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j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

Available online at www.sciencedirect.com

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

Research on the drying kinetics for the microwave


drying of Y2O3eZrO2 ceramic powder

Wei Cao a, Ju Zhou a, Chunxiao Ren a, Mamdouh Omran c,**, Lei Gao a,****,
Ju Tang a,b,***, Fan Zhang a,b, Guo Chen a,*
a
Kunming Key Laboratory of Energy Materials Chemistry, Yunnan Minzu University, Kunming 650500, Yunnan, PR
China
b
Department of Physics, School of Electrical and Information Technology, Yunnan Minzu University, Kunming
650500, Yunnan, PR China
c
Process Metallurgy Research Group, Faculty of Technology, University of Oulu, Finland

article info abstract

Article history: Y2O3eZrO2 ceramic powder has emerged as a vital structural and functional material in
Received 7 July 2023 ceramic applications owing to its remarkable performance including wear resistance,
Accepted 18 August 2023 temperature resistance, and corrosion resistance. Agglomeration during the drying process
Available online 22 August 2023 is the other key issue that needs to be resolved, which improving the quality of zirconia
powder becomes crucial in reducing industrial expenses. This study focuses on investi-
Keywords: gating the influence of modern microwave heating technology on the drying kinetics of
Microwave drying Y2O3eZrO2 ceramic powder. The experimental results revealed that the average drying rate
Y2O3eZrO2 ceramic powder of Y2O3eZrO2 ceramic powder increased with sample water content, microwave heating
Drying rate power, and sample mass. Four kinetic fitting models, namely Page, Wang and Singh,
Drying kinetic model Quadratic Model, and Modified Page, were employed to analyze the experimental data for
Y2O3eZrO2 ceramic powder with a mass of 20 g, initial water content of 7.5%, and the
microwave heating power is 480 W. Among these models, the Modified Page model
demonstrated the best fit and effectively described the drying kinetics of Y2O3eZrO2
ceramic powder. The Modified Page model successfully captured the kinetics across
varying masses, microwave heating powers, and initial water content. FT-IR spectroscopy
was employed to describe the material before and after microwave drying. The results
exhibited a significant reduction in water molecule content in the Y2O3eZrO2 ceramic
powder after microwave drying, thus confirming the high efficiency and rapidity of the
microwave drying procedure. This research provides comprehensive experimental data
and offers a theoretical foundation for the industrial application of microwave-enhanced
drying of Y2O3eZrO2 ceramic powder.
© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

* Corresponding author.
** Corresponding author.
*** Corresponding author. Kunming Key Laboratory of Energy Materials Chemistry, Yunnan Minzu University, Kunming 650500,
Yunnan, PR China.
**** Corresponding author.
E-mail addresses: mamdouh.omran@oulu.fi (M. Omran), leigao@kust.edu.cn (L. Gao), tangju@ymu.edu.cn (J. Tang), guochen@kust.
edu.cn (G. Chen).
https://doi.org/10.1016/j.jmrt.2023.08.183
2238-7854/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
4564 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

component within the sample [18]. Unlike traditional


1. Introduction methods, microwaves directly penetrate the material, elimi-
nating the issue of slow evaporation caused by temperature
Zirconia possesses a multitude of outstanding characteristics. gradients and allowing for accelerated drying rates [19].
On the one hand, it exhibits high toughness, excellent wear Moreover, the material's properties can influence the internal
resistance, and favorable chemical properties. On the other gravitational forces that arise due to uneven heating, under-
hand, it offers strong thermal insulation and a coefficient of scoring the importance of material optimization as a crucial
thermal expansion comparable to steel [1]. Consequently, factor [20]. At the same time, software simulation can be used
zirconia has vast potential for development and application in to predict the change of conditions during microwave drying
various fields [2]. It can serve as a refractory and ceramic fiber process [21e24]. By maximizing the advantages of microwave
material [3]. In the late 1970s, zirconia was employed in heating in both industrial production and everyday life, this
foreign countries as internal components in combustion en- method is widely utilized in various applications, including
gines, sensing elements in machinery, and machine bearings. food drying and mineral dehydration [25].
Due to its impressive thermal shock resistance and excep- There are some common denominators between tradi-
tional heat insulation, it has frequent use in thermal barrier tional heating and microwave heating. But the microwave
ceramic coatings [4]. Zirconia has emerged as a remarkable heating time will be shorter, and the efficiency will be
structural and functional material, finding widespread appli- higher. P.V. Alfiya et al. [26], in their work on solar and the
cation, and its current supply surpasses demand. drying of microwave shrimp, found that the high effective
Consequently, researchers worldwide have focused on moisture diffusion rate of solar energy of microwave-dried
studying methods and process conditions for producing ultra- shrimp. The drying time was also relatively short, indi-
pure and highly dispersed zirconium oxide nanopowders. cating the rapid characteristics of microwave drying. It is
Several new preparation methods have been discovered, also verified that the microwave drying time was shorter
including the hydrothermal method [5], the solegel method than the traditional drying time. Chen Dongyu et al. [27] in
[6], and the co-precipitation method [7]. However, the wet their study of microwave-assisted drying synthesis for the
chemical method is the most commonly used in the industry preparation of cross-linked microneedle arrays, while
for zirconia nano powder preparation [8]. Most of the nano- ensuring the quality. A reduction in preparation time can be
scale zirconia powders used in China are imported from seen. The feasibility of microwave drying was verified by
abroad, leading to increased costs for the industry. Therefore, characterization using Fourier transform spectroscopy and
improving the quality of zirconia powder becomes crucial in scanned electron microscopy. Chen Aiqiang et al. [28]
reducing industrial expenses. Agglomeration during the dry- studied the evolution of the structural morphology of apples
ing process is the other key issue that needs to be resolved. under high power. The experimental results showed that
Various drying methods have been employed, including the the designed microwave drying experimental device could
ultrasonic cavitation method [9], freeze-drying [10], and effectively dry apple slices, thus achieving the experimental
organic dispersant replacement drying [11], all of which aim to purpose. In a study conducted by Sara Guemouni et al. [29]
prevent agglomeration. Common drying methods used in in- used microwave drying of tomatoes, microwave-dried to-
dustry include conductive drying [12], convection drying [13], matoes were found to have the highest FRAP and flavonoid
radiation drying [14], and dielectric heating drying [15]. Among content. The experiment compared microwave drying and
these methods, microwave drying falls under radiation dry- air convection transfer value model. In addition, in the
ing. Compared to the ultrasonic cavitation method, freeze- current study on the kinetics of microwave drying, the
drying, and organic dispersant alternative drying, micro- drying kinetics model will be used to verify a better
wave drying offers advantages such as lower complexity in description of the effect of microwave drying. Zheng Hewen
process control, lower investment costs in the industry, et al. [30] analyze the drying characteristics of microwave-
simplicity in operation, and wide applicability in industrial heated natural titanium dioxide. The experimental data
production. Microwave drying is environmentally friendly, were fitted using nine thin-layer drying kinetic models. The
causing minimal pollution, and effectively harnesses micro- conclusions drawn in that paper had the modified Paige
wave energy. This method converts electrical energy into model most suitable. The microwave drying efficiency
electromagnetic energy to heat the material, resulting in the correlated with initial moisture content, microwave power,
absence of exhaust gas production and minimal microwave and initial mass, which verified the high efficiency of mi-
conductivity [16]. crowave drying. Insha Zahoor et al. [31] studied the drying of
Microwaves emit electromagnetic waves within fre- red bell pepper by microwave-assisted fluidized bed under
quencies ranging from 300 MHz to 300 GHz. The behavior of different conditions. The response surface was used to
microwaves can be classified into three categories: penetra- optimize the process. Experiment validation under optimal
tion, reflection, and absorption [17]. Microwave heating process conditions was conducted to verify the model's
operates on the principle of inducing heat by coupling the applicability. Liu Chenghui et al. [32] studied lignite at
electromagnetic field with the material itself. This heating different microwave powers for samples of different thick-
process uniformly warms the material from the inside out, nesses. Data fitting analysis used 13 fitting models for dry-
aligning with the diffusion of water molecules [18]. The ma- ing kinetics. The main conclusion was that the drying
terial's capacity to absorb microwave energy leads to molec- kinetic model Page model could characterize well the drying
ular vibration and friction, resulting in heating. The efficiency process in microwave depth, and the residual moisture
of microwave heating relies on the dielectric loss of each content can be predicted. The effective diffusion coefficient
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4565

Fig. 1 e XRD of zirconia raw material.

is proportional to the microwave power, indicating the


selectivity of microwave drying. The microwave drying 2. Experiments and methods
process of Y2O3eZrO2 ceramic powder used in this paper is a
typical example of microwave selective heating. Thereby 2.1. Raw materials
reducing agglomeration phenomena [33,34].
This experiment employed the microwave drying method The Y2O3eZrO2 ceramic powder used for the experiment was
to dry Y2O3eZrO2 ceramic powder. The experiments were bought from Hebei Qinghe County Tebo Metal Materials LLC.
carried out using the controlled variable method. The study The company provided the primary components of the
investigated the impact of different initial masses (10 g, 20 g, Y2O3eZrO2 ceramic powder. The composition of each
30 g, 40 g, and 50 g), microwave powers (320 W, 400 W, 480 W, component was analyzed using XRD, as shown in Fig. 1. The
560 W, and 640 W), and initial moisture contents (3%, 4.5%, 6%, JCPDS cards (card numbers 37-1484 and 80-2155) were selected
7.5%, and 9%) on the microwave drying performance of for analysis. It can be seen from Fig. 1 that the raw material's
Y2O3eZrO2 ceramic powder. Additionally, four classical drying main components of Y2O3eZrO2 ceramic powder included
kinetic models, Page, Modified Page, Wang and Singh, and monoclinic-phase zirconia (m-ZrO2) and tetrablinic-phase
Quadratic Model, were employed to fit the data obtained from zirconia (t-ZrO2). The chemical components of the experi-
Y2O3eZrO2 ceramic powder under various initial masses, mental Y2O3eZrO2 ceramic powder were presented in Table 1.
initial moisture contents, and microwave powers. Among According to Table 1, the content of zirconia oxide was
these models, the Modified Page model demonstrated excel- 90.651%, yttrium oxide was 5.206%, and hafnia dioxide was
lent performance and suitability for verifying the unique 2.382%. Silicon dioxide and aluminum oxide contents were
characteristics of microwave drying. The composition anal- 1.056% and 0.517%, respectively [2].
ysis of the major components in Y2O3eZrO2 ceramic powder
was conducted using XRD. FT-IR spectroscopy was applied to
2.2. Equipment
characterize the water molecule content of Y2O3eZrO2
The microwave drying experiments in this study were con-
ceramic powder before and after drying. In this paper, the
ducted using a modified Granz home microwave oven (model:
objective is to provide a method to reduce the agglomeration
R6-G238N4 (S1)). The X-ray diffraction analysis was made with
phenomenon and to study the kinetics of Y2O3eZrO2 powders
Bruker D8 Advance. The model instrument from Germany,
with four classical fitting models to provide basic research
with a tube pressure of 40 kV and a tube flow of 20 mA. The
data for the development of drying technology for industrial
target source used was copper (Ka, l ¼ 0.154056). For
production of Y2O3eZrO2.

Table 1 e Chemical composition of zirconium oxide raw materials (wt. %).


Composition ZrO2 Y2O3 HfO2 SiO2 Al2O3 Cs2O Sc2O3
wt. % 90.651 5.206 2.383 1.056 0.517 0.121 0.067
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Fig. 2 e Particle size distribution of Y2O3eZrO2 ceramic powder.

characterization, a NICOLET-IS10 FT-IR spectrometer from the initial mass of the material, microwave heating power,
Nicollet, USA was employed. The spectral range was opti- and initial water content on the microwave drying process of
mized in the mid-infrared region (7800 cm1- 350 cm1) with a Y2O3eZrO2 ceramic powder. Y2O3eZrO2 powder samples
KBr beam splitter. The peak-to-peak noise figure was weighing 10 g, 20 g, 30 g, 40 g, and 50 g were chosen for the
<1.24  105 AU, and the spectral resolution was better than experiment. The initial water content of the Y2O3eZrO2
0.4 cme1. The FT-IR standard linearity (ASTM E1421) was ceramic powder were maintained at 7.5%, and the microwave
<0.1% T, with KBr as the benchmark. The instrument was output power was set at 480 W. Additionally, various micro-
used for scanning and analyzing the surface functionality of wave heating outputs (320 W, 400 W, 480 W, 560 W, and 640 W)
zirconium oxide clusters. were chosen, keeping the initial moisture content at 7.5% and
The histogram displaying the distribution of zirconia par- the sample mass at 20 g.
ticle sizes and the accumulated volumetric distribution curves Furthermore, Y2O3eZrO2 ceramic powder samples with
are shown in Fig. 2. The characteristics of the zirconia particle initial moisture contents of 3%, 4.5%, 6%, 7.5% and 9% were
size allocation are summarized in Table 2. The Table 2 shows selected while maintaining 480 W of microwave power and
that particle sizes predominantly range from 0.383 mm to the quality of the sample as 20 g. Subsequently, the experi-
5.69 mm. The particle size measurements were obtained using mental samples were removed from the electric blast dryer
a laser particle sizer, with the volumetric mean diameter (Mz) and cooled at ambient temperature. The moisture content of
of 1.372 mm, and the median particle size (D50) of 0.916 mm. an individual sample was adjusted using the water molecule
These results indicate a high level of dispersion in the calculation equation, and deionized water was used for the
Y2O3eZrO2 powder following microwave drying (see Table 3). adjustment before drying experiments. The preparation ma-
terials are placed in a rectangular crucible measuring
2.3. Experimental steps 9.5 cm  6.5 cm  2 cm. The samples were dried in a micro-
wave oven once the variables were added under different
To begin the experiment, a predetermined amount of conditions. Displaying the values on the electronic scale were
Y2O3eZrO2 ceramic powder were weighed and subjected to recorded at 30-s intervals until the sample mass no longer
electrically heated blast drying at 60  C for 48 h before mi- changed, repeating this process for three cycles.
crowave drying. This step aimed to ensure the complete The microwave oven used in this study had a rated output
removal of moisture from the Y2O3eZrO2 ceramic powder. power of 800 W and operated at a frequency of 2.45 GHz with
The investigation then focused on examining the influence of an operating voltage of 220 V. The running time of the

Table 2 e Particle size distribution of Y2O3eZrO2 ceramic powder.


Particle size distribution D10 D20 D30 D40 D50 D60 D70 D80 D90 D95 Mz
Average particle size/mm 0.383 0.492 0.598 0.73 0.916 1.186 1.597 2.3 3.81 5.69 1.372
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4567

transmits the information to the computer control system,


Table 3 e Mathematical model of thin layer drying.
where the data is recorded and analyzed.
Model Model equation
1 Page MR ¼ exp ð  ktn Þ
2.5. Equations
2 Modified Page MR ¼ exp ð  ðktÞn Þ
3 Wang and Singh MR ¼ 1 þ at þ bt2
2.5.1. Wet base moisture content
4 Quadratic Model MR ¼ a þ bt þ ct2
The equation for calculating the moisture content of the
sample is as follows,
microwave oven was set to 30 s. The microwaved samples
were carefully positioned on a round tray, and the electronic Ww  Wg
MW ¼ (1)
scale displayed the current mass of each sample. As the Ww
experiment proceeded, the water within the samples evapo- Mw was the moisture content of the wet basis wt. Ww was
rated, causing a continuous change in the mass displayed on the mass of the leftover sample, g. Wg is the mass of the
the electronic scale. Different sample masses were recorded at desiccated sample, g.
various time intervals, reflecting the evolving drying process.
Finally, the experimental data were meticulously documented 2.5.2. Moisture ratio
for analysis and interpretation. The equation for the water content ratio is,

2.4. Microwave drying equipment Mw  Me


MR ¼  100% (2)
Mo  Me
Fig. 3 illustrates the graphical diagram of the microwave Me , Mo the moisture content of the wet base and the initial
drying equipment employed in this study. The microwave dry base-moisture content. In the case of the microwave
drying process comprises three essential components: the gas drying process, the water ratio has been simplified as follows,
supply, heating, and data collection. The primary role of the
gas supply system is to create a dry environment. In cases MW
MR ¼  100% (3)
MO
where the dry substance is susceptible to chemical reactions
with the ambient air, the gas supply system is employed to
2.5.3. Average drying rate
maintain a dry atmosphere. The heating system primarily
In the experimental process, the average drying rate of
consists of a microwave generator, which emits microwaves
Y2O3eZrO2 ceramic powder at time t could be expressed as the
that penetrate the sample and generate heat internally,
drying rate, and it was calculated as follows,
facilitating the drying process. The data collection system
encompasses a computer control unit and a mass collector. Ww  Wwt
DR ¼ (4)
The mass collector detects changes in sample mass and Dt

Fig. 3 e Device diagram of microwave drying.


4568 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

DR was the drying rate, g/s, Dt is the interval time, s, Wwt moisture content ratio decreases progressively and slowly as
was the mass of the sample at drying time t, g. the temperature inside the Y2O3eZrO2 ceramic powder rises.
The decelerated temperature rise stage (III) indicates the end
2.6. Kinetic modeling of drying and performance indices of evaporation. Fig. 4(b) illustrates the averaged drying rate for
the Y2O3eZrO2 ceramic powder at different masses (10 g, 20 g,
Drying kinetics involves the study of the relationship between 30 g, 40 g, and 50 g), with respective average drying rates of
the factors influencing the process of removing water from a 0.00125 g/s, 0.00202 g/s, 0.00316 g/s, 0.00389 g/s, and 0.00538 g/
material [35]. Extensive theoretical and experimental studies s. It is observed that as the sample mass increases, the average
have been conducted in previous research, resulting in the drying rate also increases. This phenomenon was attributable
development of semi-empirical and empirical models [36]. to the fact that more microwave energy is absorbed as the
These semi-theoretical and empirical models effectively mass increases, causing a faster heating rate. This observation
describe the transfer of water molecules and have been vali- aligns with the findings of Farrel et al. [39], who studied
dated for their applicability to experimental data. The microwave-dried pharmaceutical powders and observed a
empirical models not only consider the external resistance of gradual increase in drying rates with higher sample masses.
the material to water vapor during transport but also exhibit a These experimental results are consistent with the findings of
low dependency on hypothetical experiments [37]. Conse- the present study.
quently, they can provide more accurate results and enhance
the predictive capability of drying behavior. Four commonly 3.2. The influence of microwave heating power on the
used drying kinetic models were selected for this study, drying rate
namely Modified Page, Wang and Singh, Quadratic Model and
Page. Statistical indicators can identify the selection of spe- The variations of drying rates caused by the variations of
cific models, for instance, the coefficient of determination, microwave heating power, one of the most important factor of
residual sum of squares, and F-value, which can be calculated the drying process of substances, were investigated. Fig. 5
to assess the goodness of fit [38]. demonstrates the changes in the moisture content ratio of
R2 is an indication of goodness of fit, which is the degree of Y2O3eZrO2 ceramic powder with heating time under different
fit of the regression line to the observations, the closer the R2 microwave heating powers and the variation in average dry-
value is to 1, the better the fit is. RSS is the residual sum of ing speed with microwave heating power. Fig. 5(a) shows that
squares, indicating that the smaller the residual sum of the drying time decreases as the microwave heating power
squares, the better the correlation between the independent increases. This could be attributed to the higher microwave
variable and the dependent variable. F-Value is a statistic for power resulting in a faster reduction in the moisture content
analysis of variance (ANOVA), which tests whether the ratio, as it allows for more excellent microwave energy ab-
regression variance is significant; the larger the F-value, the sorption and accelerates the drying rate. Fig. 5(b) displays the
more significant the linear relationship becomes. The four average drying speed of Y2O3eZrO2 powder under different
kinetic models are empirical and semi-empirical equations. microwave heating powers: 320 W, 400 W, 480 W, 560 W, and
640 W. The corresponding average drying rates were 0.0017 g/
s, 0.00203 g/s, 0.00214 g/s, 0.00248 g/s, and 0.00267 g/s,
3. Experimental results and discussion respectively. Initially, the average drying rate of Y2O3eZrO2
ceramic powder increases slowly, followed by a more rapid
3.1. Influence of the initial mass of the samples on the increase. This behavior can be explained by the sample
drying rate gradually reaching a state of energy saturation as it absorbs
microwave energy. Once saturation is reached, further in-
Fig. 4 depicts the behavior of Y2O3eZrO2 powder samples creases in microwave power will not result in additional en-
under different conditions, with microwave power set at ergy absorption by the sample. Although microwave radiation
480 W and a moisture content of 7.5% during the microwave can penetrate the sample, it leads to a wastage of microwave
drying process. Drying time gradually increases as the initial energy if it is not absorbed. In line with the findings of this
mass of the samples increases. Fig. 4(a) shows that the experiment, Zhang et al. [40] concluded that increasing mi-
moisture content ratio of the Y2O3eZrO2 ceramic powder de- crowave power significantly reduces drying time, which aligns
creases until it reaches zero during microwave drying. The with the present study. Similarly, Dadali Goekce et al. [41]
microwave drying procedure of the Y2O3eZrO2 ceramic pow- obtained the same conclusion in their research, indicating
der can be divided into three stages: an accelerated tempera- that when the initial mass and initial moisture content are
ture rises stage (I), a constant temperature stage (II), and a kept constant, an increase in microwave power reduces dry-
decelerated temperature rise stage (III). In the accelerated ing time.
temperature rise phase (I), the aqueous solution temperature
of Y2O3eZrO2 ceramic powder gradually increases with the 3.3. Influence of initial moisture content on microwave
duration of microwave irradiation, leading to an accelerated drying rate
decline in the moisture content ratio over time. In the con-
stant temperature stage (II), the temperatures of Y2O3eZrO2 Fig. 6(a) shows the drying time gradually increases with the
ceramic powder and water molecules gradually increase with increase of the initial moisture content. Notably, a rapid in-
extended microwave irradiation time, resulting in an crease in drying time is observed at an initial moisture content
increased rate of water content reduction. At this stage, the of 7.5%. This can be attributed to higher water content leading
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4569

Fig. 4 e Moisture ratioetime curves of Y2O3eZrO2 ceramic powder at different masses (a), Average drying rate of different
masses of Y2O3eZrO2 ceramic powder (b).
4570 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

Fig. 5 e Moisture ratioetime curves of Y2O3eZrO2 ceramic powder at different power (a), Average drying rate of Y2O3eZrO2
ceramic powder with different power (b).
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4571

Fig. 6 e Moisture ratioetime curves of Y2O3eZrO2 powder at different moisture contents (a), Average drying rate of
Y2O3eZrO2 powder with different water content (b).
4572 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

to a more pronounced effect of microwave drying. As depicted


in Fig. 6(b), the average drying rates are 0.00125 g/s, 0.00166 g/
s, 0.00177 g/s, 0.00235 g/s, and 0.00289 g/s when the moisture
content is 3%, 4.5%, 6%, 7.5%, and 9%, respectively. It can be
observed that the average drying rate is positively correlated

Table 4 e Statistical indicators of the mathematical


model.
Statistical Equations
indicators
P
Leaner coefficient ðMRexp  MRexp ÞðMRpre  MRpre Þ
R2 ¼ qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ðMRexp  MRexp Þ2 ðMRpre  MRpre Þ2
Residual sum of P
N
RSS ¼ ðMRexp  MRpre Þ2
squares i¼1
F-Value MStreatment
F  Value ¼
MSerror

Table 5 e Data of 7.5% Y2O3eZrO2 ceramic powder with


water content fitted by different models.
Model Params R2 RSS F-value
Page k ¼ 5.55265E-6 0.99444 0.01671 4950.69694
n ¼ 2.07653
Modified Page k ¼ 0.00294 0.9947 0.01594 5189.717
n ¼ 2.15111
Quadratic a ¼ 1.0988 0.97819 0.06259 516.76531
b ¼ 0.00244
c ¼ 1.04681E-6
Wang and Singh a ¼ 0.00188 0.969 0.09321 878.62466
b ¼ 3.847E-7

Table 6 e Initial mass of 20 g Y2O3eZrO2 ceramic powder


mass for different model fitting.
Model Params R2 RSS F-value
Page k ¼ 1.65531E-5 0.99242 0.02939 3717.52757
n ¼ 1.89501
Modified Page k ¼ 0.003 0.99264 0.01981 3826.02222
n ¼ 1.95248
Quadratic a ¼ 1.07578 0.98854 0.02936 950.20491
b ¼ 0.00234
c ¼ 8.99089E-7
Wang and Singh a ¼ 0.00189 0.98263 0.04674 1615.82544
b ¼ 3.4513E-7

Table 7 e Different model fitting microwave power 480 W


Y2O3eZrO2 ceramic powder mass.
Model Params R2 RSS F-value
Page k ¼ 2.04317E-5 0.9938 0.01602 4104.13462
n ¼ 1.88851
Modified Page k ¼ 0.00328 0.99396 0.01561 4214.61102
n ¼ 1.93931
Quadratic a ¼ 1.07644 0.98653 0.03308 769.74831
b ¼ 0.00265
c ¼ 1.31971E-6
Fig. 7 e The variation of water content at different stages Wang and Singh a ¼ 0.00218 0.98061 0.05012 1305.29245
b ¼ 7.07835E-7
under different conditions.
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4573

Fig. 8 e The fitted curves of different drying models Page, Modified Page, Wang and Singh, Quadratic Model for the samples
under different conditions (a), (c), (e), Histograms of residuals under different models of moisture ratio data models (b), (d), (f).
4574 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

with increasing moisture content. The higher the initial stage, from 60 to 540 s is the water evaporation stage, and
moisture content, the more the water molecules will be from 540 to 690 is the end of water evaporation stage, which
absorbed by the microwaves and reach their boiling point, shows the graph the more significant the mass, the longer
resulting in their escape from the samples to the surrounding the drying time (see Table 4).
environment. In a study conducted by Dumanli Fatma Tugce
Senberber et al. [42], which focused on the microwave dehy-
dration of borax, similar conclusions were drawn. They found 4. Data fitting of the drying kinetics model
that after microwave heating, an increase in moisture content
leads to a rise in the average drying rate, aligning with the To study the effect of sample water content, microwave
findings presented in this paper. power, and sample quality on the following factors, the kinetic
Fig. 7 shows the water content at different stages of the properties of microwave drying of Y2O3eZrO2 ceramic pow-
process under different conditions. Microwave drying is pri- der, four kinetic models, namely Page, Modified Page,
marily divided in three stages. The first stage is the preheating Quadratic Model, and Wang and Singh were utilized to fit the
stage, the second stage is during the moisture evaporation experimental data. Specifically, the experiments were con-
stage, and the third stage is the end of moisture evaporation. ducted using 20 g of Y2O3eZrO2 ceramic powder with an initial
Fig. 7(a) shows the different initial water contents, the moisture content of 7.5% and a microwave power of 480 W.
graph shows the preheating stage at 1e60 s, which is also the The fitting results for the Page, Modified Page, Wang and
free water preheating and evaporation stage, the water Singh, and Quadratic Model are presented in Tables 5, 6, and 7,
evaporation stage at 60e540 s, when the free and bound respectively.
water evaporates, and the end of evaporation stage at Initially, the data were fitted for a Y2O3eZrO2 ceramic
540e690 s. The gradual decrease in moisture content can be powder mass of 20 g, an initial water content of 7.5%, and a
seen from the graph that the more moisture content, the microwave heating power of 480 W. The objective was to
more time is needed for drying. Fig. 7(b) shows different determine the best-fitting model. Compared to the three other
microwave heating power, during 1e60 s for the preheating models, the Modified Page model exhibited an R2 value closer
stage, 60-600 for the evaporation stage, and 600e750 s for the to 1, a smaller RSS value, a larger F-Value, and a Reduced Chi-
end of evaporation, it can be seen from the figure the greater Sqr value closer to 0. These results indicate that the Modified
microwave power, the shorter the drying time. Fig. 7(c) Page model describes effectively drying kinetics of Y2O3eZrO2
shows the different masses, where 1e60 s is the evaporation ceramic powder.

Table 8 e Fitting data of drying kinetic model of Y2O3eZrO2 ceramic powder under different conditions of drying.
Condition Params R2 RSS F-value
Mass 10 g k ¼ 0.00347 0.9877 0.02568 2046.40725
n ¼ 1.89365
20 g k ¼ 0.003 0.99264 0.01981 3826.02222
n ¼ 1.95248
30 g k ¼ 0.00311 0.99467 0.01396 5066.31753
n ¼ 2.01618
40 g k ¼ 0.00309 0.99561 0.01245 6182.57529
n ¼ 1.88779
50 g k ¼ 0.00329 0.99642 0.01022 6979.46346
n ¼ 1.96898
Microwave heating powder 320 W k ¼ 0.00244 0.99349 0.02045 5299.12451
n ¼ 2.21963
400 W k ¼ 0.00269 0.99316 0.01991 4525.75418
n ¼ 2.1886
480 W k ¼ 0.00328 0.99396 0.01561 4214.61103
n ¼ 1.93931
560 W k ¼ 0.00341 0.99258 0.01717 3271.54964
n ¼ 2.23971
640 W k ¼ 0.00383 0.99376 0.01419 3350.82036
n ¼ 2.24376
Water content 3.0% k ¼ 0.00368 0.98762 0.09831 1891.78701
n ¼ 1.82980
4.5% k ¼ 0.00343 0.99163 0.00106 2928.70549
n ¼ 1.90861
6.0% k ¼ 0.00321 0.9955 0.01142 5912.57156
n ¼ 1.89486
7.5% k ¼ 0.00294 0.9947 0.01594 5189.717
n ¼ 0.01594
9.0% k ¼ 0.00279 0.99646 0.01052 8421.80317
n ¼ 2.1914
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4575

Fig. 9 e Fitted plots of Modified Page moisture ratio data under different conditions (a), (c), (e), Histograms of residuals under
different conditions of Modified Page moisture ratio data model (b), (d), (f).
4576 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

Fig. 10 e Residual scatter plots for representing different fitted models at 480 W microwave power (a), (c), (e), (g), the different
model normal distributions of representing different fitted models (b), (d), (f), (h).
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0 4577

Based on Fig. 8(a), (b), and (c), it is evident that, when


compared to the other three models, the Modified Page model
provided a much better fitting to the experimental data. This
can be observed from the tighter clustering of data points
around the line of fit for the Modified Page model, particularly
in the upper right corner. As shown in Fig. 8(b), (d), and (f), the
Modified Page model exhibits a normal distribution pattern,
with a dense center and sparse sides, indicating a good fit for
the data.
Table 8 present the validation results of the Modified Page
model for different sample masses, microwave heating
powers, and moisture contents. The fitting results are shown
in Fig. 9, These fitting results clearly show that the Modified
Page model efficiently represents the microwave drying ki-
netics of Y2O3eZrO2 ceramic powder under different
Fig. 11 e Effective diffusion coefficient of Y2O3eZrO2
conditions.
powder at different microwave powers.
To verify and assess the accuracy and validity of the
experimental data, normal distribution plots and scatter plots
of residuals can be employed as references. Fig. 10(a), (c), (e),
and (g) displays the residual normal probability profiles for
various fitted model analyses. It is observed that the Modified average effective diffusion coefficient can be estimated by
Page model exhibits a closer fit to a straight line compared to using this slope according to Eq. (8),
other models, indicating its superior performance. The his-
tograms of residuals in Fig. 10(b), (d), (f), and (h) demonstrate d2
De ¼  a (8)
that the experimental data are distributed randomly and p2
show the feasibility of the experimental results. From Fig. 11, it can be seen that with the gradual increase of
microwave power, when the microwave heating power is less
than 560 W, the faster the Y2O3eZrO2 powder heats up. When
5. Calculation of effective diffusion
the microwave heating power is more significant than 560 W,
coefficient
according to the relationship between the moisture ratio and
time, the rate of the moisture ratio reaching the equilibrium
Fick's Second Law of Diffusion is often used to describe the
time is less than 560 W when the microwave power is 640 W.
drying process of various materials [43,44]. As an essential
The reason for the decrease in the diffusion coefficient of the
index of transfer rate in the microwave drying process, the
Y2O3eZrO2 powders is the fitting error.
effective diffusion coefficient contributes to the understand-
ing and behavior of water transfer in samples. The data were
linearly fitted to lnMR versus t to use microwave drying. The
6. Fourier transform infrared spectroscopy
linear plot between lnMR and t gives the slope and intercept
analysis
for assessing surface diffusion coefficients. In this drying
process of experiment, the diffusion of water in the
FT-IR was employed as a method for characterizing and
Y2O3eZrO2 powder section can be described by Fick's second
identifying compounds and for quantitative analysis. The type
law [44] as,
of compound was determined based on the measured char-
  acteristic wavenumbers, which provided insights into the
6 nX¼∞
1 4n2 p2 De
MR ¼ exp  t (5) molecule's structure and chemical bonding. In this experi-
p2 n¼1 n2 d2
ment, two sets of samples were tested: one group underwent
In a long drying process, n ¼ 1, the above Eq. (5) can be microwave drying treatment, resulting in a dehydrated state.
simplified as, In contrast, the other group remained in its natural state
  without microwave drying treatment. Fig. 12 illustrates the FI-
6 4p2 De
MR ¼ exp  t (6) TR analysis diagram. In particular, the IR spectrum of the
p2 d2
desiccated Y2O3eZrO2 ceramic powder showed a character-
Taking logarithm on both sides of Eq. (6) simultaneously istic peak at 3449.60 cm1, corresponding to molecular
gives Eq. (7), stretching vibrations [45]. Another characteristic peak
observed at 1595.78 cm1, labeled HeOeH, was attributed to
6 4p2 De
ln MR ¼ ln  t (7) the bending vibration of the molecule [46].
p2 d2
Similarly, the Y2O3eZrO2 ceramic powder before drying
In Eq. (7), De represents the effective diffusion coefficient (shown in Fig. 12) displayed characteristic peaks at
(m2/s), d represents the particle size of the material (m), and t 3437.15 cm1 (OeH stretching) and 1601.17 cm1 (HeOeH
represents the drying time (s). bending), indicating molecular stretching and bending vibra-
By fitting Eq. (7) with the relevant experimental data, a tions. Upon comparison, it was noticed that the intensities of
slope a of the fitted straight line can be obtained, and the absorption peaks of Y2O3eZrO2 samples after microwave
4578 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 3 ; 2 6 : 4 5 6 3 e4 5 8 0

the microwave drying effect was optimal at an initial


mass of 50 g, exhibiting an average drying rate of
0.00538 g/s. It was concluded that as the initial mass
increased, the microwave absorption capability, tem-
perature rise rate, and drying rate also increased.
Similarly, higher microwave heating power resulted in a
faster decline in the moisture ratio and an accelerated
average drying rate. However, it should be noted that
beyond a certain point, further increasing the micro-
wave power led to a waste of energy, as the sample
reached its maximum capacity for absorbing micro-
wave energy. Furthermore, the measured average dry-
ing rate positively correlated as the initial water content
gradually increased. This phenomenon can be attrib-
uted to water molecules' continuous absorption of mi-
crowave energy, leading to their evaporation from the
surface of Y2O3eZrO2 ceramic powder into the sur-
Fig. 12 e FT-IR analysis of Y2O3eZrO2 ceramic powder
rounding environment after reaching the boiling point,
before and after microwave drying.
Effective diffusion coefficient is proportional to micro-
wave power.
(3) The fitting of different models, including Page, Wang
and Singh, Quadratic Model, and Modified Page, was
drying treatment were lower than before the drying. This
performed to analyze the drying process of 20 g of
observation signifies the pronounced drying and dehydration
Y2O3eZrO2 ceramic powder. The initial water content
effects of microwave drying on Y2O3eZrO2 ceramic powder
was 7.5%, and the microwave power output was 480 W.
[47]. Furthermore, this finding elucidates the characteristic
The residual histogram exhibited a normal distribu-
features of microwave drying, such as uniform heating and
tion, indicating that the Modified Page model accu-
high efficiency.
rately described the drying kinetics of Y2O3eZrO2
The proportion of bound water and free water before mi-
ceramic powder. Furthermore, the IR spectral analysis
crowave drying is large. Moreover, with the increase of micro-
graph shows that the HeOeH absorbance peak in-
wave heating time, the components of free water molecules
tensity of the sample decreased after microwave dry-
asymmetric OeH stretching vibration and HeOeH bending vi-
ing treatment, highlighting the significant drying
bration decreased [48]. The intensity of the asymmetric OeH
effect.
stretching vibration and HeOeH bending vibration among
free water molecules is also different. After microwave drying,
the ratio of bound water and free water decreases, and the in-
tensity of the characteristic peaks of Y2O3eZrO2 samples is Declaration of Competing Interest
obviously smaller than that before drying.
The authors declare that they have no known competing
financial interests or personal relationships that could have
7. Conclusion appeared to influence the work reported in this paper.

(1) In the present study, microwave heating technology


was applied to dry processing of Y2O3eZrO2 ceramic Acknowledgments
powder. The effects of three variables on microwave
drying performance were investigated, namely initial Financial support from the National Natural Science Foun-
mass, microwave powers, and initial water content. A dation of China (Grant No. 51764052), Academy of Finland
thorough validation analysis was conducted using the (grant No. 349833) and Innovative Research Team (in Science
thin-layer drying kinetic model. FTIR spectroscopy was and Technology) in University of Yunnan Province.
utilized to characterize the materials before and after
microwave drying. The conclusion drawn was as
follows. references
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