Chemosphere 254 (2020) 126827

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Chemosphere
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Ultrasound-assisted Ti3C2Tx MXene adsorption of dyes: Removal

performance and mechanism analyses via dynamic light scattering
Byung-Moon Jun a, Sewoon Kim a, Hojung Rho b, Chang Min Park c, *, Yeomin Yoon a, **
a
Department of Civil and Environmental Engineering, University of South Carolina, Columbia, 300 Main Street, SC, 29208, USA
b
Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment, School of Sustainable Engineering and the Built Environment,
Arizona State University, Tempe, AZ, 85287, USA
c
Department of Environmental Engineering, Kyungpook National University, 80 Daehak-ro, Buk-gu, Daegu, 41566, Republic of Korea

h i g h l i g h t s g r a p h i c a l a b s t r a c t

Ultrasonication -assisted novel

nanomaterial Ti3C2Tx was utilized as
an adsorbent.

Ultrasonication enhanced the
dispersion of MXene at different
frequencies.

Ultrasonication-assisted Ti3C2Tx
MXene enhanced dye adsorption.

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

Article history: Herein, ultrasonication (US)-assisted novel nanomaterial Ti3C2Tx MXene was utilized as a selective
Received 23 February 2020 adsorbent for treatment of synthetic dyes in model wastewater. Two types of US frequencies, 28 and
Received in revised form 580 kHz, were applied to disperse MXene to evaluate the feasibility of US-assisted MXene for wastewater
14 April 2020
treatment. The physico-chemical properties of MXene after US were characterized by Fourier-transform
Accepted 15 April 2020
infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and zeta potential. According to
Available online 25 April 2020
FTIR and XPS, 28 kHz US-assisted MXene had a greater amount of oxygenated functional groups and
Handling Editor: Shane Snyder dispersion compared to 580 kHz US-assisted and pristine MXene. Subsequently, US-assisted MXene was
utilized as an adsorbent for the removal of positively charged methylene blue (MB) and negatively
Keywords: charged methyl orange. Both 28 and 580 kHz US-assisted MXene showed better adsorption performance
Ultrasound-assisted adsorption for only MB compared to stirring-assisted MXene based on kinetics, isotherms, and several water
Dyes chemistry factors including solution pH, temperature, ionic strength, and humic acid. Advantages of US-
MXene assisted MXene for water treatment are its fast kinetics at low dose and high selectivity for positively
Dynamic light scattering
charged target compounds (i.e., MB). The main adsorption mechanism between MXene and MB was
electrostatic interaction (attraction); however, physical properties (i.e., aggregation kinetics and hydro-
dynamic diameter), measured via dynamic light scattering, were also found to be critical factors in
controlling the adsorption performance of the system. Lastly, US-assisted MXene exhibited a high
regeneration property, based on 4th adsorption-desorption cycles.
© 2020 Elsevier Ltd. All rights reserved.

* Corresponding author.
** Corresponding author.
E-mail addresses: cmpark@knu.ac.kr (C.M. Park), yoony@cec.sc.edu (Y. Yoon).

https://doi.org/10.1016/j.chemosphere.2020.126827
0045-6535/© 2020 Elsevier Ltd. All rights reserved.
2 B.-M. Jun et al. / Chemosphere 254 (2020) 126827
1. Introduction
Treatment of wastewater containing recalcitrant organic con-
taminants has attracted critical environmental concerns as these
compounds have been detected in several water sources (e.g.,
surface water) (Joseph et al., 2019). This type of water pollution is
mainly caused by irregular discharge of wastewater (Jun et al.,
2019a). Particularly, colored wastewater containing synthetic dyes
could cause the following severe environmental issues (Oveisi et al.,
2018; Han et al., 2019a): (i) inhibition of aquatic organism photo-
synthesis due to blocked sunlight (ii) negative impacts (e.g., carci-
nogenicity), on lifeforms living in contaminated water sources, and
(iii) disruption of aquatic systems due to a lack of dissolved oxygen.
Thus, effective ways for treating wastewater containing synthetic
dyes is an important topic from an environmental perspective.
The textile industry commonly uses methylene blue (MB), a
heterocyclic compound (Mashkoor and Nasar, 2020). Over the last
several decades, various physical, chemical, and biological pro-
cesses have been applied to the treatment of wastewater containing
synthetic dyes. Physical techniques have been conducted using
membranes, sedimentation, coagulation, adsorption, and floccula-
tion (Mashkoor and Nasar, 2020). Chemical techniques have been
performed using ultrasonication (US), photocatalysis, Fenton
oxidation, and ozonation (Katheresan et al., 2018). Biological
techniques have been carried out via aerobic and anaerobic pro-
cesses depending on the composition of the wastewater (Kong
et al., 2019). The most efficient method for removal of synthetic
dyes from wastewater has been adsorption since it has low cost, fast
kinetics, simple operation, and less toxic byproducts (Han et al.,
2019b; Jun et al., 2020a).
Based on the principles of adsorption, use of proper adsorbents,
dependent on target compounds, is a significant factor in deter-
mining adsorption performance (Hasan and Jhung, 2015). Recently,
MXene-based nanomaterials have attracted attention in environ-
mental applications. MXene is a new family of 2D-based nano-
materials comprised of transition metals which are similar in
structure to graphene (Sun et al., 2018; Jun et al., 2019b). These
nanomaterials are generally fabricated by chemical etching (Jun
et al., 2020b), where removal of the ‘A’ layer from the ‘MAX’
phase (where ‘M’ is a transition metal, ‘A’ is a IIIA or IVA element of
the periodic table, and ‘X’ is carbon/nitrogen) is a general route to
obtain MXene (Jun et al., 2020b). MXene could be utilized as an
efficient adsorbent for treating organic/inorganic contaminants due
to its high theoretical surface area, hydrophilicity, unique structure,
chemical stability, and tunable chemistry (Jun et al., 2019b). Based
on these physico-chemical properties, recent publications on
MXene-based nanomaterials used as efficient adsorbents in the
removal of synthetic dyes, heavy metals, and radionuclides have
been reported (Shahzad et al., 2017, 2018; Gu et al., 2018; Dong
et al., 2019; Jun et al., 2020c, 2020d, 2020e).
One of the critical issues associated with nanomaterials in
wastewater treatment applications is known as aggregation phe-
nomenon, which results in decreased treatment performances
(Park et al., 2017). Recently, US has been utilized as an accelerating
agent for wastewater treatment (Oveisi et al., 2018). Dispersion of
nanomaterials could be achieved by US, which produces cavitation
bubbles, followed by shock waves and shear forces when they
collapsed in the bulk liquid phase (Jun et al., 2019c). Thus, US-
assisted methods could be applied to wastewater treatment
adsorption processes due to their capability for faster kinetics with
a lower amount of adsorbent, making them more cost-effective
(Oveisi et al., 2018). To the best of our knowledge, there are no
systematic investigations on the removal of synthetic dyes using
US-assisted MXene in terms of useful water chemistry conditions
and adsorption mechanism clarified by aggregation kinetics.
The main purposes of this study are to: (i) evaluate the removal
rate of positively charged methylene blue (MB) and negatively
charged methyl orange (MO) under different doses of MXene (ii)
deeply study the effects of US frequencies (i.e., 28 and 580 kHz), on
the removal of MB by MXene in terms of several water chemistry
properties (i.e., ionic strength and humic acid), and (iii) investigate
the aggregation kinetics of MXene for the removal of MB via dy-
namic light scattering (DLS). Furthermore, we investigate the ki-
netic, isotherm, and regeneration properties of the removal of MB
by MXene in detail.
2. Materials and methods
2.1. Chemicals
MXene (Ti3C2Tx) adsorbent was purchased from Advanced
Materials Development Expert Store (Hangzhou, Zhejiang, China).
Humic acid (HA), hydrochloric acid (HCl), sodium chloride (NaCl),
sodium hydroxide (NaOH), MB (C16H18ClN3S), and MO
(C14H14N3NaO3S) were obtained from Sigma-Aldrich (St. Louis, MO,
USA). The physicochemical properties of the target dyes are sum-
marized in Table S1. All chemicals were used without further pu-
rification. Nanopure deionized (DI) water was used in all feed and
stock solutions.
2.2. Characterization of adsorbents
Dispersion of MXene was conducted using the US reactor
method referenced in a previous study (Park et al., 2017). The US
power and dispersion time were 160 W and 30 min, respectively.
Surface morphology was observed by scanning electron micro-
scopy (SEM) and transmission electron microscopy (TEM) accord-
ing to a previous study (Jun et al., 2019d). Analyses of chemical
bonds and compositions were carried out using Fourier-transform
infrared spectroscopy (FTIR) and X-ray photoelectron spectros-
copy (XPS) methods, respectively, referenced from a previous study
(Jun et al., 2019e). Surface charge was measured using a zeta po-
tential analyzer (Zetapals; Brookhaven Instruments, Holtsville, NY)
from pH 4 to 10 adjusted with 0.1 M HCl and NaOH solutions (Jun
et al., 2019f). Lastly, according to a previous study (Park et al.,
2017), we measured the aggregation kinetics of MXene at 28 and
580 kHz US using DLS to clarify the adsorption mechanism of a
synthetic cationic dye (i.e., MB) by MXene.
2.3. Procedure of adsorption and desorption experiments
Basic conditions for the adsorption experiments involved 40 mL
total volume solutions containing 5 mg L1 MB and 20 mg L1
MXene in 50 mL Falcon tubes. Specific experiments were conducted
using: (i) doses of MXene of 10, 20, 33.3, and 50 mg L1; (ii) contact
times from 0 to 480 min; (iii) initial concentrations of MB of 2, 5, 10,
15, and 20 mg L1; (iv) solution pH values of 4, 7, and 10; (v) so-
lution temperatures of 293, 303, and 313 K; (vi) background ion
compositions of 10 and 50 mM NaCl; and (vii) 1 and 5 mg L1
concentrations of HA. Samples were filtered through 0.2 mm
membrane filters (Millipore, Cork, Ireland) after each contact time
listed to obtain the concentrations of the synthetic dyes. The con-
centrations of the synthetic dyes were calculated using a UVeVis
spectrophotometer (Agilent Technologies, Santa Clara, CA). The
concentrations of MB and MO were calculated using their
maximum adsorption wavelengths (Fig. S1). The maximum
adsorption wavelengths of MB and MO were 664 and 464 nm,
respectively. We referenced a previous report to conduct the
adsorption-desorption experiments (Zou et al., 2016; Shahzad et al.,
2018). These experiments were performed over four cycles to
 B.-M. Jun et al. / Chemosphere 254 (2020) 126827
evaluate regeneration properties based on adsorption performance.
Adsorption performance was determined based on removal rate
and equilibrium adsorption capacity. The removal rates of the
synthetic dyes by MXene were calculated using Eq. (1):
ðC0  Ce Þ
R¼  100%
C0
where, C0 (mg L1) and Ce (mg L1) are the initial and equilibrium
concentrations of the synthetic dyes in the sample, respectively.
The adsorption capacity (qt, mg g1) and equilibrium adsorption
capacities (qe, mg g1) of MXene to remove the synthetic dyes were
calculated using Eqs. (2) and (3), respectively:
ðC0  Ct ÞV
qt ¼
m Microscopic analyses were performed to observe the surface
ðC0  Ce ÞV
qe ¼
m MXene are shown in Figs. S2 (b), (c), and (d), respectively. The
where, Ct (mg L1) is the concentration of dye at the contact time, m
(g) is the dose of MXene, and V (L) is the volume of the sample
solution containing both MXene and the synthetic dyes. Eqs. (2)
and (3) were also used to analyze the kinetic and isotherm prop-
erties of the samples using intra-particle diffusion, Elovich, pseudo-
first, and second order kinetic models, with Langmuir and
Freundlich equations used as isotherm models.
Fig. 1. Characterizations of (1) pristine MXene, (2) sonicated MXene at 28 kHz, and (3) sonicated MXene at 580 kHz using (a) FTIR, (b) XPS, and (c) zeta potential.
3
3. Results and discussion
3.1. Characterization
Dispersion of nanomaterials by US is dependent on US fre-
quency, which results in different cavitation phenomena in bulk
liquid phase (Chang et al., 2008). That is, the sizes of cavitation
(1)
bubbles generated by lower US frequencies are relatively larger
than those of higher US frequencies, which release larger shock
waves and shear forces when cavitation bubbles collapse in bulk
liquid phase (Chu et al., 2017). Thus, irregular regions of nano-
materials could be oxidized by US, and the amounts of oxidation
could be varied based on US frequency, followed by additional
formation of oxygenated functional groups (e.g., eOH and eCOOH)
on the nanomaterial surface (Park et al., 2017). The effects of US on
the physico-chemical properties of MXene were investigated by
(2) TEM, FTIR, XPS, and zeta potential.
morphology of MXene, with representative SEM and TEM images of
pristine MXene shown in Fig. S2 (a, inset) and (a), respectively.
Subsequently, stirring-, 28 kHz US-, and 580 kHz US-assisted
(3)
degree of aggregation of MXene was observed in the following
order: stirring-assisted > 580 kHz US-assisted > 28 kHz US-
assisted. This result evidently showed that US was effective for
dispersing MXene, which might be more effective in adsorption
process applications. In addition, the 28 kHz US frequency was
more effective than the 580 kHz US frequency due to the presence
of larger shock waves and shear forces. This outcome is in good
4 B.-M. Jun et al. / Chemosphere 254 (2020) 126827
Fig. 2. Effect of stirring-assisted MXene dose on the removal rate and qe of dyes using
(a) single and (b) binary system (experimental conditions: pH 7, 5 mg L1 dyes, and
293 K).
agreement with the results of single-walled carbon nanotubes
(SWCNTs) (Park et al., 2017).
Fig. 1 (a1, 2, and 3) show information on the chemical bonds of
pristine, 28 kHz US-assisted, and 580 kHz US-assisted MXene via
FTIR. All samples contain ~3480, ~1630, and ~655 cm1 peaks,
indicating eOH, eCOOH, and TieO functional groups, respectively
(Peng et al., 2014; Park et al., 2017). According to the FTIR peaks, US-
assisted MXene had more eOH and eCOOH groups than pristine
MXene, while maintaining the same TieO functionality. This result
was quantitatively supported by XPS, Fig. 1 (b), based on oxygen
content. Subsequently, the measured slight increases in negative
surface charge with increasing solution pH for US-assisted MXene
could be attributed to more eOH and eCOOH groups on the surface
after US (Fig. 1 (c)). Thus, both XPS and zeta potential results clearly
support the FTIR results.
3.2. Effects of adsorbent dose and single/binary systems on dye
removal
Adsorption performance is generally attributed to adsorbent
dose. Fig. 2 shows the adsorption performances of MO and MB with
increasing doses of MXene, from 10 to 50 g L1. Removal rates and
qe values for MB increased and decreased, respectively, when the
MXene dose was increased. We also investigated the effects of
single and binary systems on the removal of MO and MB, Fig. 2(a)
and (b), respectively. In both cases, opposite trends between
removal rates and qe values were observed, which could be
attributed to active adsorption sites on the surface of the adsorbent
based on the fact that the degree of active adsorption sites is
dependent on the amount of both adsorbent and adsorbate (Wang
et al., 2017). Particularly, compared to the MO results, regardless of
the system, MB was effectively removed by MXene. These results
clearly support that the main adsorption mechanism between the
synthetic dyes and MXene was electrostatic interaction due to both
MO and MXene having negative surface charges at neutral pH
(Pargoletti et al., 2019). High selectivity for the removal of positively
charged MB by MXene can be regarded as an excellent property
when MXene is utilized as an adsorbent in wastewater treatment
Fig. 2 (b). Therefore, MB was chosen as a representative target
compound for further experiments based on its high adsorption
performance.
3.3. Dye removal comparison between US and stirring-assisted
adsorption
3.3.1. Kinetics and isotherms study
Fig. 3 (a) shows the adsorption kinetics for stirring- and US-
assisted MXene, with MXene achieving a nearly saturated
removal rate within 30 min, providing another excellent property
of MXene. Adsorption performances were observed in the
following order: 28 kHz US-assisted > 580 kHz US-
assisted > stirring-assisted. This trend was clarified through ag-
gregation kinetics (Fig. 3 (b)). DLS results indicated that US signif-
icantly contributed to the dispersion of MXene, with aggregation
kinetics in DI water obtained over 30 min. The hydrodynamic
diameter (Dh) order was dependent on dispersion method and was
inversely proportional to adsorption performance; therefore, US-
assisted MXene showed better mass transfer for the adsorption of
MB (Oveisi et al., 2018). The stability of aggregation kinetics was
higher when MXene was treated using US compared to stirring, and
this phenomenon can be explained by the increased negative sur-
face charge preventing aggregation (Fig. 1 (c)). In order to investi-
gate the adsorption kinetics for the removal of MB by MXene, we
applied intra-particle diffusion, Elovich, pseudo-first order, and
pseudo-second order kinetic models (Jun et al., 2019f). Fig. 3 (c)e(f)
and Table S2 summarize the kinetic parameters of MB adsorption
using stirring- and US-assisted MXene. Stirring- and US-assisted
MXene were well-fitted by the pseudo-second order kinetic
model, having the highest correlation coefficients (R2).
Fig. 4 (a) shows the effects of the initial concentration of MB on
the adsorption performance of MXene. The trend in adsorption
performance was the same as that in the kinetic study, and removal
of MB by US-assisted MXene was much greater than that by
stirring-assisted MXene. This phenomenon could be the result of
increased oxygenated functional groups (Fig. 1) as well as lower
aggregation kinetics [Fig. 3 (b)], as mentioned earlier. Meanwhile,
an opposite trend was confirmed between removal rates and qe
values with increasing MB concentration. This phenomenon is
similar to that described in the dose experiment (Section 3.2).
Subsequently, we applied Langmuir and Freundlich models to
clarify the adsorption isotherms (Jun et al., 2019f). The Langmuir
and Freundlich models indicated that surface adsorption followed
monolayer and multilayer adsorption isotherms for adsorbates and
adsorbents, respectively. Fig. 4(b) and (c) conclude that the removal
of MB by MXene well fits a Freundlich model, regardless of US.
Similar results were also confirmed in previous reports (Fard et al.,
2017; Li et al., 2019).
3.3.2. Solution pH and temperature
Surface charge is attributed to solution pH, and it is an important
parameter when an adsorption mechanism is the result of elec-
trostatic interaction. Fig. S3 shows the effects of solution pH on the
removal rates and qe values of stirring- and US-assisted MXene.
Adsorption performance improved as solution pH increased, which
 B.-M. Jun et al. / Chemosphere 254 (2020) 126827 5

Fig. 3. (a) Adsorption and (b) aggregation kinetics of stirring-assisted and US-assisted MXenes (experimental conditions: pH 7, 5 mg L1 MB, 20 mg L1 MXene, and 293 K). Fitting
lines of kinetic studies through (c) intra-particle diffusion, (d) Elovich, (e) pseudo-first order, and (f) pseudo-second order kinetic model.

could be explained by increased negative surface charge [Fig. 1 (c)].
The order of adsorption performance was dependent on dispersion
method and equal to that of the kinetic and isotherm studies;
therefore, both physical properties (i.e., aggregation kinetics and
Dh) and surface charge are critical factors in controlling adsorption
performance in this system.
Solution temperature is also a significant factor affecting
adsorption performance. Increasing the solution temperature could
increase the diffusion rate and number of active sites, improving
adsorption performance (Mirsoleimani-azizi et al., 2018). However,
desorption of adsorbates from adsorbents could also be favorable
due to an increase in vibrational energy induced by solution tem-
perature increase (Qu et al., 2009). Thus, there exists an optimal
solution temperature dependent on both adsorbate and adsorbent.
Fig. S4 shows the effects of solution temperature on the adsorption
performance of stirring- and US-assisted MXene. Adsorption per-
formance increased with increasing solution temperature in both
cases. This outcome could be predominantly the result of the
positive influence of solution temperature on adsorption perfor-
mance. Based on a previous study, we obtained thermodynamic
parameters, including dG0 dH 0 , and dS0 (Jun et al., 2019f). Table S3
summarizes the thermodynamic parameters of the adsorption of
6 B.-M. Jun et al. / Chemosphere 254 (2020) 126827
Fig. 4. (a) Effect of initial MB concentration on removal rate and qe by stirring-assisted
and US-assisted MXenes (experimental conditions: pH 7, 20 mg L1 MXene, and
293 K). Fitting lines of isotherm studies through (b) Langmuir and (c) Freundlich
model.
MB by stirring- and US-assisted MXene. Adsorption of MB by
MXene was a spontaneous, endothermic, increasingly random
process judging from the negative dG0 , positive dH 0 , and positive
dS0 values, respectively.
3.3.3. Background ion and humic acid
Both ionic strength and natural organic matter (NOM) are
practical factors in the field of water treatment, so we chose NaCl
and HA as the representative model compounds, referred from
previous studies (Park et al., 2017; Mirsoleimani-azizi et al., 2018;
Shahzad et al., 2018). Fig. 5 (a) summarized effect of background ion
(i.e., NaCl) and HA on adsorption performances by stirring-assisted
and US-assisted MXenes. In terms of ionic strength, adsorption
performances continuously decreased as NaCl concentration
increased. Decreased adsorption performances could be attributed
to the following explanations: (i) electrical double layer is attrib-
uted to ionic strength, so abundant ions might cause screening
effect on both MB and MXene, followed by decreasing electrostatic
interactions (attraction) between them (Wong et al., 2016), and (ii)
fast aggregation kinetics of MXene happens with increasing ionic
strength (Seo et al., 2016), and DLS results evidently supported fast
aggregation kinetics in the presence of abundant NaCl [Fig. 5 (b)].
That is, average Dh of stirring, 28 kHz US, and 580 kHz US-assisted
MXene in DI water/NaCl 50 mM was 610/845, 377/434, and 489/
582 nm, respectively.
Meanwhile, adsorption performances obviously increased as HA
concentration increased in terms of NOM [Fig. 5 (a)]. HA is repre-
sentative NOM which consists of aromatic rings and carboxylic
acids (Bhatnagar and Sillanpa €€a, 2017), and average Dh of stirring,
28 kHz US, and 580 kHz US-assisted MXene in DI water/HA 5 ppm
was 610/435, 377/298, and 489/342 nm, respectively. Thus, HA
played a role as inhibition of aggregation, based on the decreased
average Dh of MXene in the presence of HA, as shown in Fig. 5 (c).
This inhibition effect of HA is in good agreement with another
study assessed by SWCNTs (Park et al., 2017). When the solution
contains both NaCl 50 mM and HA 5 ppm, adsorption performances
exhibited between sole existence of NaCl and HA in the solution. In
particular, in terms of aggregation kinetics, inhibition effect of HA
was much higher than screening effect of ionic strength, resulting
to slightly increase of average Dh of MXene [Fig. 5 (d)]. This
conclusion is clearly reflected on adsorption performances, as
shown in Fig. 5 (a). Considering results of aggregation kinetics
depending on dispersion method of MXene, physical property was
significant parameter to determine the adsorption performances in
this system, even though adsorption mechanism between MXene
and adsorbates are mainly clarified by electrostatic interactions
(Shahzad et al., 2017; Gu et al., 2018; Shahzad et al., 2018; Li et al.,
2019; Jun et al., 2020b).
3.4. Regeneration property
Regeneration property is an essential factor for material utili-
zation in wastewater treatment applications from a practical
standpoint. Thus, we conducted four cycles of adsorption-
desorption processes and evaluated the regeneration property of
MXene based on its adsorption performance (Fig. 6). The adsorp-
tion performance of MB by US-assisted MXene was greater than
that of stirring-assisted MXene until the 4th regeneration cycle.
However, a slight decrease in adsorption performance was
confirmed, which could be the result of incomplete collection of
used MXene during the recovery stage. US-assisted MXene could be
utilized as an efficient route for treating positively charged com-
pounds (e.g., MB) in wastewater due to its high adsorption per-
formance and regeneration property.
4. Conclusions
In this study, 2D-based nanomaterial Ti3C2Tx MXene was uti-
lized as a selective adsorbent to treat model wastewater containing
synthetic dyes. We applied 28 and 580 kHz US frequencies to
disperse MXene to investigate the feasibility of US-assisted MXene
in wastewater treatment processing. According to FTIR and DLS
characterizations, US-assisted MXene had a greater amount of
oxygenated functional groups and dispersion compared to pristine
MXene due to shock waves and shear forces induced by the collapse
of cavitation bubbles in bulk liquid phase. Subsequently, US-
assisted MXene exhibited a better adsorption capacity compared
 B.-M. Jun et al. / Chemosphere 254 (2020) 126827 7

Fig. 5. (a) Effect of background ion and HA on removal rate and qe by stirring-assisted and US-assisted MXenes (experimental conditions: pH 7, 5 mg L1 MB, 20 mg L1 MXene, and
293 K). Aggregation kinetics of stirring-assisted and US-assisted MXenes in the presence of (b) NaCl 50 mM, (c) HA 5 ppm, and (d) NaCl 50 mM and HA 5 ppm.

kinetics, and high regeneration property.

Declaration of competing interest

The authors declare that they have no known competing

financial interests or personal relationships that could have
appeared to influence the work reported in this paper.

CRediT authorship contribution statement

Byung-Moon Jun: Funding acquisition, Writing - original draft.

Sewoon Kim: Funding acquisition. Hojung Rho: Funding acquisi-
tion. Chang Min Park: Methodology, Supervision. Yeomin Yoon:
Methodology, Supervision.

Acknowledgements
Fig. 6. Re-usability of US-assisted MXenes for removal of MB in four cycles (experi-
mental conditions: pH 7, 5 mg L1 MB, 50 mg L1 MXene, and 293 K).
This research was also supported by the Korea Ministry of
Environment, ‘The SEM projects; 2018002470005, South Korea’.
to stirring-assisted MXene based on kinetics, isotherms, and several This research was also supported by Basic Science Research Pro-
water chemistry factors, including solution pH, temperature, gram through the National Research Foundation of Korea (NRF)
background ions, and NOM. Regardless of US, MXene followed funded by the Ministry of Education (NRF-
pseudo-second order kinetic and Freundlich isotherm models. 2017R1D1A1B04033506).
Thermodynamic studies showed the adsorption between MB and
MXene was a spontaneous, endothermic, and increasingly random
Appendix A. Supplementary data
process. US-assisted MXene could be applied as an efficient method
for treating wastewater based on its high selectivity for positively
Supplementary data to this article can be found online at
charged compounds (e.g., MB), high adsorption performance, fast
https://doi.org/10.1016/j.chemosphere.2020.126827.
8 B.-M. Jun et al. / Chemosphere 254 (2020) 126827

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