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Materials and Design 30 (2009) 2867–2874

Contents lists available at ScienceDirect

Materials and Design


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

Application of back-propagation neural network technique to high-energy planetary


ball milling process for synthesizing nanocomposite WC–MgO powders
J. Ma a,b, S.G. Zhu a,b,*, C.X. Wu a,b, M.L. Zhang a
a
College of Mechanical Engineering, Donghua University, Shanghai 201620, PR China
b
College of Material Science and Engineering, Donghua University, Shanghai 201620, PR China

a r t i c l e i n f o a b s t r a c t

Article history: A series of artificial-neural-network (ANN) models is developed for the analysis and prediction of corre-
Received 12 November 2008 lations between processing (high-energy planetary ball milling) parameters and the morphological char-
Accepted 14 January 2009 acteristics of nanocomposite WC–18at.%MgO powders by applying the back-propagation (BP) neural
Available online 22 January 2009
network technique. The input parameters of the BP network are milling speed, milling ball diameter
and ball-to-powder weight ratio. The properties of the as-milled powders (specifically crystallite size,
Keywords: specific surface area and median particle size) are the output for three individual BP network models.
Nano composites
These models are based on the mathematic statistical approach and seem suitable for the complicated
Mechanical alloying
Artificial neural networks
ball milling process which is difficult to be accurately described by physical models. Well acceptable per-
formances of the neural networks are achieved. The model can be used for the prediction of properties of
composite WC–MgO powders at various milling parameters. It can also be used for the optimization of
processing and ball milling parameters.
Ó 2009 Elsevier Ltd. All rights reserved.

1. Introduction be described by physical models [15]. Hence, the ANN techniques


may be ideal for this intricate ball milling process. There has been
High-energy planetary ball milling process has been considered only limited work on the application of neural networks in the field
as a powerful and practical method to achieve solid-state amorphi- of planetary ball milling. Dashtbayazi et al. [16] have carried out
sation of various alloy systems and nanocrystalline materials [1–5]. the latest study on the artificial-neural-network modeling of the
Many advanced engineering materials, including high-thermal sta- mechanical alloying (MA) process. Their research mainly discussed
ble amorphous, nanocrystalline and nanocomposite materials, and the effects of ball milling parameters on the characteristics of the
refractory hard materials, can be prepared at room temperature as-milled metallic powders. Some property predictions of the pow-
using this method. Owing to its significant scientific and industrial ders can be achieved through the model. However, those extrapo-
importance, considerable researches have been conducted on the lation predictions can be further improved. According to the
ball milling process modeling, mainly based on the mechanistic commentary of Sha [17], it must be based on extrapolation domain
[6–10] and thermodynamic [11–13] approaches to achieve a gen- having a same kind of physical relationship as within the training
eral understanding at the atomic and phenomenological level. data domain, even for those attempting extrapolation. The extrap-
Some physical models have been developed to investigate several olation to tv (milling time  milling speed) and P1/P2 (ball-to-pow-
aspects of the planetary ball milling process, and to predict/opti- der weight ratio) have been extended approaching zero in Figs. 11
mize its results as well. However, these models cannot be fully and 12 in Ref. [16]. A zero P1/P2 means that there are no balls, and
and accurately implemented due to the multi-influencing parame- only powder, in the process, which of course is not a mechanical
ters, the inherent complexity and the oversimplified assumptions alloying process.
combined with the highly dynamic, non-linear behavior of a mul- Furthermore, the neural network algorithm and configuration
ti-physics and multi-scale nature [14]. selected in the previous work [16] can be further improved with
Artificial neural networks (ANN) are currently one of the most the development of artificial intelligence (AI) techniques. Typically,
powerful modeling techniques based on a statistical approach. It the BP network is the most commonly used model of feed-forward
is suitable for simulations of the correlations which are hard to multilayer neural network. It is fully connected, i.e. every neuron in
each layer is connected to every other neuron in the adjacent for-
ward layer. In the BP network, there are many weights, each of
* Corresponding author. Address: College of Mechanical Engineering, Donghua
University, Shanghai 201620, PR China. Tel.: +86 21 677 920 06; fax: +86 21 677
which contributes to more than one output. Therefore, the BP neu-
921 99. ral network might be appropriate for the application to the compli-
E-mail address: sgzhu@dhu.edu.cn (S.G. Zhu). cated ball milling process.

0261-3069/$ - see front matter Ó 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.matdes.2009.01.016
2868 J. Ma et al. / Materials and Design 30 (2009) 2867–2874

Recently, the planetary ball milling process has been used as an where b ¼ ðb20  b2c Þ1=2 , b0 is the full width at half maximum
inexpensive method to prepare nanocomposite WC–MgO powders. (FWHM), bc is the correction factor for instrument broadening, h
Sherif El-Eskandary [18] has primarily reported that these nano- is the angel of the peak maximum, k is the Cu Ka weighted average
scaled grains of WC–MgO emerged with unique properties to wavelength (0.15420 nm) and k is the Scherrer factor (1).The local
achieve superior hardness and toughness combination in contrast structure of the milled powders was determined by transmission
to the commercial microns- and submicrons-grained structures electron microscopy (TEM) operating at 200 kV and/or high-resolu-
of WC–Co composites. This new composite WC–MgO end-products tion transmission electron microscopy (HRTEM, JEM-2010, Japan),
forms during ball milling of WO3, Mg and C, and can be subse- using a bright-field image (BFI). All the TEM experiments of the
quently consolidated into a nanocomposite bulk compact [18]. present studies were performed using an electron beam of 4 nm.
The significant technological potential of WC–MgO powders are In the TEM experiments, the powders were mixed with pure etha-
proposed to derive from its applications in cutting tools, tips for nol and stirred for about 300 s to make a suspension. A few drops
drilling tools, and wear resistant parts in wire drawing, extrusion, of the powder suspension were dropped on a Cu micro-grid and
and pressing dies. During our detailed research, these powders can well dried before mounting on the TEM sample holder.
be obtained either by the atom-diffusion reaction or by the self- The particle size distributions, including the median particle
propagating explosive one due to various milling process parame- size and the specific surface area, were measured using particle
ters. Such a complex milling process can hardly be controlled with size analyzers (Malvern, MATERSIZER2000, United Kingdom) by
so many multi-influencing factors. the laser diffraction and scattering method (DLS). The median par-
Thus, the back-propagation neural network (BP), in the present ticle size was determined at the 50th percentile of particles under-
work, is applied to the prediction and optimization of the ball mill- size. Prior to measurement, the sample was externally dispersed
ing process for synthesizing the nanocrystallite composite WC– for 90 s with an ultrasonic homogenizer (US-300T, Nihonseiki, Ja-
18at.%MgO powders. The process parameters, including milling pan). After external dispersion, a stirrer and ultrasonicator
speed, ball-to-powder weight ratio and milling ball diameter, are equipped within the main body itself of MASTERSIZER 2000 were
applied to the neural network inputs to provide information relat- continuously operated during measurement of the particle size
ing to the entire process. The network is then trained to output the distribution for dispersion of sample. As standard operating condi-
prediction on the powders’ morphological properties respectively, tions, the following were set: beam obscuration of MASTERSIZER
including crystallite size, specific surface area and median particle 2000 was measured at 15%; tip diameter of ultrasonic homoge-
size. The viability analysis on this application and the optimization nizer was 20 mm; the ultrasonic homogenizer was also operated
of the process are carried out as well. for 90 s at tuning 2 and output ADJ 8.

2. Experimental details 3. Neural networks modeling procedure

The data used in the neural network training and testing were Artificial neural networks provide a mapping of inputs to out-
generated through the experimental results. According to the re- puts and consist of computer programs based on the structure of
search results of Sherif El-Eskandary [18], the elemental powders brain. As such, they can be trained to recognize patterns within
of WO3 (5 lm), graphite (5 lm) and Mg (750 lm) with an atomic data. In the human brain, a neuron is a nerve cell which processes
ratio of 1:1:3 were firstly mixed and sealed in a cylindrical sap- incoming information and outputs a signal to the relevant part of
phire vial under argon gas atmosphere. Among a number of param- the body accordingly. Some inputs are stronger than the others,
eters involved in the ball milling process, the variables, including i.e. they are ‘weighted’. The total effect of the inputs is the sum
milling speed (v), ball diameter (dB) and ball-to-powder weight ra- of the weighted signals, and, if this exceeds the neuron threshold,
tio (RBP) have been imperatively considered as the prime process- a response is produced. By comparison, in an artificial neural net-
ing parameters. The ball-milling experiments were carried out at work, a number of inputs are applied simultaneously, via weighted
room temperature using a QM-1SP4 planetary ball milling ma- links, and the node calculates a combined total input. The relation
chine. Constant milling time and atomic ratio of elemental pow- between the input and output is specified by a transfer or activa-
ders were maintained throughout the series of experiments as tion function, which describes the threshold for deciding on the
detailed in [18]. Table 1 shows the levels of the process variables state of the output of that particular node. A number of nodes
in the present work. may be combined to form a layer, and layers may be intercon-
The milled composite powders were characterized by means of nected to form a complete network. The procedure of designing
X-ray diffraction (XRD) with Cu Ka radiation (RIGAKU, D/Max- the neural network architecture is described in detail as follows.
2550PC, Japan) and MDI Jade 5.0 software (Materials Data Inc., Uni-
ted States). The crystallite size of the as-milled powders was deter- 3.1. Experimental data collection and preprocessing
mined by the X-ray line broadening and calculated using the
Scherrer equation: The training and testing data in the current modeling are col-
lected through the previous mentioned experimental results. The
kk
d¼ ; ð1Þ milling variables, including milling speed (v), ball diameter (dB)
b cos hhkl
and ball-to-powder weight ratio (RBP) have been chosen as the in-
put parameters. The morphology of the powders, characterized by
crystallite size (d), specific surface area (S) and median particle size
Table 1 (d50), are the individual output for three separate BP network mod-
Levels of the process variables. els. All the parameters are listed in Table 2.
Preprocessing of the data is carried out to convert them to a
Level Variables
suitable form for use with the neural network by
dB (mm) v (r/min) RBP
m  mina
1 4 200 4:1 m0 ¼ ðnewmaxa  newmina Þ þ newmina ; ð2Þ
2 6 250 6:1 maxa  mina
3 8 300 8:1
where v0 is the pattern vector, v is the value of a certain variable (it
4 10 350 10:1
can be v, dB or RBP, etc.), maxa and mina are the maximum and min-
J. Ma et al. / Materials and Design 30 (2009) 2867–2874 2869

Table 2
Core parameters of the planetary ball milling.

Process parameters Notation Remark


Milling speed v Input
Milling ball diameter dB Input
Ball-to-powder weight ratio RBP Input
Milling time t Constant
Crystallite size d Output
Specific surface area S Output
Median particle size d50 Output

Table 3
The range of the numerical values of the neural network input and output data.

Data Variable Values Mean value Standard deviation


Maximum Minimum
Input V (r/min) 350 200 275 64.550
Fig. 2. Mean square errors of different BP neural networks with different neurons in
dB (mm) 10 4 7 2.582
the hidden layer.
RBP 10 4 7 2.582
Output d (nm) 35.173 19.876 26.767 4.295
Output S (m2 g1) 7.690 0.799 3.791 2.241
Output d50 (lm) 7.842 0.703 2.276 2.226
architecture. It includes an input layer, which just propagates input
values to the nodes of the hidden layer, a single hidden layer and
an output layer. It has been proved theoretically that the BP net-
work even with only one hidden layer of neurons and a specific
type of activation function (e.g. sigmoid function) can approximate
any functional relation arbitrarily well, provided that enough hid-
den neurons are available [19]. The input–output relation between
each node of the hidden layer can be written as:
!
X
r
ak ¼ f wki pi þ bk ; ð3Þ
i¼1

where pi is the output from the ith node of the previous layer, wki is
Fig. 1. A typical BP neural network architecture [19].
the weight of the connection between ith node and the current
node, and bk is the bias of the current node. f is a function that
imum values of the independent variable. Additionally, ‘‘1” is its
can be nonlinear, e.g. log-sigmoid Eq. (4-a) or hyperbolic tangent-
new maximum value (newmaxa), and ‘‘1” is the variable’s new
sigmoid Eq. (4-b).
minimum value (newmina). The input pattern vectors are then
formed, comprising 96 pairs of input/output ones for training the 1
neural network on the basis of the previous mentioned experi- f ðzÞ ¼ ; ð4-aÞ
1 þ ez
ments, and the remaining 16 pairs are reserved for testing the per- z
e e z
formance of the trained network. The ranges of the numerical f ðzÞ ¼ z : ð4-bÞ
e þ ez
values of the network input and output are listed in Table 3.
The function used between each layer is a tangent-sigmoid one. As
3.2. Neural network architecture the conventional BP training phase is too slow for practical applica-
tion, the gradient descent with momentum and an adaptive learn-
The back-propagation (BP) network architecture is selected and ing rate algorithm is selected to minimize the total error between
applied in the present work. Fig. 1 shows a typical BP network the examined and predicted results during training.

Table 4
Specifications of the BP neural network design.

Parameters BP network type Diagram


Numbers of input layer 1
Numbers of hidden layer 1
Numbers of output layer 1
Numbers of inputs 3
Numbers of neurons in hidden layer for crystallite size 15
Numbers of neurons in hidden layer for specific surface area 13
Numbers of neurons in hidden layer for median particle size 16
Numbers of outputs 1
Activation function Tangent-sigmoid
2870 J. Ma et al. / Materials and Design 30 (2009) 2867–2874

3.3. Network training and testing training data available and large error prone to X-ray measure-
ments of crystallite size and laser measurement of specific surface
The process of fitting the network to the experimental data is area and median particle size.
called training. During its training phase, the network is repeatedly In addition, the testing dataset, the experimental results under
presented with a set of training patterns, comprising input–output the same conditions as the training data are used to compare the
pairs, until either the output error is minimized to a satisfactory le- measured results with those estimated by the BP network, as
vel (0.001) or the maximum number of training cycles is reached. shown in Fig. 3. The mean square error (MSE) for prediction of
On completion of the training, a set of previous unused patterns crystallite size, specific surface area and median particle size is
are applied to the network inputs, here without example outputs. 0.2072  102, 0.2922  102 and 0.3234  102, respectively,
In this way the ability of the network to classify the composites’
characteristics on the basis of new information is tested.
The algorithm of the conventional BP training phase (least mean
square method) can be improved by the gradient-descent momen-
tum and an adaptive learning rate method, which is more suitable
for the practical problems. It has been proved that the BP network
can perform high computations in a short time with the above
algorithm [19,20]. The employed algorithm is available inside the
Neural Network Toolbox (Version 4.0.1), MATLABÒ 7.1 (14th
release).
With the aim of estimation of a function between input and
output data by the BP architecture, each parameter is adopted with
the hidden layer. In order to determine number of the hidden
nodes in the network, several BP networks with various hidden
nodes (max to 24 nodes) are considered and the corresponding
mean square of the network errors (MSE) are calculated by

1X N
Eðw; BÞ ¼ ðt k  ak Þ2 ; ð5Þ
N i¼1

where N is the total number of training patterns, tk is the target/de-


sired value, and ak is the network output value.
Fig. 2 demonstrates that the number of neurons in the hidden
layer for crystallite size model, specific surface area model and
median particle size model is 15, 13 and 16 correspondingly, which
yield the minimum mean square error for training dataset. As a re-
sult, Table 4 lists the specifications of the architecture of the se-
lected neural network. As shown in Table 4, the number of
weights in crystallite size prediction model is
(3 + 1)  15 + (15 + 1)  1 = 76, in specific surface area model is
(3 + 1)  13 + (13 + 1)  1 = 66, and in median particle size model
is (3 + 1)  16 + (16 + 1)  1 = 81. Consequently, the number of
weights in above three separate network models is lower than
the number of training data (96 patterns). An adequate quantity
of experimental data is available in the current study. Mathemati-
cally this series of models can be justified and determined.

4. Results and discussion

The performance accuracy of the network can be checked by the


error of neural network predictions. For the test dataset neural net-
work predictions are calculated. These are compared with the cor-
responding experiment values. Thereafter, the relative errors are
calculated using
RmEXP  RmNN
Error ¼  100%; ð6Þ
RmEXP
where RmEXP is the experimental (measured) crystallite size, specific
surface area and median particle size, and RmNN is the predicted val-
ues from the neural network.
The linear regression and statistical analysis is only effective for
large quantities of data. In the current circumstances, it would
have been better to use the relative errors of model calculations
[17,21], using the formula (6) given above. The average absolute
relative error for the predictions of crystallite size, specific surface
area and median particle size is 8.22%, 7.88% and 4.05%, respec- Fig. 3. The estimated properties of the as-milled powders tested by neural network
tively. They are not too bad, considering the limited amount of model.
J. Ma et al. / Materials and Design 30 (2009) 2867–2874 2871

Fig. 4. Surface responses of crystallite size (a), specific surface area (b) and median particle size (c) of the milled powders vs. the milling parameters obtained by ANN
technique.
2872 J. Ma et al. / Materials and Design 30 (2009) 2867–2874

which is slightly higher than the MSE of the training results After the above accuracy evaluation and prediction, the neural
(0.642  103, 0.662  103 and 0.443  103, respectively). These network technique can be further applied to the optimization of
acceptable performances achieve a result that our BP network the ball milling process for fabricating the nanocomposite WC–
model can predict with sufficient accuracy for the practice. MgO powders. Fig. 4 shows the response surfaces of powder prop-
erties, obtained by BP network models, with the milling parame-
ters. Note that only two ball milling parameters (milling speed
and milling ball diameter) are discussed in the present optimiza-
tion for the reason that the remaining variable (ball-to-powder
weight ratio) is mainly affected by the milling time which is main-
tained as a constant value. According to the research of [13], ball-
to-powder weight ratio can no longer be considered with the cer-
tain milling time in the current optimization.
As to the clarification of the response surfaces, the contour plots
for those properties are demonstrated in Fig. 5. There is only one
region in Fig. 5a where the crystallite size is in the minimum level
(about 20–22 nm) with the high milling speed (v > 300 r/min) and
large milling ball diameter (dB P 8 mm). The similar situation can
also be found in Fig. 5c which illustrates the minimum and propor-
tional median particle size (1 lm) is obtained under the same
parameter conditions. The variations of the specific surface area
of the as-milled powders vs. the two milling parameters (v and
dB), shown in Fig. 5b, is opposite behavior to the former results.
Consequently, in the region the specific surface area is in the high
level of quantity (S P 7 m2 g1) when the crystallite size and med-
ian particle size of the resultants are in the low level of value
(d 6 22 nm and d50 6 1 lm).
Variations of the crystallite size, specific surface area and med-
ian particle size in the response surfaces could be confirmed with
the theories reported by many other researchers [13,22–24]. It is
widely understood that the faster the mill rotates the higher would
be the energy input into the powder. At high milling speeds (or
intensity of milling), the temperature of the vial may reach a high
value which may be advantageous in the current case where diffu-
sion is required to promote homogenization and/or alloying in the
WC powders. Additionally, the size of the grinding medium (mill-
ing ball diameter) also has an influence on the milling efficiency.
Generally speaking, a large size (and high density) of the milling
ball is useful since the larger diameter/weight of the balls will
transfer more impact energy to the powder particles.
Further milling experiment is implemented using the above
analysis results. Figs. 6 and 7 show the XRD pattern and TEM fig-
ures of the as-milled nanocomposite WC–18at.%MgO powders at
t = 50 h, v = 250 r/min together with 50 sapphire balls (10 mm in
diameter). As shown in Fig. 7a, the powders contain WC (deep-

Fig. 5. Contour plots of crystallite size (a), specific surface area (b) and median Fig. 6. X-ray diffraction patterns of milled nanocomposite WC–18at.%MgO powders
particle size (c) of the milled particles vs. the milling parameters v and dB. after 50 h of the ball-milling time (v = 250 r/min, dB = 10 mm).
J. Ma et al. / Materials and Design 30 (2009) 2867–2874 2873

Fig. 7. TEM pictures and selected area diffraction pattern (SADP) of nanocomposite
WC–18 at.%MgO after 50 h of the ball-milling time (v = 250 r/min, dB = 10 mm).

black grains of about 35 nm in diameter on an average) and MgO


(light-gray grains). The selected area diffraction pattern (SADP,
Fig. 7b) taken at the middle of the micrograph also indicates that
the as-milled powders are the composite WC–MgO materials. With
the XRD pattern, the grain size of the powders calculated through
the Scherrer equation is about 35 nm, which is in good agreement
with the TEM observations.
Fig. 8 shows the bright field image (BFI) and the corresponding
selected-area diffraction pattern of the milled powders for 50 h of
the ball-milling time, at a milling speed of 350 r/min with 50 sap-
phire balls (10 mm in diameter). Obviously, the powders contain
WC (deep-black grains of about 20 nm in diameter) and MgO
(light-gray grains). The HRTEM micrograph for composite WC–
MgO is presented in Fig. 8c. The deep-black grain is WC grain, as
suggested by the HRTEM observation of the grain oriented to be
the (1 0 0) plane direction.
In a word, the results achieved by the surface responses and
contour plots indicate that a consistent agreement exists among Fig. 8. (a) BFI (b) the corresponding SADP and (c) HRTEM micrograph of composite
the outcomes of ANN modeling, the above theoretical description WC–MgO powders after 50 h of the ball-milling time (v = 350 r/min, dB = 10 mm).
and the experimental implementation. Therefore, the response
surfaces and contour plots can be applied to the optimization of
the ball milling process of fabricating the nanocomposite powders. a statistical approach. Therefore, NN can be the ideal modeling
The nanostructured WC–MgO powders posses the excellent mor- for this multi-influencing complex ball milling process.
phological characteristics, such as homogeneous shape with fine The BP network is selected since this feed-forward multilayer
and smooth surface relief and uniform size (less than 0.8 lm in network is further fully connected. The conventional BP learning
diameter). These powders will be consolidated into the bulk mate- phase has been improved by the gradient-descent momentum
rials for the further industrial application. On the basis of the con- and an adaptive learning rate algorithm, and can be more appropri-
tour plots and current experimental circumstances, the optimized ate for the modeling of this highly complicated and non-liner high-
milling parameters (300 r/min < v 6 350 r/min and energy planetary ball milling process.
8 mm 6 dB 6 10 mm) can be obtained using this series model of As it is mentioned above, the architecture of the BP network
BP neural network. Further optimization process (v > 350 r/min models can be implemented:
and dB > 10 mm) will be present in the subsequent paper.
 The series model of BP network is designed to be ‘‘3-n-1”, i.e. it
5. Summary and conclusions includes one input layer which contains the ball milling vari-
ables (milling speed, ball-to-powder weight ratio and milling
The nanocomposite WC–18at.%MgO powders (as a kind of ad- ball diameter), one hidden layers (with different number of
vanced hard refractory material) can be prepared by the high-en- nodes [n] for different model) and one output layer which indi-
ergy planetary ball milling method. This complicated ball-milling cates the properties of the WC–MgO powders (crystallite size,
process can be hardly controlled. The neural network technique specific surface area and median particle size respectively).
(NN) is applied to this ball milling process in the reason that NN  The tangent-sigmoid function is found to be the transfer
relies less on the accurate physical model and is mainly based on activation.
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