genetic algorithm. The bias and weight
values were used to generate the adequacy function for the optimization
problem, according to Eqs. (29) and (30). GA is designed to determine
the minimum optimized value and, therefore, the function of the ANN
model was multiplied by (− 1) to obtain the maximum value of the NO
conversion. Thus, the GA adequacy function is represented by Eq. (32).
The same procedure was performed by Shin et al. [66], as the authors
also want to optimize the variables to maximize the removal of NOx in
J.O.B. Lira et al. Chemical Engineering Journal 431 (2022) 133771

Fig. 9. (a) Effect of the number of neurons in the hidden layer on the performance of the neural network. (b) Evolution of the mean square errors in the prediction of
the NO conversion (%).

Fig. 10. Regression plots for comparison of XNO by the CFD model and by the ANN model using the 4:11:1 topology for the set of (a) training, (b) validation, (c)
testing and (d) all data set.

11
J.O.B. Lira et al.
Fig. 11. Relative importance of operational parameters.
the flue gas.
( )
in
XNO = − ANN τ, E, RH, CNO
The intervals of the CFD simulations were defined as a lower bound
(lb) and upper bound (ub) in the four input variables, respectively (lb =
[0.15, 0.30, 10, 4.47 × 10− 9] and ub = [5.77, 10, 100, 4.47 × 10− 8]).
The GA parameters were defined as shown in Table 2. The GA termi­
nated only if the change in the best value of the fitness function was less
than or equal to the convergence criterion (1 0 − 6). Table 3 provides the
optimal values for the operating conditions of the microreactor for the
maximum NO conversion estimated by the artificial neural network
using the genetic algorithm optimization technique. Based on the opti­
mization result, the ideal conditions applied to the photocatalytic
microreactor for maximum NO conversion (100%) were: τ = 2.12 s, E =
10 W⋅m− 2, RH = 10% and Cin NO = 2.09 × 10
− 8
kmol⋅m− 3. Finally, the
performance of the process under the ideal conditions proposed by GA
was tested in the CFD model, also obtaining full NO conversion. The
excellent agreement between the predicted ANN-GA results and the
results from the CFD simulation confirms the model ability to predict the
photocatalytic performance using NOx abatement as a case study.
Also, an additional study was performed considering a multi-
parametric optimization taking into account the NO consumption rate
and the pressure drop in the microreactor as output of the ANN. The
ability of the GA to maximize the NO consumption rate while mini­
mizing the pressure drop was then assessed. The result of this procedure
can be observed in the Pareto front plot presented in Fig. 12, capturing
the trade-offs of the competing objectives identifying promising solu­
tions of the population.
Four points can be highlighted, indicating minimum pressure drop
(1), maximum NO consumption rate (4) and transitions (2, 3). Point 3
can be chosen as the optimal operating condition, where τ = 0.47 s, E =
3.36 W⋅m− 2, RH = 67.8% and Cin NO = 2.19 × 10
− 8
kmol⋅m− 3. At this
point, the NO consumption rate was equal to 1.99 × 10− 3 nmol⋅s− 1 (XNO
= 93.6%), while the pressure drop was equal to 16.25 Pa.
When considering the path 1 → 4, the NO conversion rate increases
by 26.416% (1 → 2), 8.823.8% (2 → 3), and 76.4% (3 → 4). On the other
hand, the pressure drop increases by 462.2% (1 → 2), 127.6% (2 → 3)
Table 3
Optimal conditions of the operational parameters.
τ(s) E(W⋅m− 2) RH(%) Cin
NO
Predicted XNO
(kmol⋅m− 3) (%)
8
Best 2.12 10 10 2.09 × 10− 100
value
Chemical Engineering Journal 431 (2022) 133771
Fig. 12. Pareto front plot for the multi-objective optimization considering the
NO consumption rate and the pressure drop as objective functions.
and 225.1% (3 → 4).
(32)
6. Conclusions
In this study, computational fluid dynamics and artificial intelligence
techniques, including ANN and GA, were applied to the analysis and
optimization of a micro-photocatalytic reactor, taking NOx abatement
as a case study. Initially, CFD was used to solve the problem and evaluate
key parameters that affect the photocatalytic process in the micro­
reactor: residence time, light intensity, relative humidity and initial
concentration of the pollutant. Based on data from the CFD simulations
(256 cases), a model was developed using the ANN algorithm to predict
the NO conversion based on the effects of the four operational variables.
The ideal structure of the ANN model includes a three-layer feed-for­
ward neural network with 11 neurons in the hidden layer (4:11:1),
logsig-logsig transfer function and Levenberg-Marquardt (LM) as the
training algorithm. The model presented high predictive capacity with
R2 of 0.9997, MSE of 4.75 × 10− 5 and RMSE of 6.90 × 10− 3. Addi­
tionally, the relative importance of the independent variables was
investigated. Thus, the residence time presented relative importance of
48.97% (i.e., with strong effect in the prediction of NO conversion),
followed by light intensity (28.17%), relative humidity (19.34%) and
initial NO concentration (3.52%). Then, the best trained neural network
was used to extract the model used as an objective function for the GA.
The GA was then used to determine the ideal operating conditions to
maximize the NO conversion. Full NO conversion was obtained, and the
optimum values of the independent variables were: τ = 2.12 s, E = 10
W⋅m− 2, RH = 10%, and Cin NO = 2.09 × 10
− 8
kmol⋅m− 3. Finally, a com­
plementary CFD study was carried out to verify the NO conversion using
the optimal operating conditions, and full NO conversion was also
achieved. The ANN was then modified to a different scenario, yielding
the NO consumption rate and the pressure drop in the system as outputs.
All parameters were kept constant, except the number of neurons in the
hidden layer (17). This model was then used as an objective function for
the GA, aiming to maximize the NO consumption rate while minimizing
the pressure drop. A Pareto front analysis was carried out and a set of
operating conditions was identified as optimal in this new scenario (τ =
0.47 s, E = 3.36 W⋅m− 2, RH = 67.8% and Cin NO = 2.19 × 10
− 8
kmol⋅m− 3).
Therefore, the hybrid CFD-ANN-GA method is an adequate technique for
modelling reactive systems, and it can be used in the future to predict the
performance of photocatalytic microreactors with different geometric
structures and reaction conditions.
12
J.O.B. Lira et al.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
The authors acknowledge CAPES (Coordination for the Improvement
of Higher-Level Personnel) for the scholarship (Finance Code 001) and
CNPq (National Council for Scientific and Technological Development)
for funding through the project number 459299/2014-0.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.cej.2021.133771.
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