Polymers 15 01728

polymers
Article
Preparation of Aloe-Emodin Microcapsules and Its Effect on
Antibacterial and Optical Properties of Water-Based Coating
Nan Huang 1,2 and Xiaoxing Yan 1,2, *
1 Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University,
Nanjing 210037, China
2 College of Furnishings and Industrial Design, Nanjing Forestry University, Nanjing 210037, China
* Correspondence: yanxiaoxing@njfu.edu.cn
Abstract: With the development of science and technology, the function of waterborne coatings
has been advanced to a higher standard, which requires researchers to innovate and expand the
research on them. Aloe-emodin is a natural material with antibacterial properties. Applying its
antibacterial effect to the coating can enrich its function and meet the diversified needs of consumers.
In this study, the urea-formaldehyde resin was used as the wall material and the aloe-emodin as
the core material to prepare the microcapsules. The coating rate, yield, and morphology of the
microcapsules were characterized. Through an orthogonal experiment and a single factor experiment,
the optimization scheme of microcapsule preparation was explored. The results indicated that the
optimum preparation process of aloe-emodin microcapsules was as follows: the mass ratio of core
material to wall material was 1:15, the molar ratio of urea to formaldehyde was 1:1.2, the temperature
of microencapsulation was 50 ◦ C, and the stirring speed of microencapsulation was 600 rpm. On
this basis, the aloe-emodin microcapsules with 0%, 1.0%, 3.0%, 6.0%, 9.0%, and 12.0% contents were
added to the waterborne coating to prepare the paint films, and their influence on the antibacterial
and optical properties of the waterborne paint films was explored. The results demonstrated that the
aloe-emodin microcapsules had antibacterial activity. When the content was 6.0%, the comprehensive
performance of the film was better. The antibacterial rate of the film against Escherichia coli was
68.1%, and against Staphylococcus aureus it was 60.7%. The color difference of the film was 59.93, and
the glossiness at 60◦ was 7.8%. In this study, the microcapsules that can improve the antibacterial
Citation: Huang, N.; Yan, X. performance of water-based coatings were prepared, which can expand the application of water-based
Preparation of Aloe-Emodin coatings and provide a reference for the study of the functionalization of water-based coatings.
Microcapsules and Its Effect on
Antibacterial and Optical Properties
Keywords: microcapsules; aloe-emodin; water-based coating; antibacterial property; optical property
of Water-Based Coating. Polymers
2023, 15, 1728. https://doi.org/
10.3390/polym15071728
Academic Editor: Lacramioara Rusu 1. Introduction

Received: 15 February 2023 With the improvement in material living conditions and the increased attention to
Revised: 22 March 2023 health, the living environment is also receiving more and more attention [1,2]. Microbial
Accepted: 28 March 2023 pollution in the living environment will affect human health. Coatings are often used on
Published: 30 March 2023 furniture, utensils, and other household items and decoration [3–8], which people come
into direct contact with in their daily life and work [9,10]. Bacteria may spread through
the carrier of the coating on the object, so the coating with antibacterial properties is an
effective way to block indirect transmission [11]. Antibacterial coatings can effectively
Copyright: © 2023 by the authors.
reduce the bacterial density on furniture and other items, optimize the living environment,
Licensee MDPI, Basel, Switzerland.
and have practical application value [12–15]. This requires us to explore the antibacterial
This article is an open access article
function of the coating.
distributed under the terms and
By wrapping the wall material around the surface of the core material, microcapsule
conditions of the Creative Commons
technology creates tiny, spherical particles with a wall–core structure [16–23]. Using
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
microcapsule technology to coat the core material with an antibacterial material can stabilize
4.0/).
the properties of the core material, thus achieving a lasting antibacterial effect. If the
Polymers 2023, 15, 1728. https://doi.org/10.3390/polym15071728 https://www.mdpi.com/journal/polymers

Polymers 2023, 15, 1728 2 of 22
antibacterial agent is formulated into microcapsules and then added to the coating, its
performance is not only optimized, but it also provides the coating with an antibacterial
function. This has practical significance for optimizing the preparation of the antibacterial
agent and enriching the functionality of the coating.
Aloe-emodin is an anthraquinone compound derived mainly from Aloe vera, Rheum
palmatum L., and other plants, and is an effective antibacterial ingredient in aloe [24]. It
is extremely sensitive to Staphylococcus and Streptococcus and is a natural antibacterial
agent. It not only effectively eliminates bacteria but is also safe and harmless without
stimulation [25–28]. Aloe-emodin can clean up the hazardous metabolites secreted in
the course of bacterial infection and the toxins that remain after the bacteria are killed,
and it has a strong inhibitory effect on the synthesis of the nucleic acid and protein of
Staphylococcus [29,30]. For instance, the α-toxin is an important cytotoxic factor released
by Staphylococcus aureus and a key toxin for some infections. Aloe-emodin can effectively
inhibit its activity and exert an antibacterial effect [31]. In addition to its good antibacterial
properties, aloe-emodin is also often used as a raw material for cosmetic and hair care
products. Thus, it will not cause harm to human skin when applied to coatings that are
in direct contact with the human body. Moreover, the preparation of microcapsules using
green and environmentally friendly materials is a hot spot of current research. However, the
aloe-emodin itself is dark in color, its material state is orange-red crystal, and its particles
are large and irregular in shape, so it is not suitable for direct addition to the coating.
The microencapsulation technology can be applied to actual production by changing its
processing performance, and it has broad development prospects.
In this study, the urea-formaldehyde resin was used as the wall material and the
aloe-emodin as the core material, and the best technological parameters for preparing
microcapsules were explored through the L9 (34 ) orthogonal experiment and single factor
experiment. The aloe-emodin microcapsules were mixed into the water-based coating with
different loadings to prepare the paint films, and the microscopic morphology and chemical
composition of the films were analyzed and investigated. The influence of the microcapsule
loading on the antibacterial property against Escherichia coli and Staphylococcus aureus,
optical properties, and roughness of the paint films was analyzed. The results provide a
reference for the study of the antibacterial property of water-based coatings.
2. Materials and Methods

2.1. Test Materials
The materials involved in this test are listed in Table 1. The coating preparation mold
was made of silica gel, and the size was 50 mm × 50 mm × 10 mm. The paint was Dulux
water-based coating. The size of the polyethylene film was 40 mm × 40 mm × 0.08 mm.
The diameter of the Petri dish was 90 mm. The Escherichia coli was the second-generation
standard strain ATCC25922, and the Staphylococcus aureus was the second-generation
standard strain ATCC6538 from the Beijing Biological Preservation Center.
Table 1. List of the test materials.
Molecular Concentration
Material MW (g/mol) CAS No.
Formula (%)
urea CH4 N2 O 60.06 57-13-6 99.0
formaldehyde solution - - - 37.0
triethanolamine C6 H15 NO3 149.19 102-71-6 99.9
polyvinyl alcohol [C2 H4 O]n - 9002-89-5 99.0
sodium dodecyl benzene
C18 H29 NaO3 S 348.48 25155-30-0 99.9
sulfonate
aloe-emodin C15 H10 O5 270.2369 481-72-1 98.0
citric acid monohydrate C6 H10 O8 210.14 5949-29-1 99.9
Polymers 2023, 15, 1728 3 of 22
Table 1. Cont.
Molecular Concentration
Material MW (g/mol) CAS No.
Formula (%)
anhydrous ethanol C2 H6 O 46.07 64-17-5 99.9
sodium chloride NaCl 58.4428 7647-14-5 99.5
silicon dioxide SiO2 60.084 14808-60-7 99.5
waterborne acrylic resin - - 9003-01-4 -
Escherichia coli - - - -
Staphylococcus aureus - - - -
nutrient agar medium - - - -
nutritional broth - - - -
polyethylene film - - - -
Petri dish - - - -
2.2. Preparation Method of the Aloe-Emodin Microcapsules

In this study, an orthogonal experiment and a single factor experiment were used
to explore the best process parameters for the synthesis of the microcapsules. First, the
L9 (34 ) orthogonal test was designed, as shown in Tables 2–4. By controlling the urea
and formaldehyde molar ratio of n (urea):n (formaldehyde), the core–wall ratio of m
(core material):m (wall material), the reaction temperature, and the stirring rate of the
microencapsulation, a variety of microcapsules were obtained, and the process parameters
with the greatest influence factors were analyzed and determined.
Table 2. Formulation scheme of the orthogonal experiment.
Factor A Factor B Factor C Factor D

Level n (Urea):n m (Core Material):m Temperature Stirring Speed
(Formaldehyde) (Wall Material) (◦ C) (rpm)
1 1:1.2 1:15 50 600
2 1:1.5 1:20 70 900
3 1:1.8 1:25 90 1200
Table 3. Preparation parameters of the orthogonal experiment.
Factor A Factor B Factor C Factor D

Sample n (Urea):n m (Core Material):m Temperature Stirring Speed
(Formaldehyde) (Wall Material) (◦ C) (rpm)
1 1:1.2 1:15 50 600
2 1:1.2 1:20 70 900
3 1:1.2 1:25 90 1200
4 1:1.5 1:15 70 1200
5 1:1.5 1:20 90 600
6 1:1.5 1:25 50 900
7 1:1.8 1:15 90 900
8 1:1.8 1:20 50 1200
9 1:1.8 1:25 70 600
Table 4. Material list of the orthogonal experiment.
Wall Polyvinyl Aloe-

Formaldehyde Deionized Emulsifier
Sample Urea (g) Material Alcohol Emodin NaCl (g) SiO2 (g)
Solution (g) Water (g) (g)
(g) (g) (g)
1 10.00 16.22 16.00 0.10 1.07 232.65 2.35 1.28 1.28
2 10.00 16.22 16.00 0.10 0.80 174.24 1.76 1.28 1.28
3 10.00 16.22 16.00 0.10 0.64 139.59 1.41 1.28 1.28
Polymers 2023, 15, 1728 4 of 22
Table 4. Cont.

(g) (g) (g)
4 10.00 20.27 17.50 0.10 1.17 255.42 2.58 1.40 1.40
5 10.00 20.27 17.50 0.10 0.88 191.07 1.93 1.40 1.40
6 10.00 20.27 17.50 0.10 0.70 152.46 1.54 1.40 1.40
7 10.00 24.32 19.00 0.10 1.27 276.21 2.79 1.52 1.52
8 10.00 24.32 19.00 0.10 0.95 213.84 2.16 1.52 1.52
9 10.00 24.32 19.00 0.10 0.76 165.33 1.67 1.52 1.52
(1) Preparation of the wall material: after a specific amount of formaldehyde solution
with a concentration of 37.0% and a specific amount of urea were mixed evenly, the
triethanolamine was used to regulate the pH value to 8.0. Then the polyvinyl alcohol was
added at a dosage of 1.0% of the mass of the urea. The solution was put into a magnetic
stirrer at 80 ◦ C and the stirring speed was set to 600 rpm. The wall material prepolymer
was prepared after reaction for 1 h.
(2) Preparation of the core material: the sodium dodecylbenzene sulfonate was used
as an emulsifier and mixed with water, and then stirred evenly. After that, the core material
aloe-emodin was added and put into a magnetic stirrer. After the corresponding reaction
temperature and stirring rate were set, the reaction lasted for 45 min, so that the aloe-emodin
was fully emulsified.
(3) Microencapsulation: the prepared wall material was gradually poured into the
prepared core material solution. The citric acid monohydrate crystal was used to regulate
the pH value to 2.5, and the NaCl and SiO2 powder were added to give the wall material
toughness and prevent the microcapsule particles from binding to each other. After contin-
uous reaction for 2 h, the resulting solution was stored for 24 h. The product was filtered by
ethanol and water several times, dried at 40 ◦ C for 24 h, and then ground. The final orange
powder was the aloe-emodin microcapsules.
On the basis of the orthogonal experiment, the single factor test was conducted on
the factor that had the greatest influence in the orthogonal experiment to further optimize
the preparation parameters of the microcapsule. The experimental materials are shown in
Table 5.
Table 5. Material list of the single factor test.

(g) (g) (g)
10 10.00 13.51 15.00 0.10 1.00 217.80 2.20 1.20 1.20
11 10.00 14.86 15.50 0.10 1.03 224.73 2.27 1.24 1.24
12 10.00 15.54 15.75 0.10 1.05 227.70 2.30 1.26 1.26
13 10.00 16.22 16.00 0.10 1.07 232.65 2.35 1.28 1.28
14 10.00 16.89 16.25 0.10 1.08 234.63 2.37 1.30 1.30
15 10.00 17.57 16.50 0.10 1.10 239.58 2.42 1.32 1.32
16 10.00 18.24 16.75 0.10 1.12 243.54 2.46 1.34 1.34
17 10.00 18.92 17.00 0.10 1.13 245.52 2.48 1.36 1.36
18 10.00 20.27 17.50 0.10 1.17 254.43 2.57 1.40 1.40
2.3. Preparation Method of the Paint Films

The best microcapsules obtained from the single factor experiment were mixed with
the water-based coating with contents of 0%, 1.0%, 3.0%, 6.0%, 9.0%, and 12.0%. The film
without microcapsules was set as the control sample. The dosages of the films are shown in
Table 6. The microcapsules and coatings were fully mixed and evenly coated in the mold,
then dried and cured in an oven at 40 ◦ C for 30 min until the quality was no longer changed,
Polymers 2023, 15, 1728 5 of 22
and then taken out. The paint film samples were gently removed from the mold to test the
antibacterial and optical properties. In addition, these coatings with microcapsules were
applied to the glass plate to test the roughness of the films.
Table 6. Dosage list of the water-based paint films.
Content of the
Microcapsule Weight (g) Coating Weight (g)
Microcapsules (%)
0 0 1.400
1.0 0.014 1.386
3.0 0.042 1.358
6.0 0.084 1.316
9.0 0.126 1.274
12.0 0.168 1.232
2.4. Testing and Characterization

2.4.1. Yield and Coverage Rate Test of the Microcapsules
The microcapsules obtained from the test were dried, weighed, and recorded, and the
yield of microcapsules was obtained. The microcapsule powder with a weight of m1 was
weighed and fully ground with a mortar until the wall material was damaged and the core
material was exposed. The powder was put into the glassware, and the hot ethanol was
added, so that the powder was soaked in it and placed in the 65 ◦ C constant temperature
environment for 2 h. The operation was repeated more than twice to fully dissolve the
exposed core material with the ethanol. After soaking, the deionized water and ethanol
were used to filter the powder, and the resulting material was dried in an oven at 40 ◦ C,
which comprised the residual wall material. The weight of the wall material was m2 , and
the coating rate of the microcapsule was calculated by Formula (1).
P = (m1 − m2 )/m1 × 100% (1)
2.4.2. Micromorphology and Chemical Composition Test of the Microcapsules

The microcapsules were observed with an optical microscope and scanning electron
microscope. The prepared aloe-emodin microcapsules were evenly spread on a slide and
placed on the stage with the cover glass side facing up. After the spring clip was fixed, the
focal length and brightness were adjusted, and the 20× lens was selected to observe and
record the micromorphology of the microcapsules. The powder tablet press compressed
the microcapsule powder into thin slices, and the infrared spectrometer characterized the
chemical composition of the microcapsules and the paint films.
2.4.3. Antibacterial Test of the Paint Films

Escherichia coli and Staphylococcus aureus were used in the antibacterial test. Based on
GB/T 21866-2008 [32], the antibacterial property of the paint films was tested and recorded.
First of all, the nutrient agar medium powder was added into purified water, heated,
dissolved, and then sub-packed into Petri dishes to make several planar nutrient agar
media for standby. The nutritional broth powder was added into purified water to make
broth culture liquid. The NaCl was added into purified water and dissolved by heating
to produce the elution solution with a concentration of 0.85%. The plane nutrient agar
medium, broth medium, and elution solution were sterilized at 121 ◦ C for 30 min. The
polyethylene film was immersed in 70.0% ethanol solution for 30 min, flushed with the
elution solution, and then dried for standby.
The slant preservation fungus was fresh fungus that had been preserved for no more
than one month. The bacteria on the slant medium were transferred to the plane nutrient
agar medium through the inoculation ring and cultured for 20 h in a constant temperature
and humidity chamber at 37 ◦ C. The 1–2 rings of fresh bacteria were taken from the plane
nutrient agar medium and added to the broth culture medium. On the basis of GB/T 4789.2-
Polymers 2023, 15, 1728 6 of 22
2016 [33], the 1:1000 bacterial suspension was prepared with tenfold increasing diluents
in sequence. A total of 0.5 mL of the bacterial suspension was dripped onto the prepared
paint film, and the sterilized polyethylene film was picked up by a pair of tweezers and
then covered on the paint film. The paint film to be tested was placed in a Petri dish and
incubated in a constant temperature and humidity chamber with a temperature of 37 ◦ C
and a humidity of 98.0% for 24 h. Two groups of parallel tests were conducted for each
sample. The samples cultured for 24 h were taken out, 20 mL of the elution solution was
added, and the sample paint films and covering film were washed repeatedly. After the
elution solution was stirred evenly, 0.5 mL of it was taken and inoculated into the plane
nutrient agar medium and cultured in the same environment for 48 h.
The plane nutrient agar medium cultured for 48 h was taken out and put into the
bacterial colony counter. Through careful observation, all the colonies displayed in the Petri
dish were counted one by one with a pen. After counting, the data on the counter were the
number of colonies in the Petri dish. The final result was the average of the two groups of
parallel tests. The measured number of colonies was multiplied by 1000, which was the
actual number of the viable bacteria recovered after 48 h of incubation. The antibacterial
rate of the paint films was calculated by Formula (2). In it, R refers to the antibacterial
rate, B refers to the average number of recovered colonies after 48 h for the film without
microcapsules, and C refers to the average number of recovered colonies after 48 h for the
films with microcapsules.
R = ( B − C )/B × 100% (2)
2.4.4. Optical Properties Test of the Paint Films

The color difference in the paint films was measured in line with GB/T 11186.3-1989
by a colorimeter [34]. The values of L, a, and b were noted during the test. L represents
the brightness value of the paint films. A higher value indicates a brighter color of the
paint film. a represents the red-green value of the paint films; a positive number indicates
the color is reddish, and a negative number indicates the color is greenish. b refers to
the yellow-blue value of the paint films. A positive number indicates the color is yellow,
and a negative number indicates the color is blue. The test values of the film without
microcapsules are L1 , a1 , b1 , and the test values of the films with microcapsules are L2 , a2 ,
b2 . The color difference ∆E was obtained by Formula (3). In it, ∆a = a2 − a1 , ∆L = L2 − L1 ,
∆b = b2 − b1 .
h i1/2
∆E = (∆L)2 + (∆a)2 + (∆b)2 (3)
The glossmeter was used to measure the gloss of the paint films at 20◦ , 60◦ , and
85◦ based on GB/T 4893.6-2013 [35]. The gloss loss rate of the paint films at 60◦ was
calculated based on Formula (4). GL is the loss rate, G0 is the gloss of the film without the
microcapsules, and G1 is the gloss of the films mixed with microcapsules.
GL = ( G0 − G1 )/G0 × 100% (4)
The ultraviolet spectrophotometer was used to test the transmittance of the paint film,
and the test wavelength range was 380–780 nm of visible light. After a beam of light passed
through the sample, the ratio of the remaining light intensity to the incident light intensity
was the transmittance.
2.4.5. Tensile and Roughness Test of the Paint Films

The tensile test of the paint film was conducted with the universal mechanical testing
machine. The stress–strain curve was drawn on the base of the test results. When the paint
film broke, the ratio of the distance beyond the original length to the original length was
the elongation at the break of the paint film.
The test method for the roughness of the paint film surface included placing the coated
glass plate on the test table of the roughness meter and adjusting the position of the contact
pin to contact the paint film to start the test and record the value of the roughness.
Polymers 2023, 15, 1728 7 of 22
Polymers 2023, 15, x FOR PEER REVIEW 7 of 23

3. Results and Discussion
3.1. Analysis of the Yield and Coverage Rate of the Microcapsules
The yield of the microcapsules was a significant indicator in the performance evalu-
3. Results and Discussion
ation of the microcapsules. To save resources and improve efficiency it was beneficial to
3.1. Analysis
prepare of the
a high Yield and Coverage
production Rate of the Microcapsules
of the aloe-emodin microcapsules with fewer crude materials.
The yield
Table of the the
7 reveals microcapsules
analysis of was a significanttest
the orthogonal indicator
resultsinofthe
theperformance
microcapsuleevalu‐
yield, and
ation of the microcapsules. To save resources and improve efficiency it was
Figure 1 shows the visual analysis of each factor and level. The yield of sample 2 was beneficial to the
prepare a high production of the aloe‐emodin microcapsules with fewer crude
highest, reaching 13.55 g, followed by sample 1, reaching 11.77 g. Through a comparison materials.
of theTable
mean 7 reveals
value, the
theanalysis
optimalof the orthogonal
level was determinedtest results
to beof the microcapsule
A1B2C1D3. yield,to the
According
and Figure 1 shows the visual analysis of each factor and level. The
comparison of the range results, the primary and secondary level of the influence ofyield of sample 2 each
was the highest, reaching 13.55 g, followed by sample 1, reaching 11.77
factor on the microcapsule yield was A > D > C > B. The most influential factor was g. Through a the
comparison of the mean value, the optimal level was determined to be A1B2C1D3. Ac‐
molar ratio of urea and formaldehyde, followed by the stirring speed of microencapsulation,
cording to the comparison of the range results, the primary and secondary level of the
followed by the reaction temperature of microencapsulation, and finally the mass ratio of
influence of each factor on the microcapsule yield was A > D > C > B. The most influen‐
core material to wall material.
tial factor was the molar ratio of urea and formaldehyde, followed by the stirring speed
of microencapsulation,
Table followed yield
7. Analysis of microcapsule by theresults.
reaction temperature of microencapsulation, and
finally the mass ratio of core material to wall material.
Factor B
Factor A Factor C Factor D
TableSample
7. Analysis of microcapsule m (Core
n (Urea):n yield results. Temperature Stirring Speed Yield (g)
Material):m
(Formaldehyde) Factor B
(◦ C)
Factor C
(rpm)
Factor D
(Wall Material)
Factor A
Sample m (Core Material):m Temperature Stirring Speed Yield (g)
1 1:1.2
n (Urea):n (Formaldehyde) 1:15 50 600 11.77
(Wall Material) (°C) (rpm)
2 1:1.2 1:20 70 900 13.55
13 1:1.2
1:1.2 1:251:15 9050 600
1200 11.7712.72
24 1:1.2
1:1.5 1:151:20 7070 900
1200 13.5510.97
35 1:1.2
1:1.5 1:201:25 9090 1200
600 12.729.72
46 1:1.5
1:1.5 1:251:15 5070 1200
900 10.9711.56
57 1:1.5
1:1.8 1:151:20 9090 600
900 9.72 8.28
68 1:1.8
1:1.5 1:201:25 5050 1200
900 11.5611.25
79 1:1.8
1:1.8 1:251:15 7090 600
900 8.28 9.48
Mean8 value 1 12.680
1:1.8 10.3401:20 11.527
50 10.323
1200 11.25
Mean9 value 2 10.417
1:1.8 11.5071:25 11.333
70 11.130
600 9.48
Meanvalue
Mean value13 9.670
12.680 11.253
10.340 10.240
11.527 11.647
10.323
Range
Mean value 2
3.010
10.417
1.167
11.507
1.287
11.333
1.324
11.130
Primary and
Mean value 3 9.670 11.253 10.240 11.647
secondary A>D>C>B
Range 3.010 1.167 1.287 1.324
order
Primary
Optimalandlevel A1 B2 C1 D3
A> D > C > B
secondary order
Optimal
Optimal level A1 A1
B2 B2 C1 D3 C1 D3
scheme
Optimal scheme A1 B2 C1 D3
Figure
Figure1.1.The
Thevisual
visualanalysis
analysischart.
chart.
Table88isisthe
Table thevariance
variance analysis
analysis table
table of microcapsule
of microcapsule yield
yield results,
results, andvariance
and the the variance
results
resultswere
werebasically
basicallyconsistent with
consistent thethe
with range results.
range The The
results. symbol “*” indicates
symbol that athat a
“*” indicates
Polymers 2023, 15, 1728 8 of 22
factor is significant. It can be seen from the sum of squares data that factor A had the
greatest impact on the yield results and was far more significant than the other three
factors. The other factors had a small impact and a small gap. Based on the results of mean
value, range, and variance, it can be seen that factor A, namely, the molar ratio of urea
and formaldehyde, had the greatest impact on the yield. The better process parameter for
preparing the urea-formaldehyde resin-coated aloe-emodin microcapsules was A1B2C1D3;
that is, the molar ratio of urea and formaldehyde was 1:1.2, the mass ratio of core material
to wall material was 1:20, the reaction temperature of microencapsulation was 50 ◦ C, and
the stirring speed of microencapsulation was 1200 rpm.
Table 8. Analysis table of variance.
Sources of Quadratic F-Critical

Free Degree F-Ratio Significance
Variation Sum Value
Factor A 13.951 2 2.564 4.460 *
Factor B 2.259 2 0.415 4.460
Factor C 2.888 2 0.531 4.460
Factor D 2.669 2 0.490 4.460
Error 21.77 8
The coverage rate of the microcapsules was the ratio of the core material to the total
microcapsule mass. The coverage rate of the core material in the microcapsules was the key
to its antibacterial effect and was an important base for measuring the performance of the
microcapsules. The mass of core material in this test was small, so the higher the coverage
rate, the more successful the preparation of the aloe-emodin microcapsules. The mean
value, range, and variance results of the coating rate of the microcapsules are shown in
Table 9, Figure 2, and Table 10. The coating rate of sample 1 was the highest, up to 9.2%. By
comparing the mean values, we inferred that the optimal level was A1B1C3D1. According
to the comparison of the range data, the primary and secondary level of the influence of
each factor on the coverage rate was B > A > D > C. The most influential factor was factor
B, followed by factor A. The result of variance was roughly the same as the result of range.
Comparing the data of the sum of squares, it was seen that factor B had the greatest impact
on the microcapsule coverage rate, followed by factor A and factor D, and finally factor C.
Combining the results of mean, range, and variance, it was deduced that factor B, namely,
the mass ratio of core material to wall material, had the greatest impact on the coating rate,
followed by factor A, namely, the molar ratio of urea and formaldehyde. The better process
parameter for preparing the urea-formaldehyde resin-coated aloe-emodin microcapsules
was A1B1C3D1; that is, the molar ratio of urea and formaldehyde was 1:1.2, the mass ratio
of core material to wall material was 1:15, the reaction temperature of microencapsulation
was 90 ◦ C, and the stirring speed of microencapsulation was 600 rpm.
Table 9. Analysis of microcapsule coverage rate results.
Factor B
m (Core Coverage
Sample n (Urea):n Temperature Stirring Speed
Material):m Rate (%)
(Formaldehyde) (◦ C) (rpm)
(Wall Material)
1 1:1.2 1:15 50 600 9.2
2 1:1.2 1:20 70 900 8.4
3 1:1.2 1:25 90 1200 5.4
4 1:1.5 1:15 70 1200 6.2
5 1:1.5 1:20 90 600 7.3
6 1:1.5 1:25 50 900 3.9
7 1:1.8 1:15 90 900 8.3
8 1:1.8 1:20 50 1200 5.1
9 1:1.8 1:25 70 600 5.0
Polymers 2023, 15, 1728 9 of 22
Table 9. Cont.
Factor B
m (Core Coverage
Sample n (Urea):n Temperature Stirring Speed
Material):m Rate (%)
(Formaldehyde) (◦ C) (rpm)
(Wall Material)
Mean value 1 7.667 7.900 6.067 7.167
Mean value 2 5.800 6.933 6.533 6.867
Mean value 3 6.133 4.767 7.000 5.567
MeanRange
value 2 1.867
5.800 3.133
6.933 0.933
6.533 1.600
6.867
Primary
Mean valueand
3 6.133 4.767 7.000 5.567
secondary
Range 1.867 B>A>D>C
3.133 0.933 1.600
order
Primary and
Optimal level A1 BB1
>A>D>C C3 D1
secondary order
Optimal
Optimal level A1 B1 B1 C3 D1
A1 C3 D1
scheme
Optimal scheme A1 B1 C3 D1
Thevisual
Figure2.2.The
Figure visualanalysis
analysis chart.
chart.
Table10.
Table Analysistable
10.Analysis table
ofof variance.
variance.
Sources of Quadratic
Quadratic F‐Critical
F-Critical
Sources of Variation Free
Free Degree
Degree F‐Ratio
F-Ratio Significance
Significance
Variation Sum Sum Value
Value
Factor
Factor A A 5.947 5.947 2 2 0.880
0.880 4.460
4.460
Factor
Factor B B 15.44715.447 2 2 2.285
2.285 4.460
4.460 * *
Factor C C
Factor 1.307 1.307 2 2 0.193
0.193 4.460
4.460
Factor D D
Factor 4.340 4.340 2 2 0.642
0.642 4.460
4.460
Error 27.04 8
Error 27.04 8
Throughaacomprehensive
Through comprehensive analysis
analysis of of
thethe orthogonal
orthogonal experiment
experiment results,
results, the primary
the prima‐
ry and
and secondarylevels
secondary levelsofofthe
the factors
factors obtained
obtained fromfromthetheyield
yieldtest
testwere
werefound
found to to
be be
A >A > D
D
>C >C > >B,B,and
andthe
theprimary
primary andand secondary
secondary levels
levelsof ofthe
thefactors
factorsobtained
obtained from
from thethe
cover‐
coverage
age
raterate
testtest
werewere
B >BA> >AD >D> >C.C.ItItcan
canbebeinferred
inferredthat
thatthe
the comprehensive
comprehensive impact impactofoffac‐
factor A
tor
wasAthewaslargest.
the largest. Considering
Considering that that in variance
in the the variance results
results of the
of the yield
yield test,test, factor
factor A the
A had
had the highest
highest impact
impact and andBfactor
factor had the B had the impact,
lowest lowest impact, while A
while factor factor
was A wassecond
only only sec‐
to factor
ond
B into
thefactor B in the
coverage ratecoverage rate test,
test, it was it was determined
determined that among thatthe
among the four factor
four factors, factors,A had
factor A had the greatest impact on the yield and coverage rate of the
the greatest impact on the yield and coverage rate of the microcapsules, namely, the molar microcapsules,
namely, the molar
ratio of urea ratio of urea and
and formaldehyde. Theformaldehyde.
better process The better obtained
parameter process parameter ob‐ test
from the yield
tained from the yield test was A1B2C1D3, and the better process parameter obtained
was A1B2C1D3, and the better process parameter obtained from the coverage rate test was
from the coverage rate test was A1B1C3D1. The reaction temperature of C3 level was 90
A1B1C3D1. The reaction temperature of C3 level was 90 ◦ C, and the rotational speed of D3
°C, and the rotational speed of D3 level was 1200 rpm. Considering that, when the reac‐
level was 1200 rpm. Considering that, when the reaction temperature is too high and the
tion temperature is too high and the rotational speed is too fast, the water in the solution
rotational speed is too fast, the water in the solution will evaporate too quickly, affecting
will evaporate too quickly, affecting the accuracy of the test, the parameters of C1 and ◦
the accuracy of the test, the parameters of C1 and D1 levels were more suitable, at 50 C
D1 levels were more suitable, at 50 °C and 600 rpm, respectively. Of the nine samples,
and 600 rpm, respectively. Of the nine samples, sample 1 had the best morphology, highest
sample 1 had the best morphology, highest coverage rate, and the second highest yield.
coverage rate,
Combined withand the second highest
the preparation parameter yield. Combined
of this sample of with the preparation
A1B1C1D1, the better parameter
prep‐ of
aration process was determined to be A1B1C1D1: the molar ratio of urea and formalde‐
hyde was 1:1.20, the mass ratio of core material to wall material was 1:15, the tempera‐
ture was 50 °C, and the stirring speed was 600 rpm.
Polymers 2023, 15, 1728 10 of 22
this sample of A1B1C1D1, the better preparation process was determined to be A1B1C1D1:
the molar ratio of urea and formaldehyde was 1:1.20, the mass ratio of core material to wall
material was 1:15, the temperature was 50 ◦ C, and the stirring speed was 600 rpm.
On the basis of these process parameters, in order to further study the effect of the
molarOn theof
ratio basis
ureaofand
these process parameters,
formaldehyde in order to further
on the performance study the effect
of the aloe-emodin of the
microcapsules,
molar ratio of urea and formaldehyde on the performance of the aloe‐emodin
the molar ratio of urea and formaldehyde was selected as a single factor variable to conduct microcap‐
asules, the molar ratio of urea and formaldehyde was selected as a single factor variable
single factor test. In the test of yield and coverage rate, it was found that the parameter
to conduct a single factor test. In the test of yield and coverage rate, it was found that the
with the molar ratio of urea and formaldehyde set at 1:1.2 was the best. Considering that
parameter with the molar ratio of urea and formaldehyde set at 1:1.2 was the best. Con‐
excessive formaldehyde will volatilize into the air and cause pollution, which does not
sidering that excessive formaldehyde will volatilize into the air and cause pollution,
conform to standards of health and environmental protection, in the single factor test, the
which does not conform to standards of health and environmental protection, in the sin‐
molar ratio of urea and formaldehyde was controlled as follows: 1:1.00, 1:1.10, 1:1.15, 1:1.20,
gle factor test, the molar ratio of urea and formaldehyde was controlled as follows:
1:1.25, 1:1.30, 1:1.35, 1:1.40, 1:1.50. Table 11 shows the corresponding yields and coverage
1:1.00, 1:1.10, 1:1.15, 1:1.20, 1:1.25, 1:1.30, 1:1.35, 1:1.40, 1:1.50. Table 11 shows the corre‐
rates of
sponding theyields
microcapsules
and coverage in the single
rates factor
of the test. These in
microcapsules results indicated
the single that
factor theThese
test. coverage
rate of sample
results indicated 12,that
sample 13, and sample
the coverage rate of 15 was the
sample 12, highest, exceeding
sample 13, 9.0%.
and sample 15Among
was thethem,
sample
highest, 13, namely,9.0%.
exceeding the microcapsule
Among them,with samplethe13,
molar ratiothe
namely, of urea and formaldehyde
microcapsule with the of
1:1.20, had the
molar ratio highest
of urea yield, up to 11.91
and formaldehyde g, and
of 1:1.20, was
had thethe best yield,
highest microcapsule sample
up to 11.91 g, andin the
single factor test.
was the best microcapsule sample in the single factor test.
Table Microcapsuleyields
Table 11. Microcapsule yieldsand
andcoverage
coverage rates
rates in the
in the single
single factor
factor experiment.
experiment.
Sample n (Urea):n (Formaldehyde)

n (Urea):n Yield (g) Coverage Rate (%)
Sample Yield (g) Coverage Rate (%)
10 1:1.00
(Formaldehyde) 11.59 8.4
11 10 1:1.10
1:1.00 11.78
11.59 7.3 8.4
12 11 1:1.15
1:1.10 11.27
11.78 9.1 7.3
13 12 1:1.20
1:1.15 11.91
11.27 9.3 9.1
14 13 1:1.20
1:1.25 11.91
11.51 6.8 9.3
15 14 1:1.25
1:1.30 11.51
11.11 9.1 6.8
15 1:1.30 11.11 9.1
16 1:1.35 11.32 8.1
16 1:1.35 11.32 8.1
17 17 1:1.40
1:1.40 11.21
11.21 7.9 7.9
18 18 1:1.50
1:1.50 9.769.76 6.4 6.4
3.2. Analysis of the Morphology of the Microcapsules

3.2. Analysis of the Morphology of the Microcapsules
The micromorphology of the core material aloe‐emodin powder and the urea‐
The micromorphology of the core material aloe-emodin powder and the urea-formaldehyde
formaldehyde resin wall material powder prepared in this experiment is shown in Fig‐
resin wall material powder prepared in this experiment is shown in Figure 3. Aloe-emodin
ure 3. Aloe‐emodin appears as a long crystal because aloe‐emodin itself is a large particle
appears as a long crystal because aloe-emodin itself is a large particle of dark orange
of dark orange needle‐like crystal. The wall material appears as large irregular agglom‐
needle-like crystal.
erates because The wall material resin
the urea‐formaldehyde appears as large irregular
prepolymer itself has agglomerates
viscosity. Afterbecause
being the
urea-formaldehyde resin prepolymer itself has viscosity. After being ground into powder,
ground into powder, the material particles are large, and there is still a large area of ad‐
the material
hesion particles are large, and there is still a large area of adhesion and aggregation.
and aggregation.
Figure 3.
Figure 3. OM
OMimages
imagesofofwall
walland
andcore material:
core (A)(A)
material: wall material
wall andand
material (B) core material.
(B) core material.
The micromorphology
The micromorphologyofofmicrocapsules
microcapsules prepared
preparedfrom the the
from orthogonal test is
orthogonal shown
test is shown
in Figure 4. Compared with the wall material and the core material, the prepared
in Figure 4. Compared with the wall material and the core material, the prepared micro‐ micro-
capsules had
capsules had aa significantly
significantlysmaller
smallerparticle size,
particle presenting
size, a spherical
presenting shape,
a spherical basically
shape, basically
without large agglomerates and needle‐like crystals. It can be seen that the core material
Polymers 2023, 15, 1728 11 of 22
without large agglomerates and needle-like crystals. It can be seen that the core material
was well emulsified and dispersed, and the wall material was also more evenly coated
was well emulsified and dispersed, and the wall material was also more evenly coated
around the core material. Among them, sample 1 and sample 2 had the best morphology,
around the core material. Among them, sample 1 and sample 2 had the best morphology,
with more microcapsules and uniform dispersion and less agglomeration. The morphology
with more microcapsules and uniform dispersion and less agglomeration. The morphol‐
of sample 6 and sample 9 was poor, and the microcapsules were fewer and had obvious
ogy of sample 6 and sample 9 was poor, and the microcapsules were fewer and had ob‐
aggregation. This may be because the mass ratio of the core material to the wall material of
vious aggregation. This may be because the mass ratio of the core material to the wall
the two samples was 1:25, and the excessive wall material caused the agglomeration and
material of the two samples was 1:25, and the excessive wall material caused the ag‐
deposition
glomerationofand
the deposition
redundantofurea-formaldehyde resin, which affected
the redundant urea‐formaldehyde the formation
resin, which affected and
dispersion of the microcapsules.
the formation and dispersion of the microcapsules.
Figure 4.
Figure 4. OM
OM images
images ofof microcapsules
microcapsulesininthe
theorthogonal
orthogonaltest:
test:(A) sample
(A) 1, 1,
sample (B)(B)
sample 2, (C)
sample sam‐
2, (C) sample
ple 3, (D) sample 4, (E) sample 5, (F) sample 6, (G) sample 7, (H) sample 8 and (I) sample 9.
3, (D) sample 4, (E) sample 5, (F) sample 6, (G) sample 7, (H) sample 8 and (I) sample 9.
Figure 55 shows
Figure shows thethemicromorphology
micromorphology of of
thethe
microcapsules
microcapsules prepared
preparedin thein single
the single
factor experiment. The morphology of samples 10–16 was good, and the microcapsules
factor experiment. The morphology of samples 10–16 was good, and the microcapsules
were mellow and evenly dispersed. Among them, the morphology of samples 12 and 13
were mellow and evenly dispersed. Among them, the morphology of samples 12 and
prepared with the molar ratios of urea and formaldehyde of 1:1.15 and 1:1.20 was the
13 prepared with the molar ratios of urea and formaldehyde of 1:1.15 and 1:1.20 was the
best, which indicated that this parameter was better. The micromorphology of samples
best, which indicated that this parameter was better. The micromorphology of samples
17 and 18 was poor, as the molar ratios of urea and formaldehyde were 1:1.40 and 1:1.50,
17 and 18 was poor, as the molar ratios of urea and formaldehyde were 1:1.40 and 1:1.50,
which indicated that excessive formaldehyde was not conducive to the formation of the
which indicated
microcapsules. that excessive
Figure 6 is the SEMformaldehyde was not
images of samples 10,conducive
13, 15, and to
17.the formation
In Figure 6A,B,of the
microcapsules.
we see that when the molar ratio of urea and formaldehyde was low, the microcapsules6A,B,
Figure 6 is the SEM images of samples 10, 13, 15, and 17. In Figure
we seespherical,
were that when thea molar
with smoothratio of urea
surface and aand formaldehyde
small was low, the microcapsules
amount of agglomeration. It can also
were spherical, with a smooth surface and a small amount of agglomeration.
be seen in Figure 6C,D that when the molar ratio was too high, although the microcap‐ It can also be
seen in Figure 6C,D that when the molar ratio was too high, although the
sules displayed a spherical shape, the phenomenon of adhesion was obvious, and there microcapsules
displayed
were manyaagglomerations.
spherical shape, the phenomenon of adhesion was obvious, and there were
many agglomerations.
Polymers 2023,
Polymers 15,15,
2023, 1728
x FOR PEER REVIEW 12 of 22
12 of 23
Figure 5.
Figure 5. OM
OMimages
imagesof of
microcapsules in theinsingle
microcapsules factor experiment:
the single (A) sample
factor experiment: (A)10,sample
(B) sample
10, 11,
(B)(C)
sample
sample 12, (D) sample 13, (E) sample 14, (F) sample 15, (G) sample 16, (H) sample 17, and (I) sample 18.
11,
Figure 5. OM images of microcapsules in the single factor experiment: (A) sample 10, (B) sample 11, (C) and
(C) sample 12, (D) sample 13, (E) sample 14, (F) sample 15, (G) sample 16, (H) sample 17,
(I) sample
sample 18. sample 13, (E) sample 14, (F) sample 15, (G) sample 16, (H) sample 17, and (I) sample 18.
12, (D)
Figure 6. SEM images of microcapsules in the single factor experiment: (A) sample 10, (B) sample
13, (C) sample 15, and (D) sample 17.
Figure 6.
Figure 6. SEM
SEM images
images ofof microcapsules
microcapsulesininthe
thesingle
singlefactor
factorexperiment:
experiment:(A) sample
(A) 10,10,
sample (B)(B)
sample
sample 13,
13, (C)Taking
sampleinto
15, and (D) sample 17.
account the microcapsule yield, coating rate, and micromorphology,
(C) sample 15, and (D) sample 17.
sample 13 had the highest coating rate and yield, with uniform dispersion, smooth and
roundTaking
Taking into and
into
particles, account
account the microcapsule
the
excellent microcapsule yield, coating
morphology. yield, coating
Therefore, rate,13
rate,
sample and
and
wasmicromorphology,
micromorphology,
added to the wa‐ sam-
sample 13 had the highest coating rate and yield, with uniform dispersion,
ple 13 had the highest coating rate and yield, with uniform dispersion, smooth smooth and
and round
round particles, and excellent morphology. Therefore, sample 13 was added to the
particles, and excellent morphology. Therefore, sample 13 was added to the water-based wa‐
coatings with the mass fractions of 0%, 1.0%, 3.0%, 6.0%, 9.0%, and 12.0%, and the paint
Polymers 2023, 15, 1728 13 of 22
films werecoatings
ter‐based prepared bythe
with mold to fractions
mass determine of the
0%,effect
1.0%, of the 6.0%,
3.0%, aloe-emodin microcapsules
9.0%, and 12.0%, and on
the antibacterial and optical properties of the water-based coating.
the paint films were prepared by mold to determine the effect of the aloe‐emodin micro‐
capsules on the antibacterial and optical properties of the water‐based coating.
3.3. Analysis of the Morphology of the Paint Films
Figure 7A–F
3.3. Analysis of the shows
Morphology the macro morphology
of the Paint Films of the paint films with 0%, 1.0%, 3.0%, 6.0%,
9.0%,Figure
and 12.0% aloe-emodin microcapsules
7A–F shows the macro morphology added,
of the respectively.
paint films It can0%,
with be clearly observed
1.0%, 3.0%,
from
6.0%,the figure
9.0%, andthat12.0%thealoe‐emodin
film withoutmicrocapsules
microcapsule added,loadingrespectively.
is colorless andIt can transparent,
be clearly and
the films loaded
observed from the with
figuremicrocapsules
that the filmare yellowmicrocapsule
without and transparent. loadingWhen the content
is colorless and was
higher than 6.0%,
transparent, and the it showed
films loaded orange.withWith the increase
microcapsules are in the aloe-emodin
yellow and transparent. microcapsules,
When
the
the color
content of the
waspaint
higherfilms gradually
than 6.0%, it darkened and theWith
showed orange. transparency
the increasegradually
in the decreased.
aloe‐
This
emodinoccurred becausethe
microcapsules, thecolor
microcapsules were gradually
of the paint films orange and not transparent.
darkened and the transpar‐ With the
increase in the loading,
ency gradually decreased. theThis
average distribution
occurred because the of microcapsules
microcapsules were in theorange
coating andincreased,
not
affecting
transparent. theWith
colortheandincrease
transparency of the paint
in the loading, films. In
the average addition, Figure
distribution 7E shows that
of microcapsules
in the the
when coating increased,
loading reached affecting
9.0%, tinythe color
cracks and transparency
began to appear ofatthe paint
the edge films.
of the In paint
addi‐ film.
tion, Figure 7E shows that when the loading reached 9.0%,
Figure 7F shows that when the loading was 12.0%, the cracks on the edge of the paint tiny cracks began to appear
at the
film lededge
to anofincomplete
the paint film. paint Figure 7F shows
film, and that when of
the distribution themicrocapsules
loading was 12.0%, in the the
coating
cracks on the edge of the paint film led to an incomplete paint
was uneven, resulting in uneven color and uneven paint film. This occurred because the film, and the distribution
of microcapsules
content in the coating
of the aloe-emodin was uneven, resulting
microcapsules was too in uneven
high, color and
resulting in auneven
smaller paint
content
film. This occurred because the content of the aloe‐emodin
of the water-based coating and poor viscosity and leveling, indicating that the microcapsules was too high,
coating
resulting
with 12.0% smaller was
in aloading content notofsuitable
the water‐based coating
for practical and poor viscosity
application. Figure and 8A–D leveling,
shows the
indicating that
microscopic the coating with
morphology of the12.0%
paintloading was not
films with 0%,suitable
3.0%, 6.0%,for practical
and 9.0% application.
aloe-emodin
Figure 8A–D shows the microscopic morphology of the
microcapsules added, respectively. The paint film surface without microcapsule paint films with 0%, 3.0%, 6.0%,loading
and 9.0% aloe‐emodin microcapsules added, respectively. The paint film surface without
was level and smooth. When the loading was 3.0% and 6.0%, the paint film surface showed
microcapsule loading was level and smooth. When the loading was 3.0% and 6.0%, the
slight wrinkles. When the loading reached 9.0%, as shown in Figure 8D, in addition to
paint film surface showed slight wrinkles. When the loading reached 9.0%, as shown in
wrinkles, there were many visible bumps on the paint film surface. This occurred because
Figure 8D, in addition to wrinkles, there were many visible bumps on the paint film sur‐
there were too many microcapsules, which could not be evenly dispersed in the coating, so
face. This occurred because there were too many microcapsules, which could not be
they gathered together and produced large particles on the surface. It can be seen that the
evenly dispersed in the coating, so they gathered together and produced large particles
microcapsule
on the surface.content It can higher
be seenthan that 9.0% had a strongcontent
the microcapsule negative effectthan
higher on the 9.0%transparency
had a
and flatness of the paint films.
strong negative effect on the transparency and flatness of the paint films.
Figure 7.
Figure 7. Macro
Macromorphology
morphologyof the
ofpaint films: (A)
the paint 0% microcapsule‐loaded
films: film, (B) 1.0%
(A) 0% microcapsule-loaded micro‐
film, (B) 1.0%
capsule‐loaded film, (C) 3.0% microcapsule loaded‐film, (D) 6.0% microcapsule‐loaded film, (E)
microcapsule-loaded film, (C) 3.0% microcapsule loaded-film, (D) 6.0% microcapsule-loaded film,
9.0% microcapsule‐loaded film, and (F) 12.0% microcapsule‐loaded film.
(E) 9.0% microcapsule-loaded film, and (F) 12.0% microcapsule-loaded film.
Polymers 2023,
Polymers 15,15,
2023, 1728
x FOR PEER REVIEW 14 of 22
14 of 23
Figure 8.
Figure 8. SEM
SEM images
imagesofofthe
thepaint
paintfilms: (A)(A)
films: 0%0%
microcapsule‐loaded film,film,
microcapsule-loaded (B) 3.0% microcapsule‐
(B) 3.0% microcapsule-
loaded film, (C) 6.0% microcapsule‐loaded film and (D) 12.0% microcapsule‐loaded film.
loaded film, (C) 6.0% microcapsule-loaded film and (D) 12.0% microcapsule-loaded film.
3.4. Infrared
3.4. Infrared Spectrum
SpectrumAnalysis
Analysisofofthethe
Microcapsule andand
Microcapsule Paint Films
Paint Films
Figure 99illustrates
Figure illustrates
thethe absorption
absorption spectrogram
spectrogram of theof the aloe‐emodin,
aloe-emodin, the urea‐
the urea-formaldehyde
resin, and the microcapsules. The peaks at 3350 cm , 2950 cm , and 1630 cm 1630
formaldehyde resin, and the microcapsules. The peaks at 3350 cm , 2950 cm
− 1 −1
− 1 −1, and− 1 are the
cm −1 are the stretching vibration peaks of O‐H, the bending vibration peak of C‐H, and
stretching vibration peaks of O-H, the bending vibration peak of C-H, and the stretching
the stretching
vibration peakvibration
of C=O.peak of C=O.
These These characteristic
characteristic peaks were peaks were
jointly jointly possessed
possessed by the aloe-
by the aloe‐emodin and urea‐formaldehyde resin and can also be clearly seen in the ab‐
emodin and urea-formaldehyde resin and can also be clearly seen in the absorption curve
sorption curve of microcapsules. The peak−at 1 1550 cm−1 is the characteristic peak of C‐N
of microcapsules. The peak at 1550 cm is the characteristic peak of C-N in the urea-
in the urea‐formaldehyde resin, and the peak at 1247 cm−1 was caused by the stretching
formaldehyde resin, and the peak at 1247 cm−1 was caused by the stretching vibration of
vibration of C‐N and the deformation vibration of N‐H in the urea‐formaldehyde resin.
C-N and the deformation vibration of N-H in the urea-formaldehyde resin. These were the
These were the characteristic peaks of the wall material and the microcapsules, indicat‐
characteristic peaks of the wall material and the microcapsules, indicating the existence
ing the existence of urea‐formaldehyde resin in the microcapsules [36,37]. The peak at
of urea-formaldehyde resin in the microcapsules [36,37]. The peak at 1045 cm−1 is the
1045 cm−1 is the C‐O‐C absorption peak of dimethylol urea in the urea‐formaldehyde res‐
C-O-C
in. The absorption
specific C=Cpeak of dimethylol
in aloe‐emodin urea at
appears in1570
the urea-formaldehyde resin. The
cm−1 [38], and this absorption specific
peak
C=C in aloe-emodin appears at 1570 cm −1 [38], and this absorption peak also appears in
also appears in the absorption curve of microcapsules, which indicated that there was a
the absorption
chemical curveofofaloe‐emodin
component microcapsules, which
in the indicated The
microcapsules. that above
there was a chemical
characteristic compo-
peaks
nent
proved of aloe-emodin in the microcapsules.
that the microcapsules contained core The above
material andcharacteristic
wall material,peaks proved
and the that the
chemical
microcapsules
composition wascontained
not damaged,coreproving
material
thatand
the wall material,
microcapsule and the
coating waschemical
successful.composition
was not damaged, proving that the microcapsule coating was successful.
Figure 10 is the absorption spectrogram of the film without microcapsules and the
films with microcapsules. The peaks at 3350 cm−1 , 2950 cm−1 , and 1144 cm−1 are the peaks
of O-H, C-H, and C-O that were found in the water-based coating and the microcapsules.
The characteristic peak at 1729 cm−1 belongs to the telescopic vibration peak of C=O in
the water-based coating. The expansion vibration peak of (-CH2 )-CH2 in the waterborne
coating appears at 1450 cm−1 . These characteristic peaks can be seen in the four curves,
indicating that the chemical composition of the water-based coating was not damaged
after mixing with the microcapsules. The 1560 cm−1 peak is characteristic of C=N in the
microcapsule wall material, and the peak at 1632 cm−1 is the absorption peak of C=O in
the microcapsule core material. These peaks can be seen in the curves of the films loaded
with microcapsules, which proved that the chemical composition of the microcapsules
in the water-based coating did not change. The existence of these characteristic peaks
indicates that after the microcapsules were mixed with the water-based coating, there was
no chemical reaction with the coating, and the components of the water-based coating and
the microcapsules remained intact and effective.
Polymers 2023, 15, 1728 15 of 22
Figure 9. FTIR image of the core material, the wall material, and the microcapsules.
films with microcapsules. The peaks at 3350 cm−1, 2950 cm−1, and 1144 cm−1 are the peaks
of O‐H, C‐H, and C‐O that were found in the water‐based coating and the microcap‐
sules. The characteristic peak at 1729 cm−1 belongs to the telescopic vibration peak of
C=O in the water‐based coating. The expansion vibration peak of (‐CH2)‐CH2 in the wa‐
terborne coating appears at 1450 cm−1. These characteristic peaks can be seen in the four
curves, indicating that the chemical composition of the water‐based coating was not
damaged after mixing with the microcapsules. The 1560 cm−1 peak is characteristic of
C=N in the microcapsule wall material, and the peak at 1632 cm−1 is the absorption peak
of C=O in the microcapsule core material. These peaks can be seen in the curves of the
films loaded with microcapsules, which proved that the chemical composition of the mi‐
crocapsules in the water‐based coating did not change. The existence of these character‐
istic peaks indicates that after the microcapsules were mixed with the water‐based coat‐
ing, there was no chemical reaction with the coating, and the components of the water‐
Figure
Figure9.coating
based 9.FTIR
FTIRimage ofof
image
and the the core
the material,
core thethe
material,
microcapsules remainedwall material,
wall and
material,
intact and thethe
and microcapsules.
microcapsules.
effective.
films with microcapsules. The peaks at 3350 cm−1, 2950 cm−1, and 1144 cm−1 are the peaks
of O‐H, C‐H, and C‐O that were found in the water‐based coating and the microcap‐
sules. The characteristic peak at 1729 cm−1 belongs to the telescopic vibration peak of
C=O in the water‐based coating. The expansion vibration peak of (‐CH2)‐CH2 in the wa‐
terborne coating appears at 1450 cm−1. These characteristic peaks can be seen in the four
curves, indicating that the chemical composition of the water‐based coating was not
damaged after mixing with the microcapsules. The 1560 cm−1 peak is characteristic of
C=N in the microcapsule wall material, and the peak at 1632 cm−1 is the absorption peak
of C=O in the microcapsule core material. These peaks can be seen in the curves of the
films loaded with microcapsules, which proved that the chemical composition of the mi‐
crocapsules in the water‐based coating did not change. The existence of these character‐
istic peaks indicates that after the microcapsules were mixed with the water‐based coat‐
ing, there was no chemical reaction with the coating, and the components of the water‐
based coating and the microcapsules remained intact and effective.
Figure
Figure10.
10.FTIR
FTIRimage
imageofof
thethe
paint films.
paint films.
3.5. Analysis of the Influence of Different Microcapsule Loading on the Antibacterial Property of
the Paint Films
Table 12 and Figure 11 show the actual number of colonies and the antibacterial rates
of the paint films with different loadings of the aloe-emodin microcapsules after the an-
tibacterial tests on the Escherichia coli and the Staphylococcus aureus. Figures 12 and 13 are
the bacterial colonies recovered after the antibacterial test. It can be seen from the data
that with the increase in the loading, the antibacterial rate against both kinds of bacteria
gradually increased, and the antibacterial effect gradually increased, reaching 83.6% and
81.6%, respectively. The antibacterial function of the paint films against the Escherichia
coli was slightly better than that of the Staphylococcus aureus. When the loading was 6.0%,
the antibacterial rate against the Staphylococcus aureus was slightly higher than against
the Escherichia coli. These results indicated that the microcapsules successfully played an
antibacterial role in the paint films. They showed that the aloe-emodin was microencapsu-
lated and coated with urea-formaldehyde resin, which not only improved the problems of
too-dark color and too-large particles, but also preserved its original antibacterial properties.
This may
Figure have
10. FTIR beenofbecause
image after
the paint drying, owing to the volatilization of the solvent, the wall
films.
material and the film produced tiny voids through which the aloe-emodin slowly inhibited
the growth of the Escherichia coli and the Staphylococcus aureus.
higher than against the Escherichia coli. These results indicated that the microcapsules
successfully played an antibacterial role in the paint films. They showed that the aloe‐
emodin was microencapsulated and coated with urea‐formaldehyde resin, which not
only improved the problems of too‐dark color and too‐large particles, but also preserved
Polymers 2023, 15, 1728 its original antibacterial properties. This may have been because after drying, owing to 16 of 22
the volatilization of the solvent, the wall material and the film produced tiny voids
through which the aloe‐emodin slowly inhibited the growth of the Escherichia coli and
the Staphylococcus aureus.
Table 12. Antibacterial rates of the paint films with different loadings of the microcapsules.
Table 12. Antibacterial rates of the paint films with different loadings of the microcapsules.
Average Number
Average Number Antibacterial Rate Antibacterial Rate
Content of the Antibacterial of Recovered
Content of Recovered
of the Average Number of Against
Average NumberStaphylococcus
of Re‐ Against
Antibacterial Rate
Microcapsules Rate Against
Microcapsules Recovered Escherichia coli
Escherichia Escherichia
coveredcoli
Staphylococcus Against Staphylococcus
Staphylococcus
(%) Escherichia
−1 ) coli (%) aureus
(CFU−1·piece aureus (%)
(%) coli (CFU∙piece )
(%)
aureus (CFU∙piece −1)
(CFU ·piece−1 )aureus (%)
0 0 213 213 ‐ - 163 163 ‐ -
1.0 1.0 137 137 35.7 35.7 124 124 23.9 23.9
3.0 3.0 109 109 48.8 48.8 81 81 50.3 50.3
6.0 6.0 68 68 68.1 68.1 64 64 60.7 60.7
9.0 9.0 57 57 73.2 73.2 46 46 71.8 71.8
12.0
12.0 35
35 83.6
83.6 30
30 81.6
81.6

Figure
Figure 11.11. Antibacterial
Antibacterial ratesrates of paint
of the the paint
films.films.
Figure 12.
Figure 12. Escherichia
Escherichiacoli coli
colonies recovered
colonies after antibacterial
recovered test of the paint
after antibacterial films:
test of the (A) 0% microcap‐
paint films: (A) 0%
sule‐loaded film, (B) 1.0% microcapsule‐loaded film, (C) 3.0% microcapsule‐loaded film, (D) 6.0% mi‐
microcapsule-loaded film, (B) 1.0% microcapsule-loaded film, (C) 3.0% microcapsule-loaded film,
crocapsule‐loaded film, (E) 9.0% microcapsule‐loaded film, and (F) 12.0% microcapsule‐loaded film.
(D) 6.0% microcapsule-loaded film, (E) 9.0% microcapsule-loaded film, and (F) 12.0% microcapsule-
loaded film.
Polymers 2023, 15, 1728 Figure 12. Escherichia coli colonies recovered after antibacterial test of the paint films: (A) 0% microcap‐
17 of 22
sule‐loaded film, (B) 1.0% microcapsule‐loaded film, (C) 3.0% microcapsule‐loaded film, (D) 6.0% mi‐
crocapsule‐loaded film, (E) 9.0% microcapsule‐loaded film, and (F) 12.0% microcapsule‐loaded film.
Figure 13.
Figure 13. Staphylococcus
Staphylococcusaureus
aureuscolonies recovered
colonies after
recovered antibacterial
after test of
antibacterial testthe
ofpaint films:films:
the paint (A) 0%
(A) 0%
microcapsule‐loaded film, (B) 1.0% microcapsule‐loaded film, (C) 3.0% microcapsule‐loaded film,
microcapsule-loaded film, (B) 1.0% microcapsule-loaded film, (C) 3.0% microcapsule-loaded film,
(D) 6.0% microcapsule‐loaded film, (E) 9.0% microcapsule‐loaded film, and (F) 12.0% microcap‐
(D) 6.0% microcapsule-loaded
sule‐loaded film. film, (E) 9.0% microcapsule-loaded film, and (F) 12.0% microcapsule-
loaded film.
3.6. Analysis of the Influence of Different Microcapsule Loading on the Optical Properties of the
3.6. Analysis of the Influence of Different Microcapsule Loading on the Optical Properties of the
Paint Films
Paint Films
The chromaticity value and color difference of the paint films are indicated in Table
The chromaticity value and color difference of the paint films are indicated in Table 13
13 and Figure 14. With the increase in the aloe‐emodin microcapsules, the color differ‐
and Figure 14. With the increase in the aloe-emodin microcapsules, the color difference of
ence of the films loaded with the microcapsules compared with the film without micro‐
the films loaded with the microcapsules compared with the film without microcapsules
capsules was on the rise. The b value indicating the yellow color also showed the same
was on the rise. The b value indicating the yellow color also showed the same trend, which
trend, which indicated that the yellow degree of the paint films became darker. This oc‐
indicated that the yellow degree of the paint films became darker. This occurred because
curred because the microcapsule itself was yellow. On the contrary, the value of L, which
the microcapsule itself was yellow. On the contrary, the value of L, which represented the
brightness, showed a downward trend. This occurred because the microcapsules were
granular powder and did not chemically react with the coating. The state of existence of the
coating was always granular. Therefore, after the addition of microcapsules to the coating,
the density and ductility of the liquid coating itself were affected, resulting in a reduction
in the surface smoothness and brightness of the dried paint films.
Table 13. Chromaticity value and color difference value of the paint films.
Content of the
L a b ∆E
Microcapsules (%)
0 93.64 ± 0.7 −0.77 ± 0.7 3.78 ± 0.4 -
1.0 90.57 ± 1.5 −4.67 ± 2.5 29.71 ± 0.9 26.40
3.0 83.17 ± 0.7 −1.03 ± 1.6 58.20 ± 2.8 55.41
6.0 82.82 ± 2.6 3.86 ± 1.6 62.54 ± 1.2 59.93
9.0 73.95 ± 2.4 14.99 ± 2.5 64.65 ± 1.2 65.88
12.0 59.01 ± 2.6 25.39 ± 2.1 72.69 ± 1.3 81.43
The gloss and gloss loss rates of the paint films are indicated in Table 14 and Figure 15.
As the microcapsule loading increased, the gloss gradually decreased, and the gloss loss
rate at 60◦ gradually increased. When the loading reached 12.0%, the gloss was the lowest,
and the loss rate was the highest, which was obviously not suitable for practical production
applications. This occurred because the granular microcapsules affected the smoothness of
the paint films after drying. When the content of microcapsules was high, the paint film
Content of the Microcapsules
L a b ΔE
(%)
0 93.64 ± 0.7 −0.77 ± 0.7 3.78 ± 0.4 ‐
1.0 90.57 ± 1.5 −4.67 ± 2.5 29.71 ± 0.9 26.40
Polymers 2023, 15, 1728 18 of 22
3.0 83.17 ± 0.7 −1.03 ± 1.6 58.20 ± 2.8 55.41
6.0 82.82 ± 2.6 3.86 ± 1.6 62.54 ± 1.2 59.93
9.0 73.95 ± 2.4 14.99 ± 2.5 64.65 ± 1.2 65.88
surface was12.0
rough and the diffuse
59.01reflection
± 2.6 of25.39
light±was
2.1 enhanced, so the gloss
72.69 ± 1.3 81.43 was very
low.
Figure 14. The trend of the chromaticity value and color difference value.
Figure 14. The trend of the chromaticity value and color difference value.
Table Gloss
The14.gloss and
and extinction
gloss rates
loss rates of of
thethe paint
paint films.
films are indicated in Table 14 and Figure 15.
As the microcapsule loading increased, the gloss gradually decreased, and the gloss loss rate
Content of the Gloss Loss Rate
at 60° gradually increased. When 20◦ (%) 60◦ (%)12.0%, the gloss
the loading reached 85◦ (%)
was the lowest, and
Microcapsules (%) (%)
the loss rate was the highest, which was obviously not suitable for practical production ap‐
0 occurred because
plications. This ± 0.7
93.64 the granular−microcapsules
0.77 ± 0.7 3.78 ±
affected the0.4smoothness of the
-
1.0 90.57 ± 1.5 − 4.67 ± 2.5 29.71 ± 0.9
paint films after drying. When the content of microcapsules was high, the paint film surface 26.40
was rough and 83.17 ± of
3.0 the diffuse reflection −1.03
0.7light was ± 1.6 so the58.20
enhanced, gloss±was2.8very low. 55.41
6.0 82.82 ± 2.6 3.86 ± 1.6 62.54 ± 1.2 59.93
Polymers 2023, 15, x FOR PEER REVIEW 9.0 73.95 ± 2.4 14.99 ± 2.5 64.65 ± 1.2 1965.88
of 23
Table 14. Gloss and extinction rates of the paint films.
12.0 59.01 ± 2.6 25.39 ± 2.1 72.69 ± 1.3 81.43
Content of the Microcapsules Gloss Loss Rate
20° (%) 60° (%) 85° (%)
(%) (%)
0 93.64 ± 0.7 −0.77 ± 0.7 3.78 ± 0.4 ‐
1.0 90.57 ± 1.5 −4.67 ± 2.5 29.71 ± 0.9 26.40
3.0 83.17 ± 0.7 −1.03 ± 1.6 58.20 ± 2.8 55.41
6.0 82.82 ± 2.6 3.86 ± 1.6 62.54 ± 1.2 59.93
9.0 73.95 ± 2.4 14.99 ± 2.5 64.65 ± 1.2 65.88
12.0 59.01 ± 2.6 25.39 ± 2.1 72.69 ± 1.3 81.43
Figure
Figure 15.15.
TheThe trend
trend of the
of the gloss
gloss andand
glossgloss
loss loss rate
rate of theofpaint
the paint
films.films.
AsAs shown
shown in in Figure
Figure 16, 16,
thethe transmittance
transmittance ofpaint
of the the paint filmnegatively
film was was negatively correlated
correlated
with the loading of the aloe-emodin microcapsules. The higher the loading,
with the loading of the aloe‐emodin microcapsules. The higher the loading, the lowerthe lower the
the transmittance. This occurred because the microcapsules were yellow and opaque,
and adding them to the transparent water‐based coating affected the light transmittance.
As seen from the curve, in the wavelength range of 400–480 nm, the transmittance of the
film with the microcapsules was far lower than that without the microcapsules, and the
transmittance reached the lowest value at 430 nm. This occurred because the paint films
Polymers 2023, 15, 1728 Figure 15. The trend of the gloss and gloss loss rate of the paint films. 19 of 22
As shown in Figure 16, the transmittance of the paint film was negatively correlated
with the loading of the aloe‐emodin microcapsules. The higher the loading, the lower
transmittance. This occurred because the microcapsules were yellow and opaque, and
the transmittance. This occurred because the microcapsules were yellow and opaque,
adding
and addingthem to the
them transparent
to the transparent water-based
water‐basedcoating
coating affected thelight
affected the lighttransmittance.
transmittance. As
As seen from the curve, in the wavelength range of 400–480 nm, the transmittance of theof the
seen from the curve, in the wavelength range of 400–480 nm, the transmittance
film with
film withthethemicrocapsules
microcapsules was
was farfar lower
lower thanthan
thatthat without
without the microcapsules,
the microcapsules, and the
and the
transmittance reached the lowest value at 430 nm. This occurred because the paint films films
transmittance reached the lowest value at 430 nm. This occurred because the paint
with microcapsules
with microcapsuleswere were yellow,
yellow, while
while purple
purple andand
blueblue are complementary
are the the complementary colorscolors
of of
yellow.The
yellow. Thewavelength
wavelength range
range waswas respectively
respectively between
between 400–450
400–450 nm and nm 450–480
and 450–480
nm. nm.
When the
When the visible
visible light
light passed
passed through
through the
the paint
paint films,
films, the
the purple light and blue light were
purple light
absorbed,
were and the
absorbed, andremaining
the remaininglightlight
intensity was was
intensity significantly lower
significantly thanthan
lower the the
incident
inci‐ light
intensity,
dent so the transmittance
light intensity, in this wave
so the transmittance in thisband
wavewasbandvery
waslow.
very low.
Figure16.
Figure Thetrend
16.The trendofofthe
the transmittance
transmittance of the
of the paint
paint films.
films.
3.7. Analysis of the Influence of Different Microcapsule Loadings on the Tensile Resistance and
Roughness of the Paint Films
The effect of the aloe-emodin microcapsules with different loadings on the tensile
resistance of the paint films is shown in Figure 17. It can be seen from the figure that when
the loading was less than 6.0%, the paint films had a certain elastic area, which decreased
with the increase in the loading. This may be because the microcapsule particles were
distributed in the paint film, which reduced the ductility of the water-based paint film itself.
When the content reached 9.0% and 12.0%, the tensile area of the paint films decreased
rapidly. At this time, the strain of the paint film under high stress was very small, which
indicated that the paint film was strong and had low ductility. This phenomenon may have
occurred because when the loading of the aloe-emodin microcapsules was too high, a large
number of microcapsules were filled in the paint film, which enhanced its hardness and
made it more brittle.
The elongation at the break of the paint film under different loadings is shown in
Table 15. The elongation at the break decreased with the increase in the loading. When the
loading was higher than 6.0%, the elongation at the break became very low. This occurred
because the aloe-emodin microcapsules were dispersed in the paint film in the form of
solid particles, which reduced the viscosity and elasticity of the paint itself. Therefore,
when subjected to tensile force, the relative elongation of the paint film decreased and the
elongation at the break decreased.
were distributed in the paint film, which reduced the ductility of the water‐based paint
film itself. When the content reached 9.0% and 12.0%, the tensile area of the paint films
decreased rapidly. At this time, the strain of the paint film under high stress was very
small, which indicated that the paint film was strong and had low ductility. This phe‐
nomenon may have occurred because when the loading of the aloe‐emodin microcap‐
Polymers 2023, 15, 1728 sules was too high, a large number of microcapsules were filled in the paint film, which20 of 22
enhanced its hardness and made it more brittle.
Figure
Figure17.
17.The
Thestress–strain curves
stress–strain of the
curves paint
of the films.
paint films.
TableThe
15. elongation at the
Elongation at thebreak
breakofofthe
the paint
paint film under different loadings is shown in
films.
Table 15. The elongation at the break decreased with the increase in the loading. When
the loading was higher
Content than 6.0%, the
of Microcapsules (%) elongation at the break became very
Elongation low.(%)
at Break This oc‐
curred because the aloe‐emodin microcapsules were dispersed in the paint film in the
0 31.2
form of solid particles,1.0which reduced the viscosity and elasticity 22.2 of the paint itself.
Therefore, when subjected 3.0 to tensile force, the relative elongation of 9.9 the paint film de‐
creased and the elongation6.0 at the break decreased. 4.9
9.0 4.3
Table 15. Elongation at the
12.0break of the paint films. 4.1
Content of Microcapsules (%) Elongation at Break (%)
Table 16 indicates
0 the roughness of the paint film under31.2 different microcapsule load-
ings. The roughness1.0of the paint film was on the rise because22.2the prepared microcapsules
were spherical particles
3.0 that were added to the water-based 9.9coating and then dried to
prepare the paint film.
6.0 The existing state in the paint film was granular.
4.9 With the increasing
addition, the particles
9.0 increased, resulting in the uneven surface
4.3 of the paint film and the
increase in roughness.
12.0 4.1
Table 16. Roughness of the paint films.
Content of Microcapsules (%) Roughness (µm)

0 0.13 ± 0.1
1.0 0.55 ± 0.2
3.0 0.89 ± 0.1
6.0 1.54 ± 0.1
9.0 2.14
12.0 2.67 ± 0.2
4. Conclusions
The optimum preparation parameters of the aloe-emodin microcapsules were as
follows: the molar ratio of urea and formaldehyde was 1:1.20, the mass ratio of core
material to wall material was 1:15, the reaction temperature of microencapsulation was
50 ◦ C, and the stirring speed of microencapsulation was 600 rpm. Based on the microcapsule
yield, coverage rate, and micromorphology, it can be concluded that the microcapsule had
the highest coverage rate and yield, up to 11.91 g and 9.0%, respectively, with uniform
dispersion, smooth and round particles. The effect of the increase in microcapsule loading
Polymers 2023, 15, 1728 21 of 22
on the performance of the paint films was as follows: the antibacterial rates of the paint
films against Escherichia coli and Staphylococcus aureus were gradually increased, with the
maximum reaching 83.6% and 81.6%, respectively; the color difference was increased, with
the maximum reaching 81.43; the glossiness was reduced; the light loss rate was increased;
the light transmittance was reduced; the tensile property was reduced; the elongation at the
break was decreased, with the minimum 4.1%; and the roughness was increased. When the
loading of the microcapsules was as high as 12.0%, the paint film was no longer suitable
for practical application. When the loading was 6.0%, the comprehensive performance of
the paint film was more suitable. The antibacterial microcapsules and water-based coating
were combined to successfully endow the coating with antibacterial function. This kind of
coating has potential application value in the fields of furniture painting and architectural
decoration.
Author Contributions: Conceptualization, methodology, validation, resources, data management,

and supervision, N.H.; formal analysis, investigation, X.Y.; and writing—review and editing, N.H.
All authors have read and agreed to the published version of the manuscript.
Funding: This project was partly supported by the Postgraduate Research & Practice Innovation
Program of Jiangsu Province (KYCX22_1098) and the Natural Science Foundation of Jiangsu Province
(Grant No. BK20201386).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The data presented in this study are available on request from the
corresponding author.
Conflicts of Interest: The authors declare that there is no conflict of interest.
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polymers

Academic Editor: Lacramioara Rusu 1. Introduction

Polymers 2023, 15, 1728. https://doi.org/10.3390/polym15071728 https://www.mdpi.com/journal/polymers

2. Materials and Methods

Table 1. List of the test materials.

2.2. Preparation Method of the Aloe-Emodin Microcapsules

Table 2. Formulation scheme of the orthogonal experiment.

Factor A Factor B Factor C Factor D

Table 3. Preparation parameters of the orthogonal experiment.

Factor A Factor B Factor C Factor D

Table 4. Material list of the orthogonal experiment.

Wall Polyvinyl Aloe-

Wall Polyvinyl Aloe-

Table 5. Material list of the single factor test.

Wall Polyvinyl Aloe-

2.3. Preparation Method of the Paint Films

Table 6. Dosage list of the water-based paint films.

2.4. Testing and Characterization

P = (m1 − m2 )/m1 × 100% (1)

2.4.2. Micromorphology and Chemical Composition Test of the Microcapsules

2.4.3. Antibacterial Test of the Paint Films

2.4.4. Optical Properties Test of the Paint Films

GL = ( G0 − G1 )/G0 × 100% (4)

2.4.5. Tensile and Roughness Test of the Paint Films

Polymers 2023, 15, x FOR PEER REVIEW 7 of 23

Table 8. Analysis table of variance.

Sources of Quadratic F-Critical

Table 9. Analysis of microcapsule coverage rate results.

Sample n (Urea):n (Formaldehyde)

3.2. Analysis of the Morphology of the Microcapsules

Polymers 2023, 15, x FOR PEER REVIEW 11 of 23

Polymers 2023, 15, x FOR PEER REVIEW 12 of 23

Polymers 2023, 15, x FOR PEER REVIEW 17 of 23

Table 16. Roughness of the paint films.

Content of Microcapsules (%) Roughness (µm)

Author Contributions: Conceptualization, methodology, validation, resources, data management,

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