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Universal Ligands for Dispersion of Two-

Dimensional MXene in Organic Solvents
Tae Yun Ko, Daesin Kim, Seon Joon Kim, Hyerim Kim, Arun S. Nissimagoudar, Seung-Cheol Lee,
Xiaobo Lin, Peter T. Cummings, Sehyun Doo, Seongmin Park, Tufail Hassan, Taegon Oh, Ari Chae,
Jihoon Lee, Yury Gogotsi,* Insik In,* and Chong Min Koo*
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ABSTRACT: Ligands can control the surface chemistry,

physicochemical properties, processing, and applications of
nanomaterials. MXenes are the fastest growing family of two-
dimensional (2D) nanomaterials, showing promise for energy,
electronic, and environmental applications. However, complex
oxidation states, surface terminal groups, and interaction with
the environment have hindered the development of organic
ligands suitable for MXenes. Here, we demonstrate a simple,
fast, scalable, and universally applicable ligand chemistry for
MXenes using alkylated 3,4-dihydroxy- L -phenylalanine
(ADOPA). Due to the strong hydrogen-bonding and π-electron
interactions between the catechol head and surface terminal
groups of MXenes and the presence of a hydrophobic
fluorinated alkyl tail compatible with organic solvents, the ADOPA ligands functionalize MXene surfaces under mild
reaction conditions without sacrificing their properties. Stable colloidal solutions and highly concentrated liquid crystals of
various MXenes, including Ti2CTx, Nb2CTx, V2CTx, Mo2CTx, Ti3C2Tx, Ti3CNTx, Mo2TiC2Tx, Mo2Ti2C3Tx, and Ti4N3Tx, have
been produced in various organic solvents. Such products offer excellent electrical conductivity, improved oxidation stability,
and excellent processability, enabling applications in flexible electrodes and electromagnetic interference shielding.
KEYWORDS: two-dimensional (2D) materials, MXene, ligand chemistry, surface functionalization, organic dispersion,
electrically conductive MXene organic ink

INTRODUCTION electrical conductivity is the introduction of surface ligand

MXenes have shown outstanding performance in energy chemistry. However, complex oxidation states,18,19 surface
storage, electromagnetic interference shielding, optoelec- terminal groups,4 and interaction with the environment19 have
tronics, sensors, thermal heaters, and environmental applica- hindered the development of organic ligands suitable for
tions due to their excellent metallic conductivity, transparency, MXenes.
and outstanding solution processability in water.1−11 These The development of MXene ligand chemistry is challenging
transition-metal carbides/carbonitrides/nitrides are a family of for multiple reasons. The complex oxidation states of the
2D materials with the general formula Mn+1XnTx (n = 1−4), transition metals in MXene (e.g., Ti+, Ti2+, Ti3+, and Ti4+ for
where M, X, and Tx represent transition metal(s), carbon or Ti3C2Tx MXene) and diverse terminal groups make it difficult
nitrogen, and surface terminal groups such as −OH, −O, and to design organic ligands suitable for MXenes.18,19 The strong
−F, respectively.12,13 Despite these advantages, for excellent hydrophilicity and limited oxidation stability in aqueous media
oxidation stability, efficient processing, and composites with limit the ligand chemistry of MXenes in organic environ-
hydrophobic polymers, MXenes must break away from the
existing water dispersion system and a stable organic solvent Received: August 16, 2022
dispersion with high electrical conductivity is essential. Since Accepted: November 7, 2022
the organic ligand molecules can control the surface chemistry,
physicochemical properties, processing, and applications of
nanomaterials,14−17 the most efficient method for the develop-
ment of a stable organic dispersion of MXene with high

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Figure 1. Schematic illustration and characterization of AD1-Ti3C2Tx flakes. (a) Schematic of the surface functionalization of MXene with
ADOPA1. (b) TEM image (inset: SAED pattern) of an AD1-Ti3C2Tx flake. Scale bar: 5 1/nm in the inset. (c) F 1s (top) and N 1s (bottom)
XPS curves of ADOPA1-Ti3C2Tx. (d) Digital photographs of AD1-Ti3C2Tx, DOPA-Ti3C2Tx, polyAD1-Ti3C2Tx, and pristine Ti3C2Tx in
acetone. (e) Cross-sectional SEM images of AD1-Ti3C2Tx (top) and pristine Ti3C2Tx (bottom) films. (f) XRD curves of AD1-Ti3C2Tx and
pristine Ti3C2Tx. (g) Electrical conductivities of AD1-Ti3C2Tx, C10PA-Ti3C2Tx, and DHT-Ti3C2Tx. The C10PA and DHT organic ligands
represent decylphosphonate and di(hydrogenated tallow)benzyl methylammonium chloride, respectively. The electrical conductivity of the
C10PA-Ti3C2Tx film was measured on the sample prepared by the method in ref 22. The electrical conductivity of the DHT-Ti3C2Tx film was
sourced from the literature.24 (h) Projected electronic band structure of bulk (multi)layered Ti3C2(OH)2 with ADOPA1 adsorbed. (i) Total
contribution of projected density of states from carbon pz orbitals of the benzene ring in ADOPA1 adsorbed on Ti3C2(OH)2. The Fermi
level is set to zero (marked by a dashed line).

ments.19−21 The harsh reaction conditions required for most attracted attention as ligands for the surface functionalization
covalent and many noncovalent functionalization reactions, of nanomaterials because of their strong interaction with the
such as strong acids or bases, accelerate the oxidative hydrophilic metal oxides or strong adhesion strength even on
degradation of MXenes.22,23 Conventional functionalization hydrophobic substrates.16,17,25,26 However, there have been no
also requires long reaction times, mostly in aqueous media, reports on the functionalization of hydrophobic catechol
which may accelerate the degradation of MXenes.22−24 derivatives on MXenes to improve their dispersion stability in
Different ligand chemistries must be developed for each organic solvents, oxidation stability, or electrical conductivity.
MXene surface chemistry, depending on the M element and In this study, we developed alkylated 3,4-dihydroxy-L-
the surface termination groups of MXene. Moreover, insulative phenylalanine (ADOPA) to achieve fast functionalization of
organic ligands adsorbed on the surface strongly affect the all types of MXenes. The ADOPA ligands contain not only a
interlayer electronic transport of functionalized MXenes and hydrophilic catechol head but also a hydrophobic fluoroalkyl
drastically decrease their conductivity.22−24 tail (Figure 1a). The catechol moiety coupled with an amino
Catechol derivatives, such as dopamine and DOPA, that group forms strong noncovalent hydrogen bonds with the
undergo the polycatechol polymerization process have surface functional groups of MXene in a very short time at
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Figure 2. Dispersion and oxidation stability of AD1-Ti3C2Tx flakes in various organic solvents. Digital photographs of (a) AD1-Ti3C2Tx and
(b) pristine Ti3C2Tx dispersions at low concentrations in various organic solvents after 6 h of storage. (c) Digital photographs of nine
different MXenes after surface functionalization with ADOPA1 in ethanol. (d) UV−visible absorbance spectra of nine different AD1-MXene
dispersions in ethanol. TEM images of (e) AD1-Ti3C2Tx flakes in EtOH and (f) pristine Ti3C2Tx in water after 50 days of storage. The
oxidation of aqueous Ti3C2Tx dispersions produces TiO2 and amorphous carbon. A-TiO2 (red) and R-TiO2 (blue) indicate anatase and rutile
TiO2 crystal structures, respectively. (g) Normalized intensity of UV−visible absorbance peak at ∼760 nm for pristine Ti3C2Tx in water
(black line), AD1-Ti3C2Tx in EtOH (red line), and AD1-Ti3C2Tx in IPA (blue line) as a function of storage time. (h) Water contact angles of
AD1-Ti3C2Tx, AD4-Ti3C2Tx, and pristine Ti3C2Tx films. (i) Change in electrical conductivity of AD1-Ti3C2Tx, AD4-Ti3C2Tx, and pristine
Ti3C2Tx films under 85 °C and 85% RH test conditions for 20 days. After drying at 150 °C, the recovery of the electrical conductivity was
monitored. (j) Ti 2p XPS spectra of AD1-Ti3C2Tx and pristine Ti3C2Tx films after 85/85 testing.

room temperature and moderate pH. The hydrophobic tail element A (Al) from the corresponding parent MAX phases
improves the compatibility with various organic solvents. (Supplementary Text and Figures S5−S13). In a typical
When aqueous MXene suspensions were added to an ADOPA- surface functionalization experiment, the as-prepared aqueous
containing organic solution at room temperature, the MXene dispersion of Ti3C2Tx MXene flakes was mixed with ADOPA1
flakes were immediately functionalized and became dispersible having a 1H,1H,2H,2H-perfluoro-1-hexanol tail group in an
in organic solvents (Figure 1a, the Supplementary Text, and organic solvent at room temperature for 1 min to obtain
Videos S1 and S2). surface-functionalized AD1-Ti3C2Tx MXenes in almost 100%
yield (Figure S14). Transmission electron microscopy (TEM)
RESULTS AND DISCUSSION and atomic force microscopy (AFM) images revealed that
AD-MXene Preparation and Characterization. AD1-Ti3C2Tx retained its original delaminated single-sheet
ADOPA ligands, such as ADOPA1, ADOPA2, ADOPA3, morphology with an average size of 3.41 μm, whereas the
and ADOPA4, were synthesized by esterification of 3,4- selected area electron diffraction (SAED) pattern demon-
dihydroxy-L-phenylalanine (DOPA) with hydrophobic tails, strated its hexagonal symmetry (Figure 1b and Figures S15−
such as 1H,1H,2H,2H-perfluoro-1-hexanol, 1H,1H,2H,2H- S17).5 AD1-Ti3C2Tx exhibited two characteristic peaks of the
perfluoro-1-octanol, 1H,1H,2H,2H-perfluoro-1-decanol, and Ti−F bond from pristine Ti3C2Tx and the C−F bond from
1-decanol, respectively (Supplementary Text, Scheme S1, and ADOPA1 in the F 1s X-ray photoelectron spectroscopy (XPS)
Figures S1−S4). Pristine MXene flakes and their aqueous curve (Figure 1c, upper spectrum, and Figure S18a,b). In the
dispersions were synthesized by the selective etching of N 1s XPS curves, ADOPA1 and AD1-Ti3C2Tx showed only a
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primary amine peak at 400.5 eV without a secondary amine can lead to high electrical conduction. Further analysis of the
peak at 396.9 eV. These results indicate the homogeneous projected density of states revealed that the carbon pz orbitals
adsorption of ADOPA1 molecules on MXenes without a (π electrons) of the benzene ring in ADOPA contribute to
polycatechol reaction (Figure 1c, lower spectrum, and Figure bands near the Fermi energy (Figure 1j). However, other
S18c and Scheme S2).16,17,27 carbon and nitrogen atoms in ADOPA and another organic
With the adsorption of a small amount of the ligand (∼6.5 molecule such as hexane do not contribute to states near the
wt %), AD1-Ti3C2Tx showed excellent dispersion stability in Fermi level (Figures S24 and S25). These calculations indicate
organic solvents, such as acetone, whereas pristine Ti3C2Tx and that the high electronic conductivity of ADOPA-functionalized
the functionalized MXenes with DOPA were aggregated MXene is attributed not only to the minimal interlayer distance
(Figure 1d and Figure S19). These results indicate that between MXene sheets caused by the minimal coverage and
organic ligands should include a hydrophilic DOPA head, the planar conformation structure of ADOPA molecules on the
which strongly interacts with the terminal groups of MXenes, MXene but also to the strong π electron interaction of ADOPA
and a hydrophobic alkyl tail compatible with organic solvents. with MXenes.
Additionally, for the uniform functionalization of MXenes at Dispersion and Oxidation Stability of AD-MXene in
minimal ADOPA loading, ADOPA ligand molecules should be Organic Media. The AD1-Ti3C2Tx flakes exhibited excellent
adsorbed on the surface of MXenes without polymerization, dispersion stability in various organic media. The AD1-
because polyADOPA would not cover the entire MXene sheet Ti3C2Tx dispersions showed a clear, bright green color and
evenly at a low loading, resulting in agglomeration of MXene in the corresponding UV−vis spectra with two characteristic
organic dispersions (Figure 1d and Supplementary Text and peaks at approximately 320 and 760 nm in various organic
Scheme S2). solvents, including ethanol (EtOH), methanol (MeOH),
The AD-Ti3C2Tx organic dispersions produced a well- isopropyl alcohol (IPA), acetone, acetonitrile (MeCN),
oriented flexible laminate film after vacuum filtration (Figure dimethyl sulfoxide (DMSO), dimethylformamide (DMF), N-
1e and Figure S20). X-ray diffraction (XRD; Figure 1f) methyl-2-pyrrolidone (NMP), and propylene carbonate (PC)
patterns of both pristine and functionalized films showed only (Figure 2a and Figure S26).12,13,20,29 This result indicates that
(00l) peaks of MXene without a (110) peak, which confirmed the AD1-Ti3C2Tx sheets were homogeneously dispersed at the
the delamination and good alignment of the MXene flakes in single-sheet level in all organic solvents tested, as their
the film.12,13,28 After surface functionalization, the AD1- characteristic color and the corresponding UV−vis spectrum
Ti3C2Tx film revealed a (002) peak upshift from 7.32 to result from the surface plasmonic resonance of the MXene
6.32°, corresponding to an interlayer spacing expansion from single sheet.19,20,22 However, the pristine Ti3C2Tx dispersions
1.22 to 1.40 nm, due to adsorption of ADOPA1 on the surface were dark gray with the corresponding UV−vis spectra in most
of the MXenes. organic solvents, but a green color and the corresponding UV−
Surprisingly, despite the homogeneous surface functionaliza- vis spectra appeared in a few polar organic solvents, such as
tion with the insulating ADOPA1 ligands, AD1-Ti3C2Tx DMSO, DMF, NMP, and PC (Figure 2b). This result indicates
exhibited an excellent electrical conductivity of 6,404 S cm−1, that pristine Ti3C2Tx was not homogeneously dispersed and
which is much superior to those of Ti3C2Tx MXenes surface- agglomerated in organic solvents because of its strong surface
functionalized with decylphosphonate (C10PA)22 and di- hydrophilicity.20,22 Solvents supporting stable colloidal sol-
(hydrogenated tallow)benzyl methylammonium chloride utions of MXenes, such as DMSO, DMF, NMP, and PC, may
(DHT)24 (Figure 1g). The MXene film showed a linear I−V not be ideal for practical applications because of their toxicity,
relation, indicating formation of an Ohmic contact (Figure high boiling points, and low dispersion yield.
S21). This indicates that the rapid and mild functionalization Nine different MXenes, including four M2X (Ti2CTx,
process does not cause any degradation of MXenes. The high Nb2CTx, Mo2CTx, and V2CTx), three M3X2 (Ti3C2Tx,
metallic conductivity of MXene maintained in the multilayer Ti3CNTx, and Mo2TiC2Tx), and two M4X3 (Mo2Ti2C3Tx
film is an extremely important observation. and Ti4N3Tx) (Supplementary Text and Figures S5−S13),
To better understand the functionalization mechanism and were functionalized with ADOPA1, and all the synthesized
high electrical conductivity, molecular dynamics (MD) and AD1-MXenes were well dispersed in various organic solvents.
density functional theory (DFT) theoretical calculations of Figure 2c,d shows that each of the AD1-MXene organic
ADOPA1 interacting with MXene were performed (see details dispersions exhibited their own characteristic colors and
in the Supplementary Text). MD simulations indicated that the corresponding UV−vis spectra. Figure S27 shows that this
hydrogen bonding between the catechol/amine moieties of corresponded to those of pristine MXene aqueous dispersions
ADOPA1 and the hydroxyl terminal groups of MXene is the with good dispersion stabilities.22,29
major functionalization reaction pathway that also causes the These results indicate that the ADOPA ligand chemistry is
ligand molecules to favor the parallel orientation conformation very efficient for functionalizing MXenes and producing
structure in solution and dried film states (Videos S3 and S4 MXene dispersions in various organic media without sacrificing
and Figure S22). The minimal increase in interlayer spacing their physical properties. The designed ADOPA ligand
after the adsorption of ADOPA1 is attributed to the minimal chemistry is universally applicable to MXenes, regardless of
coverage, as well as the planar conformation structure of the the oxidation state of the transition metals, surface functional
ADOPA1 molecules on MXene. groups, or the transition metals in MXene. It is also easily
DFT calculations also present the energetically optimized scalable for mass production with almost 100% yield.
conformation structure and band structure of AD1-Ti3C2Tx Interestingly, regardless of the length and type of the
along the out-of-plane direction (Figure 1h and Figures S23− hydrophobic tail in the ADOPA organic ligand, AD-Ti3C2Tx
S25). Along the out-of-plane (Γ−L) symmetry path, electronic showed good dispersion stability in all organic solvents tested
bands shift upward, and more states with light bands are and also exhibited high electrical conductivity comparable to
available near the Fermi energy. These light electronic bands that of pristine Ti3C2Tx fabricated from aqueous dispersions,
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Figure 3. Optical birefringence and viscoelastic properties of AD1-MXene flakes in acetonitrile. (a) POM images of AD1-Ti3C2Tx dispersions
in acetonitrile at various concentrations. (b) Upside-down vial images of AD1-Ti3C2Tx dispersions in acetonitrile at concentrations of 3 and
50 mg mL−1. (c) Dynamic storage and loss moduli (G′ and G″) of AD1-Ti3C2Tx dispersions in acetonitrile at various concentrations. (d)
POM images of different AD1-MXenes at a concentration of 50 mg mL−1 in ethanol.

due to the strong hydrogen bond and π electron interactions under ambient conditions is attributed to the low content of
between ADOPA and MXenes (Figure S28 and Table S1). water molecules in organic solvents compared to water,22 as
The AD1-Ti3C2Tx organic dispersions showed significantly well as to the surface passivation of MXene defects with
improved stability against oxidation, as confirmed by Figures ADOPA ligands.
2e−2g and Figures S29−S31. After 50 days of storage in air The AD1-Ti3C2Tx dispersions formed a lyotropic nematic
exposure at room temperature, the AD1-Ti3C2Tx dispersions liquid-crystalline phase at high concentrations (above 20 mg
retained their original 2D morphology with a high crystallinity mL−1) in various organic solvents, which was confirmed by
as well as a dark green color in organic solvents, and the strong optical birefringence in polarized optical microscopy
intensity of the UV−vis absorbance peak at 760 nm was (POM) and a frequency-independent storage modulus (G′),
retained. In contrast, the pristine Ti3C2Tx aqueous dispersions called the nonterminal elastic gel property in rheological
changed from black to translucent, cloudy liquids and showed dynamic shear tests (Figures 3a−c and Figures S32 and S33a
a rapid exponential decay of the UV−vis absorbance peak at and Video S5).3,30 Liquid crystals represent the mesomorphic
760 nm because of the oxidation of Ti3C2Tx into TiO2 ordered state of anisotropic mesogen moieties, such as 2D
nanocrystals and amorphous carbon, along with gaseous MXene flakes, which bear liquid-like fluidity and crystal-like
reaction products.19,23 ordering.3,30 The formation of a liquid-crystalline phase at high
The ADOPA-functionalized Ti3C2Tx films also showed an concentrations verifies the excellent dispersion stability of the
improved oxidation stability under 85°C/85% relative functionalized MXenes in organic solvents, because 2D MXene
humidity conditions for 20 days (Figures 2h−2j). The pristine flakes with high shape anisotropy should be homogeneously
Ti3C2Tx film revealed a significant decrease in electrical dispersed in a medium to produce liquid crystals (see
conductivity (83% decrease in the 85/85 test and 60% inhomogeneous dispersions in Figures S33b and S34). The
permanent decrease even after drying at 150 °C). In contrast, ADOPA-functionalized MXenes and their polymer composites
the AD1-Ti3C2Tx and AD4-Ti3C2Tx films revealed conductiv- also formed nematic liquid crystals in organic solvents at high
ity decreases of 20% and 40%, respectively, during the 85/85 concentrations (Figure 3d and Figure S35).
test, which were dependent on the water wettability (water Application of Electrically Conductive AD-MXene Ink.
contact angled of 106, 86, and 60° for AD1-, AD4-, and The ADOPA ligand chemistry significantly expands the utility
pristine Ti3C2Tx, respectively). However, both functionalized of MXenes in coating and printing electrical circuits on
MXene films completely recovered their initial conductivities hydrophobic substrates. The presence of hydrophobic
after drying. This indicates that the conductivity decrease (fluorinated tales) and hydrophilic (DOPA) patches on the
during the 85/85 test was caused by the moisture adsorption, surface allows the ADOPA1-functionalized MXene to bind
not oxidative degradation, which was confirmed by the Ti 2p well to substrates that are widely employed in flexible
XPS spectra (Figure 2j). Therefore, the improved stability of electronics and wearable devices, such as metals, polymers,
the ADOPA-functionalized-Ti3C2Tx in organic solvents and and even highly hydrophobic polytetrafluoroethylene (Teflon)
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Figure 4. Coating, printing capabilities, and EMI shielding performance of AD1-Ti3C2Tx. Digital photographs of various substrates dip-
coated with (a) AD1-Ti3C2Tx ethanol dispersions and (b) pristine Ti3C2Tx aqueous dispersions. (c) Digital photographs and SEM image of
AD1-Ti3C2Tx-coated shrinkable PS film after thermal shrinkage at 150 °C. (d) Digital photograph and optical microscope (red frame), SEM
(blue frame), and TEM (green frame) images of fabric screen-printed with AD1-Ti3C2Tx ethanol dispersions. (e) Digital photographs of
highly concentrated AD1-Ti3C2Tx liquid crystals and the electrically conductive “MXene” letters written with AD1-Ti3C2Tx. (f) EMI SE of
AD1-Ti3C2Tx, C10PA-Ti3C2Tx, and DHT-Ti3C2Tx films with a thickness of ∼30 μm. The EMI SE of DHT-Ti3C2Tx was theoretically
calculated through the transfer matrix method.11 The EMI SE of C10PA-Ti3C2Tx was measured in this work using a sample prepared by
interfacial grafting.22 (g) SET, SER, and SEA of AD1-Ti3C2Tx and pristine Ti3C2Tx at 12.4 GHz.

(Figure 4a). In contrast, the aqueous pristine Ti3C2Tx comparable to that of pristine Ti3C2Tx MXene with the same
dispersions showed poor adhesion to hydrophobic substrates thickness (Figure 4f). These results are attributed to AD1-
(Figure 4b). An AD1-Ti3C2Tx film spin-coated onto a Ti3C2Tx, which was successfully functionalized with ADOPA
polystyrene (PS) film retained a good adhesion without ligands and retained its intrinsic high conductivity even after
delamination, even after the significant thermal shrinkage of functionalization. Additionally, the functionalization of MXene
the PS substrate at 150 °C (Figure 4c and Figure S36). The with ADOPA ligands enhances the dielectric relaxation
concentrated AD1-MXene organic dispersions are also suitable behavior, which improves the energy dissipation of electro-
for screen printing on fabric and direct writing of electrical magnetic waves and absorption shielding ability (SEA) (Figure
circuits on various substrates (Figure 4d,e and Figures S37 and 4g).7
S38 and Videos S6 and S7). The AD1-Ti3C2Tx dispersions
were uniformly screen-printed on white cotton fabric, and the CONCLUSIONS
AD1-Ti3C2Tx flakes were uniformly coated onto fine cotton In this work, the ADOPA ligand chemistry efficiently and
fibers with an average diameter of 15 μm. The liquid-crystalline universally functionalized various types of MXenes without any
MXene paste also facilitated the fabrication of a well-oriented physical degradation under mild conditions in a simple and fast
MXene electrode with high electrical conductivity to light an manner, due to the synergistic combination of the DOPA head
LED.30,31 The AD1-Ti3C2Tx exhibited an electromagnetic strongly interacting with the MXene surface and the hydro-
interference shielding effectiveness (EMI SE) of approximately phobic tail being compatible with organic solvents. This
80 dB, which is much larger than those of Ti3C2Tx MXenes finding should stimulate further studies on the surface
surface-functionalized with other organic ligands, such as chemistry of MXenes, promote a better understanding of the
C10PA and DHT, at the same thickness of ∼30 μm and is properties and applications of MXene-based liquid crystals, and
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lead to practical applications of highly stable MXene organic Science and Engineering, Sungkyunkwan University, Suwon-
dispersions in the manufacturing of polymer matrix compo- si, Gyeonggi-do 16419, Republic of Korea; School of
sites, films, and coatings. Chemical Engineering, Sungkyunkwan University, Suwon-si,
Gyeonggi-do 16419, Republic of Korea; [Link]/0000-
EXPERIMENTAL SECTION 0002-8674-9236; Email: chongminkoo@[Link]
Materials. Ti3AlC2, Ti2AlC, and Ti3AlCN MAX phase powders
were purchased from Carbon-Ukraine, Ltd. (Ukraine). V2AlC and Authors
Nb2AlC were purchased from Laizhou Kai Ceramic Materials Co. Ltd. Tae Yun Ko − Materials Architecturing Research Center,
(China). Mo2Ga2C, Mo2TiAlC2, Mo2Ti2AlC3, and Ti4AlN3 were
purchased from Jilin 11 Technology Co. Ltd. (China). MXene flakes,
Korea Institute of Science and Technology, Seoul 02792,
with an average particle size of ∼40 μm, were sieved using a 400 mesh Republic of Korea
screen. Lithium fluoride (LiF, 98.5%) was purchased from Alfa Aesar. Daesin Kim − Materials Architecturing Research Center,
Hydrochloric acid (HCl, 37% in H2O), sulfuric acid (H2SO4, 98%), Korea Institute of Science and Technology, Seoul 02792,
potassium fluoride (KF, anhydrous 98%), sodium fluoride (NaF, Republic of Korea; KU-KIST Graduate School of Converging
98%), ethyl alcohol (EtOH, 99.9%), methyl alcohol (MeOH, 99.9%), Science and Technology, Korea University, Seoul 02841,
isopropyl alcohol (IPA, 99.9%), acetone (99.5%), acetonitrile Republic of Korea
(MeCN, 99.5%), dimethyl sulfoxide (DMSO, 99.5%), and N,N- Seon Joon Kim − Materials Architecturing Research Center,
dimethylformamide (DMF, 99.8%) were purchased from Daejung Korea Institute of Science and Technology, Seoul 02792,
Chemicals (Republic of Korea). Hydrofluoric acid (HF, 48% in H2O),
tetramethylammonium hydroxide (TMAOH, 25 wt % in H2O), N-
Republic of Korea; [Link]/0000-0002-5338-3856
methyl-2-pyrrolidone (NMP, 99.5%), propylene carbonate (PC, Hyerim Kim − Materials Architecturing Research Center,
99.5%), toluene (99.8%), 3,4-dihydroxy-L-phenylalanine (DOPA), Korea Institute of Science and Technology, Seoul 02792,
1H,1H,2H,2H-perfluoro-1-decanol (97%), 1H,1H,2H,2H-perfluoro-1- Republic of Korea; KU-KIST Graduate School of Converging
octanol (97%), 1H,1H,2H,2H-perfluoro-1-hexanol (97%), 1-decanol Science and Technology, Korea University, Seoul 02841,
(98%), and p-toluenesulfonic acid monohydrate (98%) were acquired Republic of Korea
from Sigma-Aldrich. Decylphosphonic aicd (C10PA, 98%) was Arun S. Nissimagoudar − Indo-Korea Science and Technology
purchased from TCI (Tokyo Chemical Industry Co, Ltd.). All Center, Korea Institute of Science and Technology, Bangalore
chemicals were used as received. 560065, India
Seung-Cheol Lee − Indo-Korea Science and Technology
ASSOCIATED CONTENT
Center, Korea Institute of Science and Technology, Bangalore
*
sı Supporting Information
560065, India; [Link]/0000-0002-9741-6955
The Supporting Information is available free of charge at Xiaobo Lin − Department of Chemical and Biomolecular
[Link] Engineering and Multiscale Modeling and Simulation Center,
Experimental details, preparations of MXene and Vanderbilt University, Nashville, Tennessee 37235, United
ADOPA derivatives, and AD-MXene, and character- States
ization data (PDF) Peter T. Cummings − Department of Chemical and
Functionalization of MXene flakes (MP4) Biomolecular Engineering and Multiscale Modeling and
Functionalization of MXene flakes (MP4) Simulation Center, Vanderbilt University, Nashville,
Functionalization reaction pathway (MOV) Tennessee 37235, United States
Functionalization reaction pathway (MOV) Sehyun Doo − Materials Architecturing Research Center,
Frequency-indepent storage modulus (MP4) Korea Institute of Science and Technology, Seoul 02792,
Republic of Korea; KU-KIST Graduate School of Converging
Screen printing of AD1-MXene dispersion (MP4)
Science and Technology, Korea University, Seoul 02841,
Printing of an electrical circuit with AD1-MXene Republic of Korea
dispersion (MP4) Seongmin Park − Department of IT Energy Convergence and
Department of Polymer Science and Engineering, Korea
AUTHOR INFORMATION National University of Transportation, Chungju, Chungbuk
Corresponding Authors 27469, Republic of Korea; [Link]/0000-0002-9828-
Yury Gogotsi − Department of Materials Science and 7972
Engineering and A. J. Drexel Nanomaterials Institute, Drexel Tufail Hassan − Materials Architecturing Research Center,
University, Philadelphia, Pennsylvania 19104, United States; Korea Institute of Science and Technology, Seoul 02792,
[Link]/0000-0001-9423-4032; Email: gogotsi@ Republic of Korea; KU-KIST Graduate School of Converging
[Link] Science and Technology, Korea University, Seoul 02841,
Insik In − Department of IT Energy Convergence and Republic of Korea; School of Advanced Materials Science and
Department of Polymer Science and Engineering, Korea Engineering, Sungkyunkwan University, Suwon-si, Gyeonggi-
National University of Transportation, Chungju, Chungbuk do 16419, Republic of Korea
27469, Republic of Korea; [Link]/0000-0001-7852- Taegon Oh − Materials Architecturing Research Center, Korea
1162; Email: in1@[Link] Institute of Science and Technology, Seoul 02792, Republic of
Chong Min Koo − Materials Architecturing Research Center, Korea; [Link]/0000-0003-1981-7742
Korea Institute of Science and Technology, Seoul 02792, Ari Chae − Materials Architecturing Research Center, Korea
Republic of Korea; KU-KIST Graduate School of Converging Institute of Science and Technology, Seoul 02792, Republic of
Science and Technology, Korea University, Seoul 02841, Korea; [Link]/0000-0003-2815-192X
Republic of Korea; School of Advanced Materials Science and Jihoon Lee − Department of IT Energy Convergence and
Engineering, Sungkyunkwan University, Suwon-si, Gyeonggi- Department of Polymer Science and Engineering, Korea
do 16419, Republic of Korea; School of Advanced Materials National University of Transportation, Chungju, Chungbuk
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(11) Xie, X.; et al. Microstructure and surface control of MXene
characterization and discussed the overall experimental
films for water purification. Nat. Sustain. 2019, 2, 856−862.
concepts. A.S.N. and S.-C.L. contributed to the DFT (12) Naguib, M.; et al. Two-dimensional nanocrystals produced by
calculations. X.L. and P.T.C. contributed to MD simulations. exfoliation of Ti3AlC2. Adv. Mater. 2011, 23, 4248−4253.
T.Y.K. and C.M.K. drafted the manuscript. Y.G., S.J.K., T.O., (13) Anasori, B.; Lukatskaya, M. R.; Gogotsi, Y. 2D metal carbides
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(15) Boles, M. A.; Ling, D.; Hyeon, T.; Talapin, D. V. The surface
ACKNOWLEDGMENTS science of nanocrystals. Nat. Mater. 2016, 15, 141−153.
This work was supported by grants from the Basic Science (16) Lee, H.; Dellatore, S. M.; Miller, W. M.; Messersmith, P. B.
Mussel-inspired surface chemistry for multifunctional coatings. science
Research Program (2022R1A2C3006277 and
2007, 318, 426−430.
2021M3H4A1A03047327) through the National Research (17) Liu, Y.; Ai, K.; Lu, L. Polydopamine and its derivative materials:
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and Future Planning, and the Industrial Strategic Technology biomedical fields. Chem. Rev. 2014, 114, 5057−5115.
Development Program (20020855) funded by the Ministry of (18) Halim, J.; et al. X-ray photoelectron spectroscopy of select
Trade, Industry and Energy, Republic of Korea. This work was multi-layered transition metal carbides (MXenes). Appl. Surf. Sci.
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start-up fund (S-2022-0096-000) from Sungkyunkwan Uni- 4848−4856.
(20) Maleski, K.; Mochalin, V. N.; Gogotsi, Y. Dispersions of two-
versity. This work was partially supported by the Korea
dimensional titanium carbide MXene in organic solvents. Chem.
Institute of Science and Technology (KIST). This research was Mater. 2017, 29, 1632−1640.
also partially supported by the Basic Science Research Program (21) Natu, V.; et al. Edge capping of 2D-MXene sheets with
through the National Research Foundation of Korea (NRF) polyanionic salts to mitigate oxidation in aqueous colloidal
funded by the Ministry of Education suspensions. Angew. Chem., Int. Ed. 2019, 58, 12655−12660.
(2018R1A6A1A03023788 and 2019R1A2C1010692). The (22) Kim, D.; et al. Nonpolar organic dispersion of 2D Ti3C2Tx
collaboration between Drexel University and KIST was MXene flakes via simultaneous interfacial chemical grafting and phase
supported by the Global Research and Development Center transfer method. ACS Nano 2019, 13, 13818−13828.
Program (NNFC-Drexel-SMU FIRST Nano Co-op Centre, (23) Doo, S.; et al. Mechanism and kinetics of oxidation reaction of
2015K1A4A3047100). This work was also supported as part of aqueous Ti3C2Tx suspensions at different pHs and temperatures. ACS
Appl. Mater. Interfaces 2021, 13, 22855−22865.
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