TRANSITION METAL CARBONITRIDE MXENE FILMS FOR EMI SHIELDING

Abstract

In an aspect, the present disclosure provides a heat-treated transition metal carbonitride MXene film annealed at high temperatures and a polymer composite comprising the same. In another aspect, the present disclosure provides a method for producing a heat-treated transition metal carbonitride MXene film comprising: obtaining a MXene aqueous solution containing dispersed 2-dimensional (2D) MXenes through an acid etching process; filtering the obtained MXene aqueous solution through a vacuum filtration process to produce a free-standing film; and annealing the produced free-standing film at high temperatures to obtain a heat-treated transition metal carbonitride MXene film. In still another aspect, the present disclosure provides an electromagnetic interference (EMI) shielding method comprising: superposing a coating comprising a heat-treated transition metal carbonitride MXene film on at least one surface of an object in a contact or non-contact manner.

Claims

1. A heat-treated transition metal carbonitride MXene film annealed at 100-500° C.

2. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein the MXene film has a porous structure with laminated transition metal carbonitride 2-dimensional (2D) MXenes.

3. The heat-treated transition metal carbonitride MXene film according to claim 2, wherein the transition metal carbonitride 2D MXenes comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M.sub.n+1X.sub.n, each X is positioned within an octahedral array of M, M is a transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X is a solid solution of C and N, and n is 1, 2 or 3.

4. The heat-treated transition metal carbonitride MXene film according to claim 2, wherein the transition metal carbonitride 2D MXenes comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M′.sub.2M″.sub.nX.sub.n+1, each X is positioned within an octahedral array of M′ and M″, M′ and M″ are different transition metals selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X is a solid solution of C and N, and n is 1 or 2.

5. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein porosity of the MXene film is 2-90% (v/v).

6. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein surface electrical conductivity of the MXene film is 10-5,000 S/cm.

7. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein the MXene film exhibits electromagnetic interference (EMI) shielding effectiveness (SE) of 50-200 dB in a frequency range of 0.1-100 GHz.

8. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein a thickness of the MXene film is 0.1-5,000 μm.

9. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein the annealing is performed for 0.1-24 hours.

10. The heat-treated transition metal carbonitride MXene film according to claim 1, wherein the MXene film is for EMI shielding and electromagnetic absorption.

11. A polymer composite for electromagnetic interference (EMI) shielding and electromagnetic absorption, comprising the heat-treated transition metal carbonitride MXene film according to claim 1.

12. The polymer composite for EMI shielding and electromagnetic absorption according to claim 11, wherein the heat-treated transition metal carbonitride MXene film is sandwiched between polymers.

13. A method for producing the heat-treated transition metal carbonitride MXene film according to claim 1, the method comprising: obtaining a MXene aqueous solution containing dispersed 2-dimensional (2D) MXenes from MAX through an acid etching process; filtering the obtained MXene aqueous solution through a vacuum filtration process to produce a free-standing film; and annealing the produced free-standing film at a temperature of 100-500° C. for 0.1-24 hours to obtain a heat-treated transition metal carbonitride MXene film, wherein M is at least one transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, A is any one selected from Group 13 or 14 elements, and X represents carbon and nitrogen.

14. The method according to claim 13, wherein the annealing is performed under a continuous argon (Ar) flow condition.

15. An electromagnetic interference (EMI) shielding method, comprising: superposing a coating comprising the heat-treated transition metal carbonitride MXene film according to claim 1 on at least one surface of an object in a contact or non-contact manner.

Description

BRIEF DESCRIPTION OF DRAWINGS

[0017] The present disclosure is described in more detail with reference to the accompanying drawings. Although exemplary embodiments for describing the present disclosure are shown in the drawings, the disclosed subject matter is not limited to the disclosure in the drawings. Additionally, the drawings are not necessarily drawn to scale.

[0018] FIG. 1A schematically shows the atomic crystal structure of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes. FIG. 1B shows X-ray diffraction (XRD) patterns of Ti.sub.3AlCN and Ti.sub.3AlC.sub.2 MAX phases and their corresponding Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes. FIG. 1C shows a transmission electron microscopy (TEM) image of monolayer Ti.sub.3CNT.sub.x MXene flake with the selected area electron diffraction (SAED) pattern in the inset. FIG. 1D shows optical images of aqueous dispersions of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes. FIG. 1E shows XRD patterns of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at different annealing temperatures. FIG. 1F shows XRD patterns of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at different annealing temperatures. FIG. 1G shows the comparison results of d-spacing values of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes annealed at different annealing temperatures.

[0019] FIGS. 2A to 2C show TEM images (upper) and SAED patterns (lower) of Ti.sub.3CNT.sub.x MXenes as a function of annealing temperature (as-synthesized, 250° C., 350° C.), respectively.

[0020] FIGS. 3A to 3C show TEM images (upper) and SAED patterns (lower) of Ti.sub.3C.sub.2T.sub.x MXenes as a function of annealing temperature (as-synthesized, 250° C., 350° C.), respectively.

[0021] FIG. 4A shows a thermogravimetric analysis-mass spectrometry (TGA-MS) thermogram of Ti.sub.3CNT.sub.x MXene. FIG. 4B shows a TGA-MS thermogram of Ti.sub.3C.sub.2T.sub.x MXene.

[0022] FIG. 5A shows X-ray photoelectron spectroscopy (XPS) survey spectra of as-synthesized Ti.sub.3CNT.sub.x MXene film for chemical composition analysis. FIG. 5B shows XPS survey spectra of as-synthesized Ti.sub.3C.sub.2T.sub.x MXene film for chemical composition analysis.

[0023] FIG. 6A shows high resolution XPS spectra of Ti 2p peaks of Ti.sub.3CNT.sub.x MXene films annealed at different annealing temperatures. FIG. 6B shows high resolution XPS spectra of O 1 s peaks of Ti.sub.3CNT.sub.x MXene films annealed at different annealing temperatures.

[0024] FIG. 7A shows high resolution XPS spectra of Ti 2p peaks of Ti.sub.3C.sub.2T.sub.x MXene films annealed at different annealing temperatures. FIG. 7B shows high resolution XPS spectra of O 1 s peaks of Ti.sub.3C.sub.2T.sub.x MXene films annealed at different annealing temperatures.

[0025] FIG. 8A shows a cross-sectional TEM image of Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 8B shows a high resolution TEM image of a partially oxidized upper surface of Ti.sub.3CNT.sub.x MXene film annealed at 350° C. having a lattice d-spacing of 0.352 nm, attributed to anatase TiO.sub.2. FIG. 8C shows the unoxidized inner part of Ti.sub.3CNT.sub.x MXene film annealed at 350° C.

[0026] FIG. 9A shows a cross-sectional TEM image of as-synthesized (room temperature) Ti.sub.3CNT.sub.x MXene film. FIG. 9B shows a cross-sectional TEM image of Ti.sub.3CNT.sub.x MXene film annealed at 150° C. for 6 hours. FIG. 9C shows a cross-sectional TEM image of Ti.sub.3CNT.sub.x MXene film annealed at 250° C. for 6 hours. FIG. 9D shows a cross-sectional TEM image of Ti.sub.3CNT.sub.x MXene film annealed as 350° C. for 6 hours.

[0027] FIG. 10A shows a cross-sectional scanning electron microscopy (SEM) image of as-synthesized 40 μm-thick Ti.sub.3CNT.sub.x MXene film. FIG. 10B shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 150° C. for 6 hours. FIG. 10C shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 250° C. for 6 hours. FIG. 10D shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 350° C. for 6 hours.

[0028] FIG. 11A shows a cross-sectional SEM image of as-synthesized 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene film. FIG. 11B shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene film annealed at 150° C. for 6 hours. FIG. 11C shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene film annealed at 250° C. for 6 hours. FIG. 11D shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene film annealed at 350° C. for 6 hours.

[0029] FIG. 12 shows the comparison results of porosity in 40 μm-thick annealed Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films as a function of annealing temperature.

[0030] FIG. 13A shows a cross-sectional SEM image of 10 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 13B shows a cross-sectional SEM image of 20 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 13C shows a cross-sectional SEM image of 30 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 13D shows a cross-sectional SEM image of 40 μm-thick Ti.sub.3CNT.sub.x MXene film annealed at 350° C.

[0031] FIG. 14 shows the comparison of porosity in annealed Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene as a function of initial thickness of the films.

[0032] FIG. 15 shows the comparison of electrical conductivity of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films as a function of annealing temperature.

[0033] FIG. 16A shows the total electromagnetic interference (EMI) shielding efficiency (SE.sub.T) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at different annealing temperatures. FIG. 16B shows the total EMI shielding efficiency (SE.sub.T) of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16C shows reflection EMI SE (SE.sub.R) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at different temperatures. FIG. 16D shows the total EMI SE.sub.R of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16E shows absorption EMI SE (SE.sub.A) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at different temperatures. FIG. 16F shows EMI SE.sub.A of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16G shows the comparison results of EMI SE.sub.T, SE.sub.R, and SE.sub.A of 40 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films annealed at different annealing temperatures. FIG. 16H shows the comparison of ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A of 10 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16I shows the comparison of ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A of 20 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16J shows the comparison of ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A of 30 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures. FIG. 16K shows the comparison of ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A of 40 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films annealed at different temperatures.

[0034] FIG. 17A shows EMI SE.sub.T of Ti.sub.3CNT.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17B shows EMI SE.sub.R of Ti.sub.3CNT.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17C shows EMI SE.sub.A of Ti.sub.3CNT.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17D shows EMI SE.sub.T of Ti.sub.3C.sub.2T.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17E shows EMI SE.sub.R of Ti.sub.3C.sub.2T.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17F shows EMI SE.sub.A of Ti.sub.3C.sub.2T.sub.x MXene films having different thicknesses annealed at 350° C. FIG. 17G shows the comparison of ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films having different thicknesses annealed at 350° C.

[0035] FIG. 18A shows absolute shielding effectiveness SE.sub.T, SE.sub.R, and SE.sub.A, and electrical conductivity of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times. FIG. 18B shows XRD patterns of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times. FIG. 18C shows induced porosity in 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times. FIG. 18D shows EMI SE.sub.T of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times. FIG. 18E shows EMI SE.sub.R of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times. FIG. 18F shows EMI SE.sub.A of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different annealing times.

[0036] FIG. 19 shows the comparison between experimental EMI SE.sub.T and theoretical EMI SE.sub.T of as-synthesized Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films.

[0037] FIG. 20A shows the comparison between experimental EMI SE.sub.T values (indicated by symbols) and theoretical EMI SE.sub.T values (indicated by solid lines) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. FIG. 20B shows the comparison between experimental EMI SE.sub.R values (indicated by symbols) and theoretical EMI SE.sub.R values (indicated by solid lines) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. FIG. 20C shows the comparison between experimental EMI SE.sub.A values (indicated by symbols) and theoretical EMI SE.sub.A values (indicated by solid lines) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. In FIGS. 20A to 20C, the EMI absolute shielding effectiveness SE.sub.T, SE.sub.R, and SE.sub.A values were measured at 8.2 GHz frequency.

[0038] FIG. 21A shows the comparison between experimental EMI SE.sub.T values (indicated by symbols) and theoretical EMI SE.sub.T values (indicated by solid lines) of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at 350° C. FIG. 21B shows the comparison between experimental EMI SE.sub.R values (indicated by symbols) and theoretical EMI SE.sub.R values (indicated by solid lines) of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at 350° C. FIG. 21C shows the comparison between experimental EMI SE.sub.A values (indicated by symbols) and theoretical EMI SE.sub.A values (indicated by solid lines) of 40 μm-thick Ti.sub.3C.sub.2T.sub.x MXene films annealed at 350° C. In FIGS. 21A to 21C, the EMI absolute shielding effectiveness SE.sub.T, SE.sub.R, and SE.sub.A values were measured at 8.2 GHz frequency.

[0039] FIG. 22 shows the comparison of EMI SE.sub.T of the reported shielding materials and Ti.sub.3CNT.sub.x MXene films.

[0040] FIG. 23A shows the dimensional stability of Ti.sub.3CNT.sub.x MXene film before annealing. FIG. 23B shows the dimensional stability of Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 23C shows the dimensional stability and adhesive strength of Ti.sub.3CNT.sub.x MXene film spray-coated on a glass substrate before annealing. FIG. 23D shows the dimensional stability and adhesive strength of Ti.sub.3CNT.sub.x MXene film spray-coated on a glass substrate, annealed at 350° C. FIG. 23E shows the mechanical flexibility of Ti.sub.3CNT.sub.x MXene film before annealing. FIG. 23F shows the mechanical flexibility of Ti.sub.3CNT.sub.x MXene film annealed at 350° C.

DETAILED DESCRIPTION

[0041] Ti.sub.3C.sub.2T.sub.x MXene, which is a typical 2-dimensional (2D) MXene material, has the highest electrical conductivity among MXenes, and accordingly, it has been expected that Ti.sub.3C.sub.2T.sub.x MXene would provide the best electromagnetic interference (EMI) shielding properties, but due to high electron density, Ti.sub.3C.sub.2T.sub.x MXene shows strong reflection of EMWs, and there was a risk of secondary damage caused by the strong reflection.

[0042] To solve the problem, the inventors developed MXene materials with improved electromagnetic absorption properties. The heat-treated transition metal carbonitride MXene film disclosed herein has improved absorption properties by changes of surface terminations through annealing and pore formation in the film, and consequential significant increase in EMI shielding effectiveness (SE).

[0043] Accordingly, the present disclosure relates to a transition metal carbonitride MXene film which is effective for EMI shielding and absorption and a method producing the same, and an EMI shielding method using the same.

[0044] In an aspect, the present disclosure may relate to a heat-treated transition metal carbonitride MXene film annealed at 100-500° C.

[0045] In an embodiment, the heat-treated transition metal carbonitride MXene film may be annealed at the temperature of 100° C. or more, 110° C. or more, 120° C. or more, 130° C. or more, 140° C. or more, 150° C. or more, 160° C. or more, 170° C. or more, 180° C. or more, 190° C. or more, 200° C. or more, 210° C. or more, 220° C. or more, 230° C. or more, 240° C. or more, 250° C. or more, 260° C. or more, 270° C. or more, 280° C. or more, 290° C. or more, 300° C. or more, 310° C. or more, 320° C. or more, 330° C. or more, 340° C. or more, 350° C. or more, 360° C. or more, 370° C. or more, 380° C. or more, 390° C. or more, 400° C. or more, 410° C. or more, 420° C. or more, 430° C. or more, 440° C. or more, 450° C. or more, 460° C. or more, 470° C. or more, 480° C. or more, or 490° C. or more, and the heat-treated transition metal carbonitride MXene film may be annealed at the temperature of 500° C. or less, 490° C. or less, 480° C. or less, 470° C. or less, 460° C. or less, 450° C. or less, 440° C. or less, 430° C. or less, 420° C. or less, 410° C. or less, 400° C. or less, 390° C. or less, 380° C. or less, 370° C. or less, 360° C. or less, 350° C. or less, 340° C. or less, 330° C. or less, 320° C. or less, 310° C. or less, 300° C. or less, 290° C. or less, 280° C. or less, 270° C. or less, 260° C. or less, 250° C. or less, 240° C. or less, 230° C. or less, 220° C. or less, 210° C. or less, 200° C. or less, 190° C. or less, 180° C. or less, 170° C. or less, or 160° C. or less.

[0046] In an embodiment, the MXene film may have a porous structure with laminated transition metal carbonitride 2D MXenes. That is, the MXene film may have a porous structure such that MXene layers of free-standing 2D assemblies with a continuous crystal structure are laminated and pores are formed between the MXene layers.

[0047] In an embodiment, the transition metal carbonitride 2D MXenes may comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M.sub.n+1X.sub.n.

[0048] Here, each X may be positioned within an octahedral array of M, M may be a transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X may be a solid solution of C and N, and n may be 1, 2 or 3.

[0049] In an embodiment, M may be, for example, Sc, Y, Lu, Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W or a combination thereof, but is not limited thereto, and the empirical formula of M.sub.n+1X.sub.n may be, for example, Ti.sub.3CN and Ti.sub.2C.sub.0.5N.sub.0.5, but is not limited thereto.

[0050] In an embodiment, the transition metal carbonitride 2D MXenes may comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M′.sub.2M″.sub.nX.sub.n+1.

[0051] Here, each X may be positioned within an octahedral array of M′ and M″, M′ and M″ may be different transition metals selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X may be a solid solution C and N, and n may be 1 or 2.

[0052] In an embodiment, M may be, for example, Ti, V, Nb, Ta, Cr, Mo or a combination thereof, but is not limited thereto, and the empirical formula of M′.sub.2M″.sub.nX.sub.n+1 may be, for example, Ti.sub.2MoCN, but is not limited thereto.

[0053] FIG. 1A schematically shows the atomic crystal structure of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes.

[0054] As shown in FIG. 1A, one or two surfaces of each layer of 2D MXenes may include hydrophilic terminations indicated by T.sub.x during synthesis from MAX phases, and in an embodiment, the terminations may be selected from alkoxide, carboxylate, halide, hydroxide, hydride, oxide, sub-oxide, nitride, sub-nitride, sulfide, thiol or a combination thereof, and may be selected from, for example, —OH, ═O, —F or a combination thereof.

[0055] In an embodiment, the porosity of the heat-treated transition metal carbonitride MXene film may be 2-90% (v/v). More specifically, the porosity of the heat-treated transition metal carbonitride MXene film may be 2% (v/v) or more, 4% (v/v) or more, 6% (v/v) or more, 8% (v/v) or more, 9% (v/v) or more, 10% (v/v) or more, 11% (v/v) or more, 12% (v/v) or more, 13% (v/v) or more, 14% (v/v) or more, 15% (v/v) or more, 16% (v/v) or more, 17% (v/v) or more, 18% (v/v) or more, 19% (v/v) or more, 20% (v/v) or more, 23% (v/v) or more, 25% (v/v) or more, 27% (v/v) or more, 30% (v/v) or more, 33% (v/v) or more, 35% (v/v) or more, 37% (v/v) or more, 40% (v/v) or more, 45% (v/v) or more, 50% (v/v) or more, 55% (v/v) or more, 60% (v/v) or more, 65% (v/v) or more, 70% (v/v) or more, 75% (v/v) or more, 80% (v/v) or more, or 85% (v/v) or more, and the porosity of the heat-treated transition metal carbonitride MXene film may be 90% (v/v) or less, 85% (v/v) or less, 80% (v/v) or less, 75% (v/v) or less, 70% (v/v) or less, 65% (v/v) or less, 60% (v/v) or less, 55% (v/v) or less, 50% (v/v) or less, 47% (v/v) or less, 45% (v/v) or less, 40% (v/v) or less, 37% (v/v) or less, 35% (v/v) or less, 33% (v/v) or less, 30% (v/v) or less, 27% (v/v) or less, 25% (v/v) or less, 23% (v/v) or less, 20% (v/v) or less, 19% (v/v) or less, 18% (v/v) or less, 17% (v/v) or less, 16% (v/v) or less, 15% (v/v) or less, 14% (v/v) or less, 13% (v/v) or less, 12% (v/v) or less, 11% (v/v) or less, 10% (v/v) or less, 9% (v/v) or less, 8% (v/v) or less, 6% (v/v) or less, or 4% (v/v) or less.

[0056] In an embodiment, the heat-treated transition metal carbonitride MXene film may have surface electrical conductivity of 10-5,000 S/cm. More specifically, the heat-treated transition metal carbonitride MXene film may have surface electrical conductivity of 10 S/cm or more, 50 S/cm or more, 100 S/cm or more, 200 S/cm or more, 300 S/cm or more, 400 S/cm or more, 500 S/cm or more, 600 S/cm or more, 700 S/cm or more, 800 S/cm or more, 900 S/cm or more, 1,000 S/cm or more, 1,050 S/cm or more, 1,100 S/cm or more, 1,120 S/cm or more, 1,125 S/cm or more, 1,150 S/cm or more, 1,200 S/cm or more, 1,300 S/cm or more, 1,400 S/cm or more, 1,500 S/cm or more, 1,600 S/cm or more, 1,700 S/cm or more, 1,800 S/cm or more, 1,900 S/cm or more, 2,000 S/cm or more, 2,100 S/cm or more, 2,200 S/cm or more, 2,300 S/cm or more, 2,400 S/cm or more, 2,450 S/cm or more, 2,500 S/cm or more, 2600 S/cm or more, 2,800 S/cm or more, 3,000 S/cm or more, 3,200 S/cm or more, 3,400 S/cm or more, 3,600 S/cm or more, 3,800 S/cm or more, 4,000 S/cm or more, 4,200 S/cm or more, 4,400 S/cm or more, 4,600 S/cm or more, or 4,800 S/cm or more, and the heat-treated transition metal carbonitride MXene film may have surface electrical conductivity of 5,000 S/cm or less, 4,800 S/cm or less, 4,600 S/cm or less, 4,400 S/cm or less, 4,200 S/cm or less, 4,000 S/cm or less, 3,800 S/cm or less, 3,600 S/cm or less, 3,400 S/cm or less, 3,200 S/cm or less, 3,000 S/cm or less, 2,800 S/cm or less, 2,600 S/cm or less, 2,490 S/cm or less, 2,480 S/cm or less, 2,475 S/cm or less, 2,400 S/cm or less, 2,300 S/cm or less, 2,200 S/cm or less, 2,100 S/cm or less, 2,000 S/cm or less, 1,900 S/cm or less, 1,800 S/cm or less, 1,700 S/cm or less, 1,600 S/cm or less, 1,500 S/cm or less, 1,400 S/cm or less, 1,300 S/cm or less, 1,200 S/cm or less, 1,100 S/cm or less, 1,000 S/cm or less, 900 S/cm or less, 800 S/cm or less, 700 S/cm or less, 600 S/cm or less, 500 S/cm or less, 400 S/cm or less, 300 S/cm or less, 200 S/cm or less, 100 S/cm or less, or 50 S/cm or less.

[0057] In an embodiment, the heat-treated transition metal carbonitride MXene film may exhibit EMI SE of 50-200 dB in the frequency range of 0.1-100 GHz. More specifically, the heat-treated transition metal carbonitride MXene film may exhibit EMI SE of 50 dB or more, 55 dB or more, 60 dB or more, 70 dB or more, 80 dB or more, 90 dB or more, 100 dB or more, 110 dB or more, 120 dB or more, 130 dB or more, 140 dB or more, 150 dB or more, 160 dB or more, 170 dB or more, 180 dB or more, or 190 dB or more in the frequency range of 0.1 GHz or more, 0.3 GHz or more, 0.5 GHz or more, 1 GHz or more, 2 GHz or more, 3 GHz or more, 5 GHz or more, 8 GHz or more, 9 GHz or more, 10 GHz or more, 11 GHz or more, 12 GHz or more, 15 GHz or more, 20 GHz or more, 30 GHz or more, 40 GHz or more, 50 GHz or more, 60 GHz or more, 70 GHz or more, 80 GHz or more, or 90 GHz or more, and 100 GHz or less, 90 GHz or less, 80 GHz or less, 70 GHz or less, 60 GHz or less, 50 GHz or less, 40 GHz or less, 30 GHz or less, 20 GHz or less, 15 GHz or less, 13 GHz or less, 12 GHz or less, 11 GHz or less, 10 GHz or less, 9 GHz or less, 8 GHz or less, 5 GHz or less, 3 GHz or less, 2 GHz or less, 1 GHz or less, 0.5 GHz or less, or 0.3 GHz or less, and the heat-treated transition metal carbonitride MXene film may exhibit EMI SE of 200 dB or less, 190 dB or less, 180 dB or less, 170 dB or less, 160 dB or less, 150 dB or less, 140 dB or less, 130 dB or less, 120 dB or less, 110 dB or less, 100 dB or less, 90 dB or less, 80 dB or less, 70 dB or less, 65 dB or less, 60 dB or less, or 55 dB or less in the above-described frequency range.

[0058] In an embodiment, the heat-treated transition metal carbonitride MXene film may be 0.1-5,000 μm in thickness. More specifically, the thickness of the heat-treated transition metal carbonitride MXene film may be 0.1 μm or more, 0.3 μm or more, 0.5 μm or more, 0.7 μm or more, 1 μm or more, 1.5 μm or more, 2 μm or more, 2.5 μm or more, 3 μm or more, 3.5 μm or more, 4 μm or more, 4.5 μm or more, 5 μm or more, 6 μm or more, 7 μm or more, 8 μm or more, 9 μm or more, 10 μm or more, 15 μm or more, 20 μm or more, 25 μm or more, 30 μm or more, 35 μm or more, 40 μm or more, 45 μm or more, 50 μm or more, 70 μm or more, 100 μm or more, 200 μm or more, 300 μm or more, 400 μm or more, 500 μm or more, 600 μm or more, 700 μm or more, 800 μm or more, 900 μm or more, 1,000 μm or more, 1,500 μm or more, 2,000 μm or more, 2,500 μm or more, 3,000 μm or more, 3,500 μm or more, 4,000 μm or more, or 4,500 μm or more, and the thickness of the heat-treated transition metal carbonitride MXene film may be 5,000 μm or less, 4,500 μm or less, 4,000 μm or less, 3,500 μm or less, 3,000 μm or less, 2,500 μm or less, 2,000 μm or less, 1,500 μm or less, 1,000 μm or less, 900 μm or less, 800 μm or less, 700 μm or less, 600 μm or less, 500 μm or less, 400 μm or less, 300 μm or less, 200 μm or less, 100 μm or less, 70 μm or less, 50 μm or less, 45 μm or less, 40 μm or less, 35 μm or less, 30 μm or less, 25 μm or less, 20 μm or less, 15 μm or less, 10 μm or less, 9 μm or less, 8 μm or less, 7 μm or less, 6 μm or less, 5 μm or less, 4.5 μm or less, 4 μm or less, 3.5 μm or less, 3 μm or less, 2.5 μm or less, 2 μm or less, 1.5 μm or less, 1 μm or less, 0.7 μm or less, 0.5 μm or less, or 0.3 μm or less.

[0059] In an embodiment, the annealing may be performed for 0.1-24 hours. More specifically, the heat-treated transition metal carbonitride MXene film may be produced by annealing the transition metal carbonitride MXene film for 0.1 hours or more, 0.5 hours or more, 1 hour or more, 2 hours or more, 3 hours or more, 4 hours or more, 5 hours or more, 6 hours or more, 7 hours or more, 8 hours or more, 10 hours or more, 12 hours or more, 14 hours or more, 16 hours or more, 18 hours or more, 20 hours or more, or 22 hours or more, and the heat-treated transition metal carbonitride MXene film may be produced by annealing the transition metal carbonitride MXene film for 24 hours or less, 22 hours or less, 20 hours or less, 18 hours or less, 16 hours or less, 14 hours or less, 12 hours or less, 10 hours or less, 8 hours or less, 7 hours or less, 6 hours or less, 5 hours or less, 4 hours or less, 3 hours or less, 2 hours or less, or 1 hour or less.

[0060] In an embodiment, the heat-treated transition metal carbonitride MXene film may be for EMI shielding and electromagnetic absorption.

[0061] In another aspect, the present disclosure may relate to a polymer composite for EMI shielding and electromagnetic absorption, comprising the heat-treated transition metal carbonitride MXene film.

[0062] In an embodiment, the polymer composite may comprise the heat-treated transition metal carbonitride MXene film sandwiched between polymers.

[0063] In an embodiment, the heat-treated transition metal carbonitride MXene film may form a composite with polymer, and the polymer may include organic polymer, to be more specific, thermosetting or thermoplastic polymer or polymer resin, elastomer or a mixture thereof. The polymer may include, for example, polyester, polyethylenenaphthalate (PEN), polybutylene terephthalate (PBT), polyethersulfone (PES), polytetrafluoroethylene (PTFE), polyvinylfluoride (PVF), epoxy resin, polyvinyl chloride (PVC), polypropylene (PP), polyethylene (PE), polyetherimide (PEI), acrylate-based resin, polyamide (PA), acrylonitrile-butadiene-styrene (ABS) resin, polyamide imide (PAI), polybenzoimidazol (PBI), polyphenylene sulfide (PPS), polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), polyethylene terephthalate (PET), polyoxymethylene (POM), polyetherketone (PEK), polyetheretherketone (PEEK), polyaryletherketone (PAEK), liquid crystal polymer (LCP), polyimide (PI), polycarbonate (PC), sulfonated polyphenylene (SPR), (meth)acrylate-based polymer, urethane(meth)acrylate-based polymer, polystyrene (PS), polyurethane and polysiloxane, but is not limited thereto.

[0064] In another aspect, the present disclosure a method for producing the heat-treated transition metal carbonitride MXene film, comprising: obtaining a MXene aqueous solution containing dispersed 2D MXenes from MAX through an acid etching process; filtering the obtained MXene aqueous solution through a vacuum filtration process to produce a free-standing film; and annealing the produced free-standing film at the temperature of 100-500° C. for 0.1-24 hours to obtain a heat-treated transition metal carbonitride MXene film.

[0065] Here, M is at least one transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, A is any one selected from Group 13 or 14 elements, X represents carbon and nitrogen, and each of M, A and X is the same as described in detail above.

[0066] In an embodiment, an etchant used in the acid etching process may include strong acids containing F such as HF, NH.sub.4HF.sub.2 or HCl—LiF mixture, but is not limited thereto. The MXene produced by the acid etching process may be indicated by M.sub.n+1X.sub.n(T.sub.x) or M′.sub.2M″.sub.nX.sub.n+1(T.sub.x), where T.sub.x denotes terminations formed on the surface of the 2D MXene via etching as described in detail above, and may be, for example, —OH, ═O, —F or a combination thereof.

[0067] Additionally, the MXene aqueous solution prepared by the acid etching process may be an acidic solution with a pH of 1-6, a neutral solution with a pH of 6-7, and a basic solution with a pH of 8-14 by adjusting its pH.

[0068] In an embodiment, the annealing may be performed under continuous argon (Ar) flow conditions.

[0069] The annealing temperature and time in the annealing step is the same as described in detail above.

[0070] In another aspect, the present disclosure may relate to an EMI shielding method comprising: superposing a coating comprising the heat-treated transition metal carbonitride MXene film on at least one surface of an object in a contact or non-contact manner.

[0071] That is, the present disclosure may relate to a method for shielding an object from EMI by superposing a coating comprising the heat-treated transition metal carbonitride MXene film according to an aspect of the present disclosure on at least one surface of the object in a contact or non-contact manner.

[0072] As an embodiment, the present disclosure may provide the following embodiments, and the following embodiments are provided to supplement the previous description, but not intended to replace or substitute the previous description.

[0073] A first embodiment may provide a heat-treated transition metal carbonitride MXene film annealed at 100-500° C.

[0074] A second embodiment may provide the heat-treated transition metal carbonitride MXene film according to the first embodiment, wherein the MXene film has a porous structure with laminated transition metal carbonitride 2D MXenes.

[0075] A third embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first and second embodiments, wherein the transition metal carbonitride 2D MXenes comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M.sub.n+1X.sub.n, each X is positioned within an octahedral array of M, M is a transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X is a solid solution of C and N, and n is 1, 2 or 3.

[0076] A fourth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to third embodiments, wherein the transition metal carbonitride 2D MXenes comprise at least one layer, each layer comprising a 2D array of crystalline cells having an empirical formula of M′.sub.2M″.sub.nX.sub.n+1, each X is positioned within an octahedral array of M′ and M″, M′ and M″ are different transition metals selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, X is a solid solution of C and N, and n is 1 or 2.

[0077] A fifth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to fourth embodiments, wherein porosity of the MXene film is 2-90% (v/v).

[0078] A sixth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to fifth embodiments, wherein surface electrical conductivity of the MXene film is 10-5,000 S/cm.

[0079] A seventh embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to sixth embodiments, wherein the heat-treated transition metal carbonitride MXene film exhibits EMI SE of 50-200 dB in a frequency range of 0.1-100 GHz.

[0080] An eighth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to seventh embodiment, wherein a thickness of the MXene film is 0.1-5,000 μm.

[0081] A ninth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to eighth embodiments, wherein the annealing is performed for 0.1-24 hours.

[0082] A tenth embodiment may provide the heat-treated transition metal carbonitride MXene film according to at least one of the first to ninth embodiments, wherein the MXene film is for EMI shielding and electromagnetic absorption.

[0083] An eleventh embodiment may provide a polymer composite for EMI shielding and electromagnetic absorption, comprising the heat-treated transition metal carbonitride MXene film according to any one of the first to tenth embodiments.

[0084] A twelfth embodiment may provide the polymer composite for EMI shielding and electromagnetic absorption according to the eleventh embodiment, wherein the heat-treated transition metal carbonitride MXene film is sandwiched between polymers.

[0085] A thirteenth embodiment may provide a method for producing the heat-treated transition metal carbonitride MXene film according to any one of the first to tenth embodiments, comprising: obtaining a MXene aqueous solution containing dispersed 2D MXenes through an acid etching process; filtering the obtained MXene aqueous solution through a vacuum filtration process to produce a free-standing film; and annealing the produced free-standing film at the temperature of 100-500° C. for 0.1-24 hours to obtain a heat-treated transition metal carbonitride MXene film, where M is at least one transition metal selected from the group consisting of Group IIIB metal, Group IVB metal, Group VB metal and Group VIB metal, A is any one selected from Group 13 or 14 elements, and X denotes carbon and nitrogen.

[0086] A fourteenth embodiment may provide the method according to the thirteenth embodiment, wherein the annealing is performed under a continuous argon (Ar) flow condition.

[0087] A fifteenth embodiment may provide an EMI shielding method comprising: superposing a coating comprising the heat-treated transition metal carbonitride MXene film according to any one of the first to tenth embodiments on at least one surface of an object in a contact or non-contact manner.

[0088] The transition metal carbonitride MXene according to an aspect of the present disclosure is a solid solution MXene in which half of carbon atoms occupying octahedral sites in AB-AB hexagonal structure are substituted by nitrogen atoms, and due to the change in chemical composition, the transition metal carbonitride MXene has unique properties that are very different from the counterpart transition metal carbide MXene, i.e., having the same transition metal.

[0089] Specifically, the transition metal carbonitride MXene film, according to an aspect of the present disclosure, exhibits a larger interlayer spacing (d-spacing). The large d-spacing of transition metal carbonitride MXene is due to its high tendency to absorb water molecules, and this may be the cause of its low electrical conductivity at room temperature. The following examples confirmed that when the transition metal carbonitride MXene film according to an aspect of the present disclosure is annealed, as the annealing temperature increases, the desorption of water molecules increases and the surface terminations of each layer are removed, and thus the d-spacing value decreases and the electrical conductivity increases.

[0090] The removal of water molecules and surface terminations gives rise to porosity in transition metal carbonitride MXene film, and this shows a direct relationship with the annealing temperature. It is expected that the induced porosity will improve the total EMI shielding and electromagnetic absorption in the porous structure of transition metal carbonitride MXene film, and the porous structure has a positive influence on EMI shielding by extending the path length of EMWs before transmission and improving the subsequent absorption phenomenon with the introduction of multiple interfaces acting as scattering sites for the incident EMWs.

[0091] Additionally, according to theoretical studies, as the porosity is higher, EMI shielding properties are enhanced and absorption contribution is improved. This factor may be enhanced when high porosity does not reduce the electrical conductivity of shielding materials. The following examples confirmed that in the case of the transition metal carbonitride MXene film according to an aspect of the present disclosure, the porosity linearly increases with the increasing annealing temperature, but as the temperature increases, the film becomes unstable for oxidation, and transition metal oxide nanocrystals which are dielectrics are formed on the surface of the film, resulting in low electrical conductivity, and severe oxidation causes degradation of the electrical properties of the film and degradation of the overall EMI shielding properties.

[0092] However, the following examples confirmed that as a result of analyzing the EMI shielding properties of transition metal carbide MXene film annealed in the same condition, as opposed to transition metal carbonitride MXene film, it is stable for oxidation, has a small d-spacing value and high electrical conductivity, and undergoes less volume expansion arising from porosity due to annealing, but rather results in lower final EMI shielding properties.

EXAMPLES

[0093] Hereinafter, the following examples are provided to describe the present disclosure in more detail. Each example is regarded as providing each specific embodiment of compositions and fabrication and use methods, but none of the examples should be deemed as limiting the more generic embodiments described herein. In particular, the following examples focus specific 2-dimensional (2D) titanium carbonitride Ti.sub.3CNT.sub.x MXenes and their fabrication methods and their electromagnetic shielding effectiveness, but the described principle may be applied to other 2D transition metal carbonitride MXenes. That is, these examples are provided to help the understanding of the present disclosure and should not be interpreted as limiting the present disclosure, and modifications, substitutions and addition commonly known in the art may be made thereto, and the scope of the present disclosure covers such modifications, substitutions and addition.

[0094] In the following examples, attempts have been made to ensure accuracy of the used names and figures (for example, composition, amount, temperature, thickness, etc.), but some experimental errors and deviations should be considered, and unless otherwise stated, the temperature is in degree Celsius (° C.) and the pressure is at or near atmospheric.

Example 1. Materials and Methods

Example 1.1 Materials

[0095] Ti.sub.3AlCN MAX powder with a particle size of less than 38 μm was synthesized at the lab scale following Hantanasirisakul, K., et al., Effects of Synthesis and Processing on Optoelectronic Properties of Titanium Carbonitride MXene. Chemistry of Materials, 2019. 31: p. 2941-2951, and Ti.sub.3AlC.sub.2 MAX powder with a particle size of less than 38 μm was purchased from Carbon-Ukraine ltd. Lithium fluoride (LiF, 98.5%) and hydrochloric acid (HCl, 37%) were purchased from Alfa Aesar, and polypropylene membrane (Celgard, pore size 0.064 μm) was used to obtain MXene films via vacuum-assisted filtration.

Example 1.2 Synthesis of Ti.SUB.3.CNT.SUB.x .MXene

[0096] Ti.sub.3CNT.sub.x was synthesized from Ti.sub.3AlCN MAX phase. In this synthesis protocol, Ti.sub.3AlCN was used instead of Ti.sub.3AlC.sub.2. Briefly describing, 1 g of Ti.sub.3AlCN MAX was gradually added to a mixture of 20 mL of 9 M HCl and 1.6 g of LiF in a 100 mL polypropylene bottle with continuous stirring at room temperature for 24 hours. The obtained mixture was washed with deionized water 5-6 times by centrifugation at 3500 rpm to reach close to a neutral pH value. Finally, a stable well-dispersed suspension containing single-to-few layer Ti.sub.3CNT.sub.x MXene flakes was obtained by collecting the supernatant after centrifugation at 3500 rpm for 5 minutes.

Example 1.3 Preparation of Ti.SUB.3.CNT.SUB.x .MXene Film

[0097] Free-standing films were prepared by filtering a measured amount of MXene dispersion through a Celgard membrane. The thickness of the films was controlled by the volume of the as-synthesized dispersion during vacuum filtration.

Example 1.4 Annealing of Ti.SUB.3.CNT.SUB.x .MXene Film

[0098] The films with different thicknesses were thermally treated in an inert environment of continuous argon (Ar) flow at different annealing temperatures of 150° C., 250° C. and 350° C. for 6 hours. Additionally, 40 μm-thick Ti.sub.3CNT.sub.x MXene films were annealed at 350° C. for different annealing times of 0.5, 1, 2, 3, 6, 12 and 24 hours.

Example 1.5 Synthesis of Ti.SUB.3.C.SUB.2.T.SUB.x .MXene

[0099] Ti.sub.3C.sub.2T.sub.x was synthesized from Ti.sub.3AlC.sub.2 MAX powder after etching “Al” layers. The synthesis method of Ti.sub.3C.sub.2T.sub.x is the same as described in U.S. patent application Ser. No. 16/092,338 filed on Apr. 21, 2017, and all the conditions were the same as those reported above for Ti.sub.3CNT.sub.x except the synthesis temperature. In this case, the synthesis temperature was increased up to 35° C. to get a higher yield from the reaction. The obtained films (similar in thickness to Ti.sub.3CNT.sub.x film) after vacuum filtration of the solution were annealed at the same temperature as Ti.sub.3CNT.sub.x.

Example 1.6 Annealing of Spray-Coated MXene Films on a Glass Substrate

[0100] Micrometer-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films were spray-coated on a glass substrate and completely dried on a hot plate set to the temperature of 90° C. The spray-coated films were annealed to analyze the adhesive strength of the MXene films during heat treatment. In this instance, the spray-coated Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films on the glass substrate were annealed at 350° C. for 6 hours.

Example 2 Materials Characterization

Example 2.1 Characterization

[0101] The structure and morphology of pristine and heat-treated Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films were investigated by a scanning electron microscope (SEM) (Inspect F50, FEI, USA) and a transmission electron microscope (TEM) (Tecnai F20 G2, FEI, at 200.0 kV voltage). The initial thickness measurements were performed using a highly accurate length gauge (with a tolerance factor of ±0.1 μm) of Heidenhain Instruments (Germany), and were verified using SEM.

[0102] A focused ion beam (FIB) (Nova 600 Nanolab, FEI Company, Netherland) was used to cut the cross-section of the films in order to analyze the cross-sectional morphology of the samples using high resolution TEM images and element mapping (high resolution TEM (HRTEM) Talos, FEI Company, F200X).

[0103] X-ray diffraction (XRD) patterns were obtained using a D8 diffractometer with Cu-Kα radiation (40 kV and 44 mA) at a 28 (theta) range of 4° to 70° with a scanning step of 0.02°, a step time of 0.5 s, and a window slit of 10×10 mm.sup.2. Changes in chemical structure were examined using X-ray photoelectron spectroscopy (XPS, PHI 5000 VersaProbe, Ulvac-PHI, Japan) by Al-Kα as the X-ray source with a power of 25 W.

[0104] Simultaneous thermogravimetric-mass spectrometry analysis (TGA-MS) was performed on a Discovery SDT 650 model connected to a Discovery mass spectrometer (TA Instruments, DE). Vacuum-filtered films of MXenes were cut into small pieces and packed in a 90 μL alumina pan. Before heating, the analysis chamber was flushed with helium (He) gas at 100 mL/min for 1 hour to reduce residual air. The samples were heated to 350° C. at a constant heating rate of 10° C./min in the He atmosphere (100 mL/min).

[0105] The density and porosity were calculated experimentally using the mass and volume of the films.

[0106] Electrical conductivity of the samples was measured using an advanced four probe (MCP-TP06P PSP) connected with Loresta-GP meter (Model MCP-T610, Mitsubishi Chemical, Japan). The distance between pins of the probe was 1.5 mm, and the open circuit voltage was set to 10 V. The 4-pin probe was positioned at different locations of the film (a minimum of 5 locations to obtain an average value) and the sheet resistance was recorded. Subsequently, the electrical conductivity of all the samples was calculated by σ=(R.sub.s×t).sup.−1, where σ is the electrical conductivity [S/cm], R.sub.s is the sheet resistance [Ω/sq], and t is the thickness [cm] of the sample.

[0107] Electromagnetic interference (EMI) shielding effectiveness (SE) of all the samples was measured by WR-90 rectangular waveguide using a 2-port network analyzer (ENA5071C, Agilent Technologies, USA) in the frequency range of 8.2-12.4 GHz (X-band). The standard calibration procedure for equipment calibration was performed using short offset, short and load on both ports. The pristine and annealed samples were cut into rectangular dimensions of 25×12 mm.sup.2, slightly larger than that of sample holder's opening 22.84×10.14 mm.sup.2. The samples were mounted carefully to avoid any leakage from the edges of the waveguide and screwed tightly before taking the final measurements.

Example 2.2 EMI Shielding Effectiveness Measurements

[0108] EMI SE is the ability of a material to attenuate the energy of incident EMWs. When electromagnetic radiations interact with the material under test (shield), the shielding phenomenon is governed by reflection (R), absorption (A) and transmission (T), collectively must add up to 1. That is, the following equation is given:


R+T+A=1  (1)

[0109] The reflection (R) and transmission (T) coefficients are obtained from the network analyzer in the form of scattering parameters (S.sub.12, S.sub.12, S.sub.21, S.sub.22), which can be used to find the R and T coefficients as:


R=|S.sub.11|.sup.2=|S.sub.22|.sup.2  (2)


T=|S.sub.21|.sup.2=|S.sub.12|.sup.2  (3)

[0110] The total EMI SE (EMI SE.sub.T) is the sum of the contributions from reflection (SE.sub.R), absorption (SE.sub.A) and multiple internal reflections (SE.sub.MR). The total EMI SE.sub.T can be written as:


SE.sub.T=SE.sub.R+SE.sub.A+SE.sub.MR  (4)

[0111] For calculations, SE.sub.MR is generally considered negligible when SE.sub.T is higher than 15 dB. SE.sub.R and SE.sub.A can be expressed in terms of reflection and absorption coefficient considering the power of the incident EMWs inside the shielding material as:

[00001] SE R = 10 log ( 1 1 - R ) = 10 log ( 1 1 - .Math. S 11 .Math. 2 ) ( 5 ) SE A = 10 log ( 1 - R T ) = 10 log ( 1 - .Math. S 11 .Math. 2 .Math. S 21 .Math. 2 ) ( 6 )

[0112] Assuming propagation of EMWs in a nonmagnetic and highly conducting medium, the Fresnel formula for reflection, absorption and multiple reflections, using equation 4, can be given as:

[00002] SE T = 10 log ( 1 T ) = 10 log ( E i E t ) 2 = 20 log .Math. ( 1 + N ) 2 4 N e - kd [ 1 - ( 1 - N 1 + N ) 2 e 2 ikd ] .Math. ( 7 )

[0113] where E.sub.i and E.sub.t are incident and transmitted intensities of electric field of the EMWs, respectively; N is the complex refractive index of the shield, k is the imaginary part of refractive index, and d is the shield thickness. Due to its excellent conductivity (5,000-10,000 S/cm), the complex refractive index (Nm) of MXene is given as:

[00003] N m = σ 2 ω.Math. 0 ( 1 + i )

[0114] In equation 7, the quantitative contributions from SE.sub.R, SE.sub.A and SE.sub.MR are expressed as:

[00004] SE R = 20 log ( ( 1 + N ) 2 4 .Math. N .Math. ) = 50 + 10 log ( σ f ) ( 8 ) SE A = 20 log e - kd = 20 log e α d = 8.686 α d = 1.7 d σ f ( 9 ) SE MR = 20 log .Math. 1 - e ( 2 ikd ) ( 1 - N ) 2 ( 1 + N ) 2 .Math. ( 10 )

[0115] In equation 9, α is the attenuation constant indicating the ability of a material to absorb the associated energy of incident EMWs. Neglecting the role of multiple reflection for total shielding efficiency SE.sub.T higher than 15 dB, using equations 4, 8 and 9, SE.sub.T can be written as the following equation known as Simon's formula:

[00005] SE T = 50 + 10 log ( σ f ) + 1.7 d σ f ( 11 )

Example 2.3 Theoretical Calculation of EMI Shielding Effectiveness (SE)

[0116] Theoretical EMI SE.sub.T, SE.sub.E, and SE.sub.A for Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes were calculated by transfer matrix method. The transfer matrix method considers analytical solution for calculating transmission, reflection, and absorption of EMWs propagating through a 2D infinite plane interface and layers with known thickness.

[0117] This method provides an exact solution for multiple reflections between layers having much smaller thickness than the wavelength of incident waves. The transfer equation for the propagation through N thin layers is expressed as follows:

[00006] ( E t + E t - ) = [ M 2 . M 1 ] N ( E i + E i - ) = ( a b c d ) ( E i + E i - ) ( 12 )

[0118] where M1 and M2 are the transfer matrices for the propagation through an interface and propagation within a layer, respectively. E.sup.+ and E.sup.− represent the electric field amplitudes of the forward and backward EMWs in a medium, respectively.

[0119] In homogeneous and isotropic media, the matrices M1 and M2 are expressed as:

[00007] M 1 ( i , j ) = 1 t i , j ( 1 - r ij - r ij 1 ) , and M 2 ( n , l ) = ( Φ - 1 0 0 Φ ) ( 13 )

[0120] Here, r.sub.ij and t.sub.ij are the complex amplitude reflection and transmission Fresnel coefficients, respectively, and EMWs propagate from the i layer to the j layer through the interfaces. ϕ is represented as

[00008] ϕ = e - i 2 π λ nl ,

where n and I are the complex refractive index and the thickness, respectively, and A is the wavelength of the EMWs propagating in free space.

[0121] From equation 12, the reflection and transmission coefficients are calculated as below:

[00009] R = - c d and T = a - bc d ( 14 )

[0122] Therefore, using equation 14, SE.sub.T, SE.sub.R and SE.sub.A can be expressed as below:

[00010] SE T = 10 log ( 1 T ) = 10 log ( 1 .Math. t .Math. 2 ) ( 15 ) SE R = 10 log ( 1 1 - R ) = 10 log ( 1 1 - .Math. r .Math. 2 ) ( 16 ) SE A = SE T - SE R ( 17 )

Example 3 Analysis Results

Example 3.1 Structural Characterization of MAX and MXene

[0123] As in the above example 1, Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes were synthesized by chemical etching of the Al atoms from their parent MAX phases, Ti.sub.3AlCN and Ti.sub.3AlC.sub.2, respectively, and XRD patterns of the parent MAX phases and the corresponding MXenes are shown in FIG. 1B. Ti.sub.3AlC.sub.2 was a single-phase M.sub.3AX.sub.2, whereas the Ti.sub.3AlCN contained traces of M.sub.4AX.sub.3 and M.sub.2AX phases, which were below detection limit after etching and delamination. The characteristic (002) peak shifted towards the lower angle with the absence of non-basal plane peaks of MAX phases confirming their complete etching and delamination to Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes. FIG. 10 shows a TEM image of monolayer Ti.sub.3CNT.sub.x MXene flake with the selected area electron diffraction (SAED) pattern in the inset. It was found in FIG. 10 that the 2D flake retained the crystallinity and hexagonal structure of the carbonitride layers. FIG. 1D shows an optical image of dilute aqueous dispersions of Ti.sub.3CNT.sub.x (left) and Ti.sub.3C.sub.2T.sub.x (right) MXenes. Ti.sub.3CNT.sub.x MXene showed dark grey color, while green or green tinted black was observed in Ti.sub.3C.sub.2T.sub.x MXene.

Example 3.2 Fabrication of Free-Standing Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Films, Annealing the Same, and Structural Characterization of the Same

[0124] Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x free-standing films of different thickness were fabricated via vacuum-assisted filtration of aqueous suspensions of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes, respectively, followed by annealing at different temperatures of 150° C., 250° C. and 350° C. for 6 hours under an argon atmosphere. Structural changes in Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films under thermal annealing were analyzed by XRD as shown in FIGS. 1E and 1F, respectively. The (002) peak of the Ti.sub.3CNT.sub.x gradually shifts from 5.76° for the as-synthesized (room temperature) film to higher angles of 6.3°, 6.76° and 7.1° for the films annealed at 150° C., 250° C. and 350° C., respectively. Additionally, as shown in FIG. 1G, the d-spacing of the MXene films gradually decreases from 1.36 nm (room temperature) to 1.34 nm, 1.27 nm and 1.21 nm with increasing annealing temperature. Ti.sub.3C.sub.2T.sub.x also shows similar changes in the d-spacing on annealing. However, it can be seen from FIG. 1G that the d-spacing for Ti.sub.3CNT.sub.x MXene film remains larger than the d-spacing of Ti.sub.3C.sub.2T.sub.x MXene film at the same annealing temperature. The decrement in d-spacing is due to the removal of intercalated water and hydroxyl surface terminations at elevated temperatures. It was found that even though the d-spacing reduced with increasing annealing temperature, the pore size and pore volume gradually increased with temperature annealing temperature. Additionally, unlike Ti.sub.3C.sub.2T.sub.x, Ti.sub.3CNT.sub.x MXene films reveal a small TiO.sub.2 peak of (101) plane after annealing at 350° C., indicating partial surface oxidation of the films (FIG. 1E). As the temperature increases, severer oxidation occurs and the properties of Ti.sub.3CNT.sub.x films greatly degrade. FIGS. 2A to 2C and FIGS. 3A to 3C show the analysis results of thermal stability of Ti.sub.3CNT.sub.x (FIGS. 2A to 2C) and Ti.sub.3C.sub.2T.sub.x MXenes (FIGS. 3A to 3C). The distorted SAED pattern in the lower drawing of FIG. 2C arises from TiO.sub.2 nanocrystals formed on the surface of Ti.sub.3CNT.sub.x MXene flakes, and it confirmed the partial oxidation of MXene film surface.

Example 3.3 Thermogravimetric Analysis of Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Film

[0125] FIGS. 4A and 4B show the thermogravimetric analysis results coupled with the mass spectroscopy (TGA-MS) results of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXenes, respectively. Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x exhibit a strong and broad peak at the mass to charge ratio (m/z) of 18 caused by the removal of absorbed water, and a strong peak at the m/z value of 17, representing the removal of the hydroxyl ion. The results indicate that pristine Ti.sub.3CNT.sub.x exhibits a larger weight loss of ˜6% as compared to only ˜2% in Ti.sub.3C.sub.2T.sub.x, indicating that Ti.sub.3CNT.sub.x holds a larger content of water compared to Ti.sub.3C.sub.2T.sub.x. Unlike Ti.sub.3C.sub.2T.sub.x, Ti.sub.3CNT.sub.x reveals a small signal of m/z=44 attributed to the evolution of CO.sub.2 above 300° C., indicating that Ti.sub.3CNT.sub.x is less resistive to oxidation than Ti.sub.3C.sub.2T.sub.x at high temperatures. These results are consistent with the results of FIGS. 2A to 2C and FIGS. 3A to 3C.

Example 3.4 Structural Analysis of Annealed Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Film

[0126] X-ray photoelectron spectroscopy (XPS) survey spectra before thermal annealing (FIG. 5A) exhibit an N peak in addition to the peaks for Ti, C, F, O and Cl elements, which originate from the titanium carbonitride structure of Ti.sub.3CNT.sub.x with surface terminations. On the other hand, according to FIG. 5B, XPS survey spectra for Ti.sub.3C.sub.2T.sub.x have no N peak, showing the absence of nitrogen. High resolution XPS spectra of Ti2p and O1 s of Ti.sub.3CNT.sub.x annealed at different temperatures (150° C., 250° C., 350° C.) are shown in FIGS. 6A and 6B, and reveal that the Ti—OH content decreases with increasing the annealing temperature up to 300° C. but further increase in temperature initiate surface oxidation, resulting in the growth of TiO.sub.2 nanocrystals at 350° C. In contrast, Ti.sub.3C.sub.2T.sub.x films did not show the formation of TiO.sub.2 crystals under identical annealing conditions (FIGS. 7A and 7B). These results are in good agreement with XRD and TEM analysis results.

[0127] FIG. 8A shows a cross-sectional TEM image of Ti.sub.3CNT.sub.x film annealed at 350° C., coupled with energy dispersive spectroscopy (EDS) mapping. FIG. 8A reveals that oxidation occurred only in a very thin surface layer and should have a little effect on electrical conductivity measurement. HRTEM image of the surface part of the film depicts a lattice d-spacing of 0.352 nm assigned to (101) plane of anatase TiO.sub.2 due to oxidation (FIG. 8B), whereas the inner part of the film (FIG. 8C) shows no oxidation and sustains the layered morphology with d-spacing value of 1.21 nm which is consistent with the XRD data in FIG. 1G.

Example 3.5 Cross-Sectional Morphology of Annealed Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Film

[0128] Cross-sectional high-resolution TEM (HRTEM) images show structural changes in 40-μm-thick Ti.sub.3CNT.sub.x film as a function of annealing temperature (FIGS. 9A to 9D). The low magnification scanning electron microscopy (SEM) images in FIGS. 10A to 10D provide morphological changes more clearly. As shown in FIGS. 9A and 10A, the as-prepared (room temperature) Ti.sub.3CNT.sub.x film shows a compact and well-aligned laminate morphology. In contrast, as shown in FIGS. 9B to 9D and FIGS. 10B to 10D, slit pores were developed in the annealed films with a broad size distribution ranging from tens of nanometers to micrometers, and the pore size and pore volume rapidly increase with the annealing temperature. According to FIGS. 11A to 11D, Ti.sub.3C.sub.2T.sub.x also exhibits similar pore generation behavior in the annealed samples, but the pore size and pore volume is much smaller than Ti.sub.3CNT.sub.x films at the same temperature.

[0129] As shown in FIG. 12, at the film thickness of 40 μm, the porosity increases with annealing temperature and this effect is much larger in the case of Ti.sub.3CNT.sub.x films compared to Ti.sub.3C.sub.2T.sub.x. The pores are mainly generated by the loss of intercalated water and the loosely-absorbed molecules on the surface as well as the hydroxyl terminal groups for both Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x as observed in FIGS. 4A and 4B. The larger pore size and porosity of Ti.sub.3CNT.sub.x films are due to the larger amount of intercalated water compared to Ti.sub.3C.sub.2T.sub.x films under the same condition as suggested by TGA-MS result.

[0130] The porosity also depends on the initial thickness of the films annealed at fixed temperature of 350° C. as shown in FIGS. 13A to 13D and FIG. 14. The larger porosity in thicker film is attributed to the fact that larger amounts of gaseous compounds generated during heat treatment are entrapped in the film because of difficulty in escaping from the thick and compact laminate structure, resulting in creation of larger pores and localized ruptures in the thicker laminates.

Example 3.6 Electrical Conductivity of Annealed Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Film

[0131] FIG. 15 shows the electrical conductivity of Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x MXene films before and after annealing. As shown in FIG. 15, as-synthesized (room temperature) Ti.sub.3CNT.sub.x has an average electrical conductivity of 1125 S/cm which gradually increases with annealing temperature and reaches a maximum value of 2475 S/cm at 250° C. which is 120% higher than that of as-synthesized films. This increase in electrical conductivity is due to the removal of intercalated water and other molecules leading to the reduction in interlayer spacing in the annealed samples. The reduced d-spacing decreases the inter-flake resistance between MXene sheets to facilitate electron conduction. A further increase in annealing temperature above 250° C. results in some decrease in conductivity to 1786 S/cm at 350° C. primarily because of increasing pore volume.

[0132] On the contrary, Ti.sub.3C.sub.2T.sub.x films showed a monotonous increment in electrical conductivity from 4500 to 5225 S/cm with increasing annealing temperature, indicating that Ti.sub.3C.sub.2T.sub.x films are more stable and develop less porosity as compared to Ti.sub.3CNT.sub.x films.

Example 3.7 EMI Shielding of Annealed Ti.SUB.3.CNT.SUB.x .and Ti.SUB.3.C.SUB.2.T.SUB.x .MXene Film

[0133] FIGS. 16A and 16B show the total EMI shielding effectiveness (SE.sub.T) of 40 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x films in the X-band frequency range after annealing at various temperatures. The shielding effectiveness values due to reflection (SE.sub.R) and absorption (SE.sub.A) for both MXenes are shown in FIGS. 16C to 16F. As shown in FIG. 16A, as-synthesized Ti.sub.3CNT.sub.x film without heat treatment shows an SE.sub.T of 61 dB, which dramatically rises to 77 dB, 99 dB and 116 dB at the annealing temperatures of 150° C., 250° C. and 350° C., respectively. In contrast, as shown in FIG. 16B, as-synthesized Ti.sub.3C.sub.2T.sub.x reveals an SE.sub.T of 84 dB, which gradually rises to 87 dB, 92 dB and 93 dB at the annealing temperatures of 150° C., 250° C. and 350° C., respectively.

[0134] FIG. 16G summarizes the absolute shielding effectiveness SE.sub.T, SE.sub.R and SE.sub.A for 40 μm-thick Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x films annealed at various temperatures. The increments in SE.sub.T, SE.sub.R and SE.sub.A values with the increasing film thickness (10 μm, 20 μm, 30 μm, and 40 μm) are expressed as ΔSE.sub.T, ΔSE.sub.R, and ΔSE.sub.A, respectively, as a function of annealing temperature in FIGS. 16H to 16K. ΔSE represents the extent of SE increase after annealing compared with as-synthesized materials.

[0135] It can be seen from FIGS. 16A to 16F that the SE.sub.T and SE.sub.A of Ti.sub.3CNT.sub.x films rapidly increase with increasing annealing temperature, while the SE.sub.r values rarely depend on annealing temperature, and Ti.sub.3C.sub.2T.sub.x films also reveal the same trend as Ti.sub.3CNT.sub.x films. However, it is found that the increment rate in Ti.sub.3C.sub.2T.sub.x is much smaller than that in Ti.sub.3CNT.sub.x at the same annealing conditions. As shown in FIG. 16K, ΔSE.sub.T values for pristine and annealed films of 40 μm thickness after annealing at 350° C. reach 55 dB for Ti.sub.3CNT.sub.x and 9 dB for Ti.sub.3C.sub.2T.sub.x, which are equivalent to 90% and 12.6% improvement in SE.sub.T compared to the as-synthesized materials, respectively.

[0136] The thickness dependences at the annealing temperature of 350° C. are shown in FIGS. 17A to 17F. The temperature dependences of ΔSE for the samples with different thicknesses (as shown in FIG. 17G, each 10, 20, 30 and 40 μm) follow the same trend for both MXenes, Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x. However, at the same annealing temperature, as the sample thickness increases from 10 μm to 40 μm, in the case of Ti.sub.3CNT.sub.x, ΔSE.sub.T increases substantially from 31.6 dB to 54.7 dB, while in the case of Ti.sub.3C.sub.2T.sub.x, ΔSE.sub.T just slightly increases from 6.0 dB to 8.6 dB. A difference in ΔSE.sub.T between Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x films becomes larger with increasing sample thickness. As a result, it can be seen that even though the as-synthesized Ti.sub.3CNT.sub.x films always have smaller SE.sub.T and SE.sub.A values than the as-synthesized Ti.sub.3C.sub.2T.sub.x films, the annealed Ti.sub.3CNT.sub.x films have larger SE.sub.T and SE.sub.A values than the annealed Ti.sub.3C.sub.2T.sub.x films. It can notably be seen that the enhancement in SE.sub.T and ΔSE.sub.T of Ti.sub.3CNT.sub.x films after annealing or in thicker samples is solely contributed by the SE.sub.A and ΔSE.sub.A since the SE.sub.R values are almost independent of the annealing temperature.

Example 3.8 Influence of Annealing Time on Ti.SUB.3.CNT.SUB.x .MXene Film

[0137] FIGS. 18A to 18F show the absolute shielding effectiveness SE.sub.T, SE.sub.R, and SE.sub.A, and electrical conductivity (FIG. 18A), XRD patterns (FIG. 18B), induced porosity in the film (FIG. 18C), EMI SE.sub.T (FIG. 18D), EMI SE.sub.R (FIG. 18E) and EMI SE.sub.A (FIG. 18F) of 40 μm-thick Ti.sub.3CNT.sub.x MXene films annealed at 350° C. for different times, respectively. As shown in FIGS. 18A to 18F, the annealing time also strongly affects the structure and shielding performance of Ti.sub.3CNT.sub.x films. After annealing at 350° C. for 1 hour, the electrical conductivity of Ti.sub.3CNT.sub.x film increases from 1125 S/cm to 2520 S/cm and gradually decreases until reaching 512 S/cm (FIG. 18A) in 24 hours, and this is caused by excessive oxidation (FIG. 18B). The EMI SE of Ti.sub.3CNT.sub.x film also shows a similar tendency. However, when the electrical conductivity value is 1786 S/cm through appropriate oxidation after 6 hour-annealing, highest EMI SE of 116 dB is shown (FIG. 18D), confirming that 2D materials do not have a monotonous increment in EMI SE with increasing conductivity. Due to the saturated pore volume of all the samples treated at 350° C. for the annealing time of the range shown in FIG. 18C, all the annealed films showed similar SE.sub.R values (FIG. 18E), but they had a significant increase in SE.sub.A until the annealing time of up to 6 hours (FIG. 18F), showing extraordinarily improved absorption of electromagnetic waves.

Example 3.9 EMI Shielding Mechanism of Ti.SUB.3.CNT.SUB.x .MXene Film

[0138] The dramatic increase in SE.sub.A as shown in FIG. 18F can partially be attributed to the improved electrical conductivity, induced porosity and dipolar polarizations in the annealed Ti.sub.3CNT.sub.x laminate films. SE.sub.A is strongly proportional to the electrical conductivity, which is responsible for the rapid exponential decay in the strength of incoming EMWs in the form of heat due to resistance (ohmic) and eddy current losses (Equation 9). The porous structure provides extra interfaces for internal reflections that extend the path length of the EM wave during propagation in the film before transmission and provide a higher chance to interact with EMWs, resulting in extra attenuation by absorption (Equations 13 and 14). The remaining surface terminations residing on the Ti.sub.3CNT.sub.x surface and formation of dielectric TiO.sub.2 may also contribute to the enhanced absorption of EMWs by generating dipole polarization losses within the shield. On the contrary, reflection contribution SE.sub.R changes depending on electrical conductivity log (Equation 8), and in this case, the changes are very small. Accordingly, the SE.sub.R values of the two MXenes, Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x, show negligible changes after thermal annealing.

[0139] The Ti.sub.3CNT.sub.x film annealed at 350° C. has much larger EMI SE.sub.A and SE.sub.T than the Ti.sub.3CNT.sub.x film annealed at 250° C. despite its lower electrical conductivity. Moreover, the Ti.sub.3CNT.sub.x film annealed at 350° C. has much larger EMI SE.sub.A and SE.sub.T than the Ti.sub.3C.sub.2T.sub.x film annealed at the same temperature, which has a much larger electrical conductivity. These results suggest a possible role of the induced porous structure coupled with partial oxidation in enhancing the electromagnetic absorption shielding efficiency, but a quantum mechanical approach is required for interaction of EMWs with nanometer-thin 2D metals, like MXenes, where macroscopic theories cannot be used.

[0140] The experimental SE.sub.T, SE.sub.E, and SE.sub.A results for Ti.sub.3CNT.sub.x and Ti.sub.3C.sub.2T.sub.x laminate films are compared with the theoretical calculations by the transfer matrix method (for data consistency, see FIG. 19) to investigate the effect of porosity (FIGS. 20A to 20C and FIGS. 21A to 21C). In the experimental data, each data point represents different annealing temperatures. The calculations assume that MXene films have the perfect laminate structure of 2D MXene sheets with infinite sheet area, and the effect of conductivity and porosity of perfect laminate structures were simultaneously considered. According to the calculations, as the conductivity and porosity increase, each of SE.sub.T and SE.sub.A increases, but SE.sub.R hardly changes. As shown in FIGS. 20A and 21A, the experimental SE.sub.T value of the as-synthesized (room temperature) Ti.sub.3CNT.sub.x without heat treatment qualitatively agrees with the theoretical value in the same way as SE.sub.T, SE.sub.E, and SE.sub.A of the as-synthesized (room temperature) and heat-treated Ti.sub.3C.sub.2T.sub.x films. However, after annealing, a mismatch between experimental and theoretical SE.sub.T values of Ti.sub.3CNT.sub.x MXene occurs and becomes more pronounced as the annealing temperature increases. Similarly, as shown in FIG. 20C, SE.sub.A values of Ti.sub.3CNT.sub.x MXene also show a considerable mismatch between experimental and theoretical values at higher annealing temperatures, whereas as shown in FIG. 20B, all the experimental SE.sub.R values are consistent with the theoretical calculations. This indicates that the mismatch in SE.sub.T is because of the mismatch in SE.sub.A, which originates from the unexpectedly large improvement in electromagnetic absorption shielding efficiency after annealing at high temperatures. This again stresses the limitations of traditional models and need for atomistic simulations.

[0141] The failure of theoretical prediction of the EMI shielding behavior of the annealed Ti.sub.3CNT.sub.x films indicates that in addition to electrical conductivity and induced porosity, dipolar polarizations and low order of magnitude of MXenes should be considered. In particular, extraordinarily large absorption of annealed Ti.sub.3CNT.sub.x films may be caused by the formation of similar structures to metamaterials from atomically thin MXene sheets after annealing. When loss components of effective dielectric constant and electromagnetic permeability of metamaterials increase, the absorption of electromagnetic radiation is improved. Accordingly, further studies are needed to understand the particular shielding mechanism of Ti.sub.3CNT.sub.x responsible for experimentally observed large absorption ability of the annealed Ti.sub.3CNT.sub.x samples.

[0142] The comparison results of EMI SE.sub.T of Ti.sub.3CNT.sub.x films with the values reported in previous studies are shown in FIG. 22 and Table 1 below. Metal-based and carbon-based materials have been on the forefront in the last decade, and in this instance, SE in excess of 50 dB for a thickness between 50 to 100 μm has been considered sufficient for EMI shielding applications. However, difficulties in processing metals into high density thin films limit the use in high-tech mobile applications. The carbon-based materials having low electrical conductivity are difficult to process them to a small thickness and can only provide shielding efficiency. In contrast, as shown in FIG. 22 and Table 1 below, the heat-treated 40 μm-thick Ti.sub.3CNT.sub.x MXene films show absorption dominant EMI SE of 116 dB, well above all materials produced to date, showing its strong potential for EMI shielding and related applications.

TABLE-US-00001 TABLE 1 Filler Thickness EMI SE Type Filler [wt. %] Matrix [cm] [dB] Ref Graphene and graphite Graphene Bulk / 0.005 60 1 Graphene Bulk / 8.40 × 10.sup.−4 20 2 Graphene(annealed) Bulk / 0.006 90 3 Graphene/CNTs Bulk / 0.16 38 4 Graphene/CNTs Bulk / 0.16 36 5 rGO 7 PS 0.25 45.1 6 rGO 30 PS 0.25 29 7 rGO 25 PEDOT:PSS 0.08 70 8 rGO 3.07 PDMS 0.2 54.2 9 Graphene 0.8 PDMS 0.1 20 10 rGO/Fe3O4 10 PEI 0.25 18 11 rGO 10 PEI 0.23 12.8 12 rGO 16 PI 0.08 21 13 rGO 1 PU 0.25 23 14 rGO 3 Epoxy 0.1 38 15 rGO/Fe.sub.3O.sub.4 Bulk / 0.03 24 16 PEDOT:PSS 4.6 rGO 0.15 91.9 17 EG 98 HANF 0.006 60.4 18 90 0.006 47.4 Carbon (fibres/nanotubes) Carbon / Bulk 1 51 19 Carbon / PN resin 0.2 51.2 20 Carbon foam / Bulk 0.2 40 21 CB 15 ABS 0.11 20 22 SWCNT 30 MWCNT 0.013 65 23 SWCNT 15 Epoxy 0.1 20 24 SWCNT 7 PS 0.12 18.5 25 MWCNT 25 MCMB 0.06 56 26 MWCNT 15 ABS 0.11 50 22 MWCNT 20 PC 0.21 39 27 MWCNT 20 PS 0.2 30 28 MWCNT 76.2 WPU 0.1 21.1 29 CNT 20 rGO 0.0015 57.6 30 CNT sponge 1 PDMS 0.18 54.8 31 Metals Al Foil Bulk / 0.80 × 10.sup.−3 66 32 Cu Foil 0.001 70 CuNi Bulk / 0.15 25 33 CuNi-CNT 0.15 54.6 Copper Bulk / 0.31 90 34 Cu coated beads / PCL 0.2 110 35 Ni filament 7 PES 0.285 86.6 36 Ag nanowire 67 Carbon 0.3 70.1 37 Ag nanowire 28.6 WPU 0.23 64 38 Ag nanowire 4.5 PI 0.5 35 39 Ag nanowire 4.5 PI 0.5 35 1 Ag nanofiber / Bulk 0.01 76 40 0.10 × 10.sup.−3 20 SS Bulk / 0.4 89 36 SS 1.1 PP 0.31 48 34 Others Carbon Foam Bulk / 0.2 51.2 41 Carbon Foam Bulk / 0.2 40 21 Flexible graphite Bulk / 0.31 130 42 0.079 102 MoS.sub.2 30 Glass 0.15 24.2 43 rGO/y-Fe.sub.2O.sub.3 75 PANI 0.25 51 44 rGO/Fe.sub.3O.sub.4 66 PANI 0.25 30 45 rGO/Fe.sub.3O.sub.4 Bulk / 0.025 24 16 rGO/CNT/Fe.sub.3O.sub.4 Bulk / 0.2 37.5 46 rGO-BaTiO.sub.3 Bulk / 0.15 41.7 47 MXenes (literature data) Ti.sub.3C.sub.2T.sub.x film Bulk / 0.15 × 10.sup.−3 48 32 0.25 × 10.sup.−3 54 0.60 × 10.sup.−3 59 1.12 × 10.sup.−3 68 2.15 × 10.sup.−3 78  4.0 × 10.sup.−3 87 4.50 × 10.sup.−3 92 Ti.sub.3C.sub.2T.sub.x film 90 SA 0.80 × 10.sup.−3 57 32 Mo.sub.2Ti.sub.2C.sub.3T.sub.x film Bulk / 0.25 × 10.sup.−3 26 32 Mo.sub.2TiC.sub.2T.sub.x film 0.25 × 10.sup.−3 23 MXene foam Bulk / 6.00 × 10.sup.−3 70 48 1.80 × 10.sup.−3 50 0.60 × 10.sup.−3 32 Ti.sub.3C.sub.2T.sub.x 50 cellulose 16.7 × 10.sup.−3 25 49 80 7.40 × 10.sup.−3 26 90 4.70 × 10.sup.−3 24 TiO.sub.2-Ti.sub.3C.sub.2/graphene / / 9.17 × 10.sup.−4 27 50 7.82 × 10.sup.−4 23.4 5.59 × 10.sup.−4 23.3 5.25 × 10.sup.−4 18 Ti.sub.3C.sub.2/SWONT / PVA/PSS 2.07 × 10.sup.−5 3.39 51 Ti.sub.3C.sub.2/MWCNT 1.70 × 10.sup.−5 2.81 Ti.sub.3C.sub.2T.sub.x aerogel Bulk 0.10 44.8 52 Ti.sub.2CT.sub.x aerogel / 0.10 48.5 Ti.sub.3CNT.sub.x aerogel 0.10 42.3 Ti.sub.2CT.sub.x Bulk /  1.1 × 10.sup.−3 50 53 V.sub.2CT.sub.x /  1.2 × 10.sup.−3 46 Nb.sub.2CT.sub.x /  1.0 × 10.sup.−3 15 Ti.sub.yNb.sub.2-yCT.sub.x /  1.4 × 10.sup.−3 50 Nb.sub.yV.sub.2-yCT.sub.x /  1.2 × 10.sup.−3 36 Ti.sub.3C.sub.2T.sub.x /  1.4 × 10.sup.−3 70 Ti.sub.3CNT.sub.x /  1.0 × 10.sup.−3 55 Mo.sub.2TiC.sub.2T.sub.x /  1.0 × 10.sup.−3 21 Nb.sub.4C.sub.3T.sub.x /  1.1 × 10.sup.−3 26 Mo.sub.2Ti.sub.2C.sub.3T.sub.x /  1.3 × 10.sup.−3 37 Ti.sub.3C.sub.2T.sub.x ultrathin film /  5.5 × 10.sup.−6 20 54 nes (this work *Pristine Ti.sub.3CNT.sub.x Bulk / 0.001 43.5 This 0.002 47.9 study 0.003 53.3 0.004 61.4 *Heat-treated Bulk / 0.001 75.1 Ti.sub.3CNT.sub.x 0.002 83.0 0.003 97.1 0.004 116.2 *Pristine Ti.sub.3C.sub.2T.sub.x Bulk / 0.001 66.5 0.002 74.6 0.003 77.9 0.004 83.5 *Heat-treated Ti.sub.3C.sub.2T.sub.x Bulk / 0.001 74.1 0.002 81.1 0.003 85.2 0.004 93.0 *CNT: carbon nanotube; rGO: reduced graphene oxide; EG: expanded graphite; CB: carbon black; SWCNT: single-wall carbon nanotube; MWCNT: multi-wall carbon nanotube; PS: polystyrene; PEDOT:PSS: poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate); PEI: polyethylenimine; PI: polyimide; PU: polyurethane; WPU: water-borne polyurethane; HANF: hydrated aramid nanofiber; MCMB: meso-carbon microbead; ABS: acrylonitrile-butadiene-styrene; PDMS; polydimethylsiloxane; PCL: poly(c-caprolactone); PES: polyethersulfone; PP: polypropylene; PANI: polyaniline; PN resin: phthalonitrile resin; PC: polycarbonate; PVA/PSS: poly(vinyl alcohol)/poly(sodium 4-styrene sulfonate); SS: stainless steel; SA: sodium alginate.

Example 3.10 Dimensional Stability of Ti.SUB.3.CNT.SUB.x .MXene Film

[0143] FIG. 23A shows the dimensional stability of Ti.sub.3CNT.sub.x film before annealing, and FIG. 23B shows the dimensional stability of Ti.sub.3CNT.sub.x MXene film annealed at 350° C. FIG. 23C shows the dimensional stability and adhesive strength of Ti.sub.3CNT.sub.x MXene film spray-coated on the glass substrate before annealing, and FIG. 23D shows the dimensional stability and adhesive strength of Ti.sub.3CNT.sub.x MXene film spray-coated on the glass substrate, annealed at 350° C. FIG. 23E shows the mechanical flexibility of Ti.sub.3CNT.sub.x MXene film before annealing, and FIG. 23F shows the mechanical flexibility of Ti.sub.3CNT.sub.x MXene film annealed at 350° C.

[0144] It can be seen from FIGS. 23A to 23F that the annealed Ti.sub.3CNT.sub.x MXene films have low weight and high EMI SE as well as sufficient mechanical strength and flexibility. It is expected that dimensional stability and good adhesion of the annealed Ti.sub.3CNT.sub.x MXene films guarantees the possibility of post-processing heat treatment for thermally stable systems and will be promising in the applications of high-tech flexible mobile electronic devices due to sufficient mechanical flexibility.