sustainability
Article
Adsorption of Methylene Blue on Azo Dye Wastewater by
Molybdenum Disulfide Nanomaterials
Xiangxiang Wang 1,2 , Pengyu Zhang 1,2 , Fangwen Xu 1,2 , Bai Sun 1,2, *, Guiyun Hong 1,2 and Lining Bao 1,2
Citation: Wang, X.; Zhang, P.; Xu, F.;
Sun, B.; Hong, G.; Bao, L. Adsorption
of Methylene Blue on Azo Dye
Wastewater by Molybdenum
Disulfide Nanomaterials.
Sustainability 2022, 14, 7585.
https://doi.org/10.3390/su14137585
Academic Editor: Danilo Spasiano
Received: 13 April 2022
Accepted: 15 June 2022
Published: 22 June 2022
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Copyright: © 2022 by the authors.
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Attribution (CC BY) license (https://
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4.0/).
Sustainability 2022, 14, 7585. https://doi.org/10.3390/su14137585
1 Engineering Research Center of Building Energy Efficiency Control and Evaluation, Ministry of Education,
Anhui Jianzhu University, Hefei 230601, China; wangxiang156@126.com (X.W.); zpy110817@163.com (P.Z.);
19955631880@163.com (F.X.); honggy@ahjzu.edu.cn (G.H.); baolining@ahjzu.edu.cn (L.B.)
2 Department of Environment and Energy Engineering, Anhui Jianzhu University, Hefei 230601, China
* Correspondence: bsun@mail.ustc.edu.cn; Tel.: +86-551-63828252
Abstract: In this study, flower-like MoS2 nanomaterials were synthesized by hydrothermal method
with excess thiourea. The adsorption performance of MoS2 adsorbent for methylene blue (MB) in
azo dye wastewater was studied. The morphology, crystal phase, and microstructure of nano MoS2
samples were characterized by X-ray diffraction, scanning electron microscopy, energy dispersive
X-ray spectroscopy, and Fourier transform infrared spectroscopy. The effects of adsorption isotherm,
kinetics, different hydrothermal time, and pH on the adsorption experiment were studied. The results
showed that the MoS2 adsorbent with a hydrothermal time of 1 h had good adsorption properties for
MB. The adsorption data accord with the Langmuir isotherm model, and the maximum adsorption
capacity of MoS2 adsorbent is 200 mg/g, and the adsorption kinetics agrees well with the pseudo
two-level model. The removal rate of MB is not significantly affected by the pH values. The large pH
range can still maintain the removal rate above 93.47%, and the regeneration and recovery properties
of MoS2 were also explored. Finally, the adsorption mechanism of MoS2 on MB is discussed.
Keywords: adsorption; methylene blue; MoS2 nanomaterials
1. Introduction
The textile industry needs to discharge 80~180 tons of wastewater for each ton of
textiles processed. Therefore, the amount of dye wastewater is large, and it has the charac-
teristics of complex composition, deep color, large changes of pH value, and high chemical
oxygen demand (COD). It is one of the most difficult types of industrial wastewater to
treat. There are carcinogens in untreated dye wastewater, threatening the environment
and human health [1,2]. Azo dyes are the most widely used synthetic dyes in the printing
and dyeing process. They are characterized by connecting aryl groups at both ends of azo
groups, which can decompose more than 20 carcinogenic aromatic amines, cause lesions,
and induce cancer by changing the structure of human DNA [3]. Methylene blue (MB) is
an azo dye with a heterocyclic aromatic cation structure, which is often used in the textile
industry. Because its complex aromatic structure is difficult to be degraded by traditional
biological treatment processes [4,5], it is necessary to find an effective treatment method.
At present, the common methods for treating dye wastewater include coagulation [6],
ozone oxidation [7], photocatalytic oxidation [8], Fenton oxidation [9], magnetic separa-
tion [10], adsorption [11,12], etc. Among them, adsorption method makes the dye molecules
in the solution phase transfer to the surface of adsorbent, which is favored because of its
high efficiency, low cost, and easy operation. Commonly used adsorbents include activated
carbon, lignin, zeolite, metal organic framework, biomass residue, nano materials [13–16],
etc. In recent years, with the rapid development of nanotechnology, the application of
nano materials in the field of environment is also common. Similarly, the adsorption of dye
wastewater by nano materials has also attracted the attention of researchers. Liu et al. [17]
synthesized three-dimensional graphene oxide sponge as an adsorbent to explore the
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Sustainability 2022, 14, 7585 2 of 12

adsorption and removal of methyl violet by three-dimensional graphene oxide sponge.

The adsorption efficiency of methyl violet by this process in 2 min is 98.8%. CoFe2 O4 /Go
prepared by Anjali Gupta [18] et al. has a good adsorption effect on methylene blue and
methyl violet under the assistance of ultrasound. The adsorption capacity of single molecu-
lar layer is 157 mg g−1 and 122 mg g−1 . Synthesized by Allen [19] et al., MFe2 O4 @GO has
a maximum adsorption capacity of (M = Cu, Co, or Ni) for methylene blue of 25.81, 50.15,
and 76.34 mg g−1 .
In this paper, MoS2 nano adsorption materials were synthesized by hydrothermal
method. MB widely existing in industrial wastewater was used as the representative of
organic azo pollutants. The adsorption isotherm and adsorption kinetics were studied.
The materials were characterized by scanning electron microscope (SEM), X-ray diffrac-
tion (XRD), energy dispersive X-ray spectroscopy (EDS), and Fourier transform infrared
spectroscopy (FTIR). In addition, the effect of pH value on the experiment was also stud-
ied. According to the experimental results, the adsorption properties of the materials
were discussed.

2. Materials and Methods

2.1. Reagents and Instruments
The reagents used in the experiment mainly include ammonium molybdate tetrahy-
drate ((NH4 )6 MoO24 4H2 O) purchased from Sinopharm Chemical Reagent Co., Ltd. (Shang-
hai, China) and thiourea (H2 NCSNH2 ) purchased from Tianjin Bodi Chemical Co., Ltd.
(Tianjin, China), which was directly used without further purification. Deionized water was
prepared by FST-TOP-A24 super-pure-water mechanism, Shanghai FuShiTe Instrument
Equipment Co., Ltd. (Shanghai, China) [20].
The instruments required for the experiment are: DHG-9023A air drying box, Shanghai
YiHeng Scientific Instrument Co., Ltd. (Shanghai, China); PHB-3 digital pH meter, Shanghai
San-Xin Instrument Factory (Shanghai, China); FA2204N electronic balance, Shanghai
Jinghai instrument Co., Ltd. (Shanghai, China); TU-1950 dual-beam ultraviolet-visible
spectrophotometer, Beijing Puxi General Instrument Co., Ltd. (China). Making use of
CuKα(λKα1 = 1.5418 Å) as a radiation source in the range of 10◦ –90◦ ) in order to obtain
an XRD profile of adsorbent in D/MaxIIIAX-ray diffrtometer (Almero, Netherlands), SEM
image of the adsorbent was obtained with an FEI Quanta 200 FEG field emission scanning
electron microscopy. The EDS spectrum and elemental mapping were performed on a
Zeiss Auriga microscope ( Oberkochen, Germany) equipped with an Oxford Inca X-Max
50 detector. The FT-IR spectra of the adsorbents before and after adsorption were recorded
with a NEXUS-870 FT-IR spectrometer (Thermo Fisher Scientific, Waltham, MA, USA) in
the range of 4000–400 cm−1 [20].

2.2. Preparation of Adsorbent

MoS2 nano materials were prepared by one-step hydrothermal method using the
hydrothermal process of excess thiourea [21]. We dissolved 0.353 g ammonium molybdate
tetrahydrate and 1.830 g thiourea (molar S/Mo = 12.0) in 15 mL distilled water. After
stirring for 30 min, we transferred the solution to a stainless steel autoclave lined with
polytetrafluoroethylene. Next, we set the heating temperature to 240 ◦ C. In order to
consider the influence of different reaction time on the experiment, we set the heating time
to 1 h, 3 h, and 6 h, respectively. After natural cooling to room temperature, it was washed
by centrifugation for several times. Finally, it was dried in a vacuum drying oven at 50 ◦ C
for 12 h, and then, the solid was collected. Solid substances produced with heating times of
1.3 and 6 h are named, respectively, after MoS2 -1, MoS2 -2, and MoS2 -3.

2.3. Batch Adsorption Experiments

In this paper, alkaline azo dye MB, which is difficult to biodegrade, was selected to
simulate printing and dyeing wastewater. We set up the adsorption experiments of three
groups of different samples, which weighed 20 mg for each of the three adsorbents MoS2 -1,
Sustainability 2022, 14, 7585 3 of 12

MoS2 -2, and MoS2 -3, respectively. That is, 20 mg adsorbent was added to 20 mg/L and
200 mL MB solution. The whole experimental process was put into a dark shaking box for
adsorption treatment. The temperature was 25 ◦ C at room temperature, and the rotating
speed was 150 rpm/min. After the adsorption equilibrium, we took a certain amount of
supernatant, measured its absorbance at 664 nm with UV–Vis, and analyzed it.

3. Results
3.1. Sample Characterization
SEM contains information about the surface topology and composition of the sample.
The image of the synthetic sample shows the particle size and high pore structure. The SEM
can obtain the morphology of MoS2 nanoparticles, and shown in Figure 1a–c are the SEM
spectra of MoS2 -1, MoS2 -2, and MoS2 -3, respectively. The three flower-like samples of MoS2
have morphologically similar structures (samples are shown as microsphere-like flowers
under scanning electron microscopy), indicating that the reaction time has little effect on
the morphology of molybdenum disulfide samples. The tiny gaps are closely connected
with each other, and the surface of the material is loose and porous, indicating that the
material has a large specific surface area, which is conducive to adsorption. Under the same
proportion, the diameters of MoS2 -1, MoS2 -2, and MoS2 -3 are also slightly different. As
can be seen from Figure 1a–c, the diameter of MoS2 -1 is about 0.8 µm. MoS2 -2 and MoS2 -3
are approximately 2 µm in diameter. Figure 1d shows the electron microscope spectrum of
Sustainability 2022, 14, x FOR PEER MoS 2 -1 after adsorbing MB for one hour. From the image, there is no obvious change
REVIEW on13
4 of
the surface of MoS2 -1 after adsorbing MB for one hour, which is due to the tight gap, loose
and porous nano flower MoS2 , and large adsorption capacity.

Figure1.1.(a–c)
Figure (a–c)SEM
SEMspectra
spectra
ofof MoSgenerated
MoS 2 generated at different preparation times (1 h, 3 h, and 6 h),and
at different preparation times (1 h, 3 h, and 6 h), and
2
(d) SEM spectra of samples adsorbed for 1 h.
(d) SEM spectra of samples adsorbed for 1 h.

Figure 2 shows the XRD patterns of MoS2 -1, MoS2 -2, and MoS2 -3. It can be seen
from the figure that the positions of the main XRD diffraction peaks of the three samples
obtained at different heating times change little; the main diffraction peak is 2θ = 14.37◦ ,
33.50◦ , 35.87◦ , 39.53◦ , and 58.33◦ ; the main diffraction peaks of the obtained products are
consistent with the diffraction peaks of hexagonal phase molybdenum disulfide (MoS2 ,
Sustainability 2022, 14, 7585 4 of 12

jcpdsno. 37-1492), corresponding to (002), (100), (102), (103), and (110) crystal planes,
respectively. Apparently, the high characteristic peak strength of MoS2 is sufficient to prove
that the sample has good crystal crystallinity. The figure shows essentially the same of the
positions of the main diffraction peaks in the XRD spectra of the three samples. The results
display that the crystallization time had no significant effect on the crystallization process
of molybdenum disulfide. Figure 3 shows the EDS spectrum of molybdenum disulfide
sample. Table 1 shows the element content of MoS2 -1. It can be seen from the table that
the sample contains o, s, and Mo, and the atomic percentage between S and Mo is close
Figure 1. (a–c) SEM spectra of MoS2 generated at different preparation times (1 h, 3 h, and 6 h),and
to 2:1, indicating that the prepared sample is MoS2 . the result is consistent with the XRD
(d) SEM spectra of samples adsorbed for 1 h.
characterization results.

Sustainability 2022, 14, x FOR PEER REVIEW 5 of 13

Figure 2. XRD pattern of MoS2-1, MoS2-2, and MoS2-3.
Figure 2. XRD pattern of MoS2 -1, MoS2 -2, and MoS2 -3.

Figure 3. EDS spectrum of MoS2 adsorbent.

Figure 3. EDS spectrum of MoS2 adsorbent.
Table 1. element content of MoS2-1 sample.
Table 1. Element content of MoS2 -1 sample.
Elements Weight% Atomic%
Elements
O Weight%
0.33 Atomic%
18.63
OS 1.89
0.33 53.29
18.63
S
Mo 1.89
2.97 53.29
28.08
Mo 2.97 28.08
Total 100
Total 100

3.2. Adsorptive Property

3.2. Adsorptive Property
We added 20 mg of MoS2-1, MoS2-2, and MoS2-3 to 20 mg/L and 200 mL of MB solu-
tion.We added
After 20 mgequilibrium,
adsorption of MoS2 -1, MoS 2 -2, a
we took and MoSamount
certain 2 -3 to 20
ofmg/L and 200measured
supernatant, mL of MBits
solution. After adsorption equilibrium, we took a certain amount of supernatant,
absorbance with UV–Vis, and analyzed it. Figure 4 shows the effect of different measured
heating
times on the adsorption performance of MoS2 adsorbent. The experimental results show
that MoS2-1 has the maximum adsorption capacity, indicating that MoS 2 adsorbent with
reaction time of 1 h has high adsorption capacity for MB dye. By comparison of MB before
and after MoS2-1 adsorption, shown in Figure 5, it is clear that MoS2 is a good adsorbent
 Mo 2.97 28.08
Total 100

3.2. Adsorptive Property

Sustainability 2022, 14, 7585
We added 20 mg of MoS2-1, MoS2-2, and MoS2-3 to 20 mg/L and 200 mL of MB solu- 5 of 12
tion. After adsorption equilibrium, we took a certain amount of supernatant, measured its
absorbance with UV–Vis, and analyzed it. Figure 4 shows the effect of different heating
times on the adsorption performance of MoS2 adsorbent. The experimental results show
its absorbance with UV–Vis, and analyzed it. Figure 4 shows the effect of different heating
that MoS2-1 has the maximum adsorption capacity, indicating that MoS 2 adsorbent with
times on the adsorption performance of MoS2 adsorbent. The experimental results show
reaction time of 1 h has high adsorption capacity for MB dye. By comparison of MB before
that MoS -1 has the maximum adsorption capacity, indicating that MoS adsorbent with
and after 2MoS2-1 adsorption, shown in Figure 5, it is clear that MoS2 is a2good adsorbent
reaction time of 1 h has high adsorption capacity for MB dye. By comparison of MB before
for MB.
and after MoS2 -1 adsorption, shown in Figure 5, it is clear that MoS2 is a good adsorbent
for MB.

Sustainability 2022, 14, x FOR PEER REVIEW 6 of 13

Figure 4.
Figure Adsorption performance
4. Adsorption performance test
test of
of MoS
MoS22 nanoparticle
nanoparticleadsorbent
adsorbentfor
forMB.
MB.

Figure5.5.Comparison
Figure Comparisonof
ofMB
MBsolution
solutionbefore
beforeand
andafter
afteradsorption.
adsorption.

3.3.
3.3. Adsorption
AdsorptionIsotherm
IsothermModels
Models
Adsorption
Adsorptionisotherm
isothermisisused to to
used describe thethe
describe interaction process
interaction between
process adsorbent
between and
adsorbent
adsorbate and the equilibrium performance of adsorbent [22]. Langmuir
and adsorbate and the equilibrium performance of adsorbent [22]. Langmuir and Freun- and Freundlich
adsorption isotherm
dlich adsorption equations
isotherm are commonly
equations used. Langmuir
are commonly isotherm isotherm
used. Langmuir equation assumes
equation
that the adsorption layer is single-molecule uniform adsorption,
assumes that the adsorption layer is single-molecule uniform adsorption, andand each molecule has
each mole-
adsorption activation energy and isoenthalpy. Different from Langmuir isotherm
cule has adsorption activation energy and isoenthalpy. Different from Langmuir isotherm equation,
Freundlich adsorption adsorption
equation, Freundlich isotherm equation
isothermcanequation
be applied
cantobemultilayer
applied to adsorption,
multilayerwhich is
adsorp-
ation,
reversible,
whichnon-ideal, and uneven
is a reversible, adsorption
non-ideal, process adsorption
and uneven [23]. In order to study
process the In
[23]. adsorption
order to
study the adsorption performance of MoS2-1, Langmuir and Freundlich models and linear
equations were used. The equations corresponding to Langmuir and Freundlich are as
follows (1) and (2):

Ce Ce 1
= + (1)
qe qm K l + qm
1
lnqe = lnCe + lnK F (2)
n
Sustainability 2022, 14, 7585 6 of 12

performance of MoS2 -1, Langmuir and Freundlich models and linear equations were used.
The equations corresponding to Langmuir and Freundlich are as follows (1) and (2):

Ce Ce 1
= + (1)
qe qm Kl + qm

1
lnqe = lnCe + lnKF (2)
n
where Ce (mg/L) is the concentration after equilibrium adsorption; Qe (mg/g) is the
adsorption capacity after equilibrium, and Qm (mg/g) is the maximum adsorption capac-
ity calculated according to Langmuir equation; Kl (L/mg) is the adsorption constant of
Langmuir equation; KF (mg/g), n is the adsorption constant of Freundlich equation.
Figure 6a shows the fitting of Langmuir and Freundlich models to experimental data.
Figure 5b,c are the linear fitting curves of Langmuir model and Freundlich model for MB
adsorption by MoS2 adsorbent, respectively. The calculation results of the two models are
shown in Table 2. The fitting results show that according to the correlation coefficients
fitted by the two models, R2L = 0.994 > R2F = 0.975, the adsorption of MB by MoS2 conforms
to the Langmuir isotherm model, the adsorption type is uniform monolayer adsorption,
and the maximum adsorption capacity of MoS2 adsorbent is 200 mg/g. When the initial
MB concentration was 50 and 5 mg/L, the adsorption capacity of MB solution reached
Sustainability 2022, 14, x FOR PEER REVIEW
175.48 and 47.43 mg/g, respectively. It can be seen that the prepared MoS2 adsorbent 7 ofhas
13
good adsorption performance for MB. Table 3 shows the comparison of the adsorption
capacity of some adsorbents.

Figure 6. (a)
Figure 6. (a) The
Theisotherm
isothermofofadsorbed
adsorbed MB;
MB; (b)(b)
andand (c) the
(c) are are linear
the linear
fittingfitting
curvescurves of Langmuir
of Langmuir model
model and Freundlich
and Freundlich model model
for the for the adsorption
adsorption of MB solution
of MB solution by MoSbyadsorbent,
MoS 2 adsorbent, respectively.
respectively.
2

Table 2. the isotherm model parameters of MB solution adsorbed by MoS 2 adsorbent.

Langmuir Freundlich
Isotherm
𝐂𝐞 𝐂𝐞 𝟏 𝟏
Model = + 𝐥𝐧𝐪𝐞 = 𝐥𝐧𝐂𝐞 + 𝐥𝐧𝐊 𝐅
𝐪𝐞 𝐪𝐦 𝐊 𝐥 + 𝐪𝐦 𝐧
Parameters K (L/mg) q (mg/g) R2 n K R2
Sustainability 2022, 14, 7585 7 of 12

Table 2. The isotherm model parameters of MB solution adsorbed by MoS2 adsorbent.

Langmuir Freundlich
IsothermModel Ce Ce 1
qe = qm + Kl +qm
lnqe = n1 lnCe +lnKF

Parameters KL (L/mg) qmax (mg/g) R2 n KF R2

1.25 200 0.994 7.299 1.55 0.746

Table 3. Comparison of adsorption capacity of different adsorbents.

Adsorbents qmax (mg/g) Reference

Carbon aerogel 55.25 [24]
Chrysotile bundles with wedge-shaped nanopores 179.24 [25]
Hydrothermal conversion of red mud into magnetic adsorbent 89.6 [26]
Cerium modified chitosan ultrafine nanobiosorbent 57.5 [27]
γ-Fe2 O3 87.35 [28]
Natural chitosan/bone char composite 21.18 [29]
Activated carbon made from palm kernel chaff 120.6 [30]
Polydopamine nanofibers mat 161.3 [31]
Powder activated charcoal/titanate nanotube nanocomposites 173.3 [32]
MoS2 -1 200 Present work

3.4. Kinetic Study

The study of adsorption kinetics can determine the adsorption rate, efficiency, and
influencing factors and analyze the adsorption mechanism. The pseudo first-order kinetic
equation and pseudo second-order kinetic equation are usually used to fit the adsorption
experimental data [20,33]. The pseudo first-order dynamic equations and pseudo second-
order dynamic equations are as follows (3) and (4):


ln qe − qt = lnqe − k1 t (3)

t 1 t
= 2
+ (4)
qe k2 qe qe
where qe and qt are MB adsorption capacity at equilibrium and at any time, respectively (mg/g);
T (min) is the adsorption time. k1 (min−1 ) is the rate constant of pseudo first-order reaction.
k2 (g/(mg·min)) is the rate constant of quasi second-order reaction.
The corresponding parameters of pseudo first-order dynamics and pseudo second-
order dynamics models are calculated from the curves of ln(qe − qt ) and t and (t/qt ) and
t, respectively. It can be seen from Figure 6a that the adsorption rate of MoS2 adsorbent
increases rapidly within 0~3 min because the adsorption site is not occupied; in the stage of
3~25 min, the adsorption rate of MoS2 adsorbent gradually slows down; after 25 min, the
MoS2 adsorbent gradually reaches equilibrium. Therefore, when the initial concentration of
MB is 5 mg/L, the volume is 200 mL, and MoS2 is 20 mg, the adsorption equilibrium time
of MoS2 is 25 min. Figure 7b shows the spectrum of UV–Vis measuring the absorbance of
MB adsorbed by MoS2 adsorbent with time. It can be seen from Table 4 that the linear corre-
lation coefficient of pseudo second-order kinetics R2 = 0.995 is greater than that of pseudo
first-order kinetics R2 = 0.974, indicating that the adsorption process follows the pseudo
second-order kinetic model, and the adsorption process is mainly electrostatic adsorption.
The maximum adsorption capacity qe calculated by fitting the pseudo second-order ki-
netic model is 47.619 mg/g, which is close to the experimental value of qe = 43.385 mg/g
measured when the initial MB concentration is 5 mg/L.

Sustainability 2022, 14, 7585
time of MoS2 is 25 min. Figure 7b shows the spectrum of UV–Vis measuring the absorb-
ance of MB adsorbed by MoS2 adsorbent with time. It can be seen from Table 4 that the
linear correlation coefficient of pseudo second-order kinetics R2 = 0.995 is greater than that
of pseudo first-order kinetics R2 = 0.974, indicating that the adsorption process follows the
pseudo second-order kinetic model, and the adsorption process is mainly electrostatic ad-
sorption. The maximum adsorption capacity qe calculated by fitting the pseudo second- 8 of 12
order kinetic model is 47.619 mg/g, which is close to the experimental value of q e = 43.385
mg/g measured when the initial MB concentration is 5 mg/L.

45
(a)
40

35
qt(mg/g)

30

25

20

15
0 5 10 15 20 25 30 35 40
t(min)

Figure 7. (a) The adsorption capacity of MoS2 to MB solution in different time periods; (b) UV
absorption spectrum of MB solution concentration change; (c) and (d) linear fitting diagrams of
pseudo first-order and second-order kinetic equations, respectively.

Table 4. The pseudo first- and second-order kinetic parameters of MB adsorbed by MoS2 .

Kinetics Model Pseudo First-Order Pseudo Second-Order

k1 /min−1 qe /mg·g−1 R2 k2 /g·(mg·min)−1 qe /mg·g−1 R2
0.126 25.084 0.974 0.011 47.619 0.995

3.5. Effect of pH on MB Adsorption

The pH value of the solution is an important factor affecting the adsorption effect [34].
In this paper, the pH range of the solution is adjusted to 3–12 with a certain concentration of
concentrated sulfuric acid and sodium hydroxide. It can be seen from Figure 8 that different
pH values have little effect on the adsorption effect. The adsorption rate of MoS2 on MB can
be maintained at more than 93.47%, indicating that the adsorbent has a wide pH adsorption
range. In the local pH range (3–5), the removal rate of MB solution by MoS2 adsorbent
decreased slightly. This is because the surface of MoS2 adsorbent has anionic charge, and
MB belongs to cationic dye. Therefore, in the strong acid environment, the strong acid may
change the charge distribution on the sample surface and affect its adsorption effect [35].

Sustainability 2022, 14, 7585
Sustainability 2022, 14, x FOR PEER REVIEW
MoS2 on MB can be maintained at more than 93.47%, indicating that the adsorbent has a
wide pH adsorption range. In the local pH range (3–5), the removal rate of MB solution
by MoS2 adsorbent decreased slightly. This is because the surface of MoS2 adsorbent has
anionic charge, and MB belongs to cationic dye. Therefore, in the strong acid environment,
the strong acid may change the charge distribution on the sample surface and affect 9 ofits
12
adsorption effect [35].
Figure 8. Effect of pH on adsorption of MB solution by MoS22 adsorbent.
3.6. Effect of Recycling of MoS2 -1 on Adsorption
3.6. Effect of Recycling of MoS2-1 on Adsorption
The regeneration and recycling performance of adsorbent is also an important index to
The regeneration and recycling performance of adsorbent is also an important index
evaluate the function of adsorbent [35]. Therefore, it is necessary to study the regeneration
to evaluate the function of adsorbent [35]. Therefore, it is necessary to study the regener-
and cycle performance of MoS2 . In alkaline solution, OH- easily competes with the active
ation and cycle performance of MoS2. In alkaline solution, OH- easily competes with the
adsorption site on the surface of MoS2 to desorb cationic dyes [36]. In this paper, 0.05 mol/L
active adsorption site on the surface of MoS 2 to desorb cationic dyes [36]. In this paper,
NaOH solution was used as the elution solution to treat the adsorption material [37].
0.05 mol/L NaOH solution was used as the elution solution to treat the adsorption10mate-
of 13
In Figure 9, the removal efficiency of MB by MoS2 for the first time is 99.5%, and the
rial [37]. In Figure 9, the removal efficiency of MB by MoS2 for the first time is 99.5%, and
removal efficiency of MB by MoS2 after five cycles is still 89.34%, which indicates that MoS2
the removal
adsorbent efficiency
has of MB by MoS
good regeneration after five performance.
and2recycling cycles is still 89.34%, which indicates that
MoS2 adsorbent has good regeneration and recycling performance.
9. Effect
Figure 9.
Figure Effect of
of recycling
recyclingon
onMB
MBadsorption.
adsorption.
3.7. Adsorption Mechanism
3.7. Adsorption Mechanism
The MoS2 adsorbent before and after adsorption was analyzed by FT-IR spectrum.
The MoS2 adsorbent before and after adsorption was analyzed by FT-IR spectrum.
As shown in Figure 10, the strong peak around 590 −1cm−1 is the characteristic tensile
As shown in Figure 10, the strong peak around 590 cm is the characteristic tensile vibra-
vibration peak of Mo-S [38,39]. The C-H vibration in the plane is the main reason for the
tion peak of Mo-S [38,39]. The C-H vibration in the−1plane is the main reason for the occur-
occurrence of new characteristic peaks at 792 cm . The peak at 901 cm−1 is caused by
rence of new characteristic peaks at 792 cm−1. The peak at 901 cm−1 is caused by C-O vibra-
C-O vibration. Partial oxidation of MoS2 after contact with air causes an absorption peak
tion. Partial oxidation of MoS2 after contact with air causes an absorption peak at 1009
at 1009 cm−1 [40]. The displacement of the absorption peak at−11125 cm−1 is caused by the
cm−1 [40]. The displacement of the absorption peak at 1125 cm is caused by the vibrational
vibrational stretching of the C-O. The peak of 1380 cm−1 is S=O peak, which is also the
stretching of the C-O. The peak of 1380 cm −1 is S=O peak, which is also the representative
representative peak of MoS2 [41]. The peak at 1600 cm−1 is caused by O-H tensile vibration
peak of MoS2 [41]. The peak at 1600 cm−1 is caused by O-H tensile vibration and bending
vibration caused by partial oxidation of MoS 2 after contact with adsorbed water [42,43].
In addition, it can be clearly seen that the peak at 3410 cm−1 after adsorption is enhanced,
which indicates that more O-H groups appear on the surface of MoS2 [44].
 As shown in Figure 10, the strong peak around 590 cm−1 is the characteristic tensile vibra-
tion peak of Mo-S [38,39]. The C-H vibration in the plane is the main reason for the occur-
rence of new characteristic peaks at 792 cm−1. The peak at 901 cm−1 is caused by C-O vibra-
tion. Partial oxidation of MoS2 after contact with air causes an absorption peak at 1009
Sustainability 2022, 14, 7585 cm−1 [40]. The displacement of the absorption peak at 1125 cm−1 is caused by the vibrational
10 of 12
stretching of the C-O. The peak of 1380 cm−1 is S=O peak, which is also the representative
peak of MoS2 [41]. The peak at 1600 cm−1 is caused by O-H tensile vibration and bending
vibration
and bendingcaused by partial
vibration oxidation
caused of MoS
by partial 2 after contact with adsorbed water [42,43].
oxidation of MoS2 after contact with adsorbed
In addition, it can be clearly seen that the peak at 3410
water [42,43]. In addition, it can be clearly seen that cm−1at
the peak after
3410adsorption
cm−1 afterisadsorption
enhanced,
which indicates that more O-H groups appear on the surface of MoS 2 [44].
is enhanced, which indicates that more O-H groups appear on the surface of MoS [44]. 2

Figure 10.FTIR
Figure10. FTIRspectra
spectraof
ofMoS
MoS22-1
-1before
beforeand
andafter
afteradsorption.
adsorption.

4.3.8.
Conclusions
Figures, Tables and Schemes
The three-dimensional
All figures nano flower-shaped
and tables should MoS2text
be cited in the main adsorbent was
as Figure synthesized
1, Table 1, etc. by a
simple, one-step hydrothermal method. When the hydrothermal time was 1 h, the prepared
MoS 2 -1 adsorbent had good adsorption for cationic dye MB. According to the analysis
4. Conclusions
of adsorption isotherm model, Langmuir isothermal adsorption model can better fit the
adsorption data. The results show that the maximum adsorption capacity of MoS2 nano
adsorbent is 200 mg/g, which belongs to uniform monolayer adsorption. The adsorption
kinetic process of MoS2 on MB follows the pseudo second-order kinetic model, which
shows that the adsorption process is mainly electrostatic adsorption. pH value has little
effect on the removal rate of MB and can maintain the removal rate of more than 93.47%,
indicating that the adsorbent can maintain high adsorption performance in a wide pH range.
In addition, the adsorbent has good recoverability, regeneration, and recycling performance
and has application potential. The treatment object of this paper is simulated printing and
dyeing wastewater, and the research results are expected to provide a theoretical basis for
the practical application of practical printing and dyeing wastewater treatment.

Author Contributions: Data curation, P.Z. and F.X.; Methodology, G.H. and L.B.; Validation, B.S.; Writing—
original draft, X.W. All authors have read and agreed to the published version of the manuscript.
Funding: This research was funded by the Project of National Key Research and Development Pro-
gram (2019YFC0408505), the Science and Technology Major projects of Anhui Province (18030801106),
the Natural Science Foundation of Anhui Province (No. 1908085QE241), the Natural Science Research
Project of the Higher Education Institutions of Anhui Province (KJ2021A0616, KJ2020A0468), the Na-
tional Natural Science Foundation of China (52103104, 61873003), the Key Research and Development
Plan of Anhui Province (201904a07020070), the first batch of natural science projects supported by
surplus funds in 2021 of Anhui Jianzhu University (JZ202129, JZ202134), and the Scientific Research
Start-up Foundation for Introduction of Talent, Anhui Jianzhu University (2016QD113).
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 no conflict of interest.
Sustainability 2022, 14, 7585 11 of 12

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