Supplementary Figure 1. Schematic representation of (Mo2/3Sc1/3)2AlC assuming a, Monoclinic (C2/c) and b, orthorhombic (Cmcm) symmetry.
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1 Supplementary Figure 1. Schematic representation of (Mo2/3Sc1/3)2AlC assuming a, Monoclinic (C2/c) and b, orthorhombic (Cmcm) symmetry. Further details of these structures are given in Supplementary Table 2.
2 Supplementary Figure 2. Calculated phonon dispersion of (Mo2/3Sc1/3)2AlC. a, Monoclinic structure with space group C2/c (supercell size of unit cells). b, Orthorhombic structure with space group Cmcm (supercell size of unit cells. 2
3 Supplementary Figure 3. EDX spectrum of (Mo2/3Sc1/3)2AlC before and after etching. Spectrum taken in connection to TEM analysis, showing that both Al and Sc are absent after etching. 3
4 Supplementary Figure 4. XRD pattern for (Mo2/3Sc1/3)2AlC etched with LiF+HCl. The c-lp of Å is slightly larger compared to the one after HF etching (19.4 Å) presumably a result of Li-ion intercalation, as previously shown for Ti3C2 and Mo2C MXenes 1, 2. 4
5 Supplementary Figure 5. Low magnification STEM showing side view of a multilayer Mo1.33C MXene flake. Scale bar corresponds to 10 µm. 5
6 Supplementary Figure 6. SEM image showing cross section of the 3 µm thick d- Mo1.33C paper. Scale bar corresponds to 1 µm. 6
7 Supplementary Figure 7. High-resolution XPS spectra with peak fittings for a, Mo 3d b, C1s c, O1s and d, F 1s. The peak fitting results for various species and the resulting elemental compositions extracted from the high resolution spectra are tabulated in Supplementary Table 4. 7
8 Supplementary Figure 8. Electrochemical performance of Mo 1.33 C in 1 M H SO in a threeelectrode Swagelok cell: Capacitance retention test on 3- m thick Mo1.33C free-standing 2 4 electrode at 10 A g -1. Inset shows voltage vs. time profile for 3 cycles. 8
9 Supplementary Table 1. Phases used in theoretical evaluation of phase stability in quaternary Sc-Mo-Al-C system. Last two entries are the most stable. Phase Prototype structure Pearson symbol Space group V (Å 3 /uc) a (Å) b (Å) c (Å) E 0 (ev/fu) Sc Mg hp2 P6 3/mmc (194) Sc Sc hp6 P6 122 (178) Sc Np tp4 P4/nmm (129) Mo W ci2 Im-3m (229) Mo Cu cf4 Fm-3m (225) Mo Mg hp2 P6 3/mmc (194) Al Cu cf4 Fm-3m (225) Al Mg hp2 P6 3/mmc (194) Al W ci2 Im-3m (229) C C (graphite) hp4 P6 3/mmc (194) Al 4C 3 Al 4C 3 hr21 R-3m h (166) Sc 2Al Ni 2In hp6 P6 3/mmc (194) ScAl CsCl cp2 Pm-3m (221) ScAl CrB oc8 Cmcm (63) ScAl 2 MgCu 2 cf24 Fd-3m (227) ScAl 3 AuCu 3 cp4 Pm-3m (221) MoAl 12 WAl 12 ci26 Im-3 (204) MoAl 5 MoAl 5 hr36 R-3c h (167) Mo 4Al 17 Mo 4Al 17 ms84 C2 (5) Mo 3Al 8 Mo 3Al 8 ms22 C2/m (12) Mo 3Al Cr 3Si cp8 Pm-3n (223) Sc 2C Ti 2C cf48 Fd-3m (227) Sc 4C 3 P 4Th 3 ci28 I-43d (220) ScC NaCl cf8 Fm-3m (225) ScC NaCl cf8 Fm-3m (225) Sc 3C 4 Sc 3C 4 tp70 P4/mnc (128) MoC TiP hp8 P6 3/mmc (194) MoC NaCl cf8 Fm-3m (225)
10 MoC η-moc hp12 P6 3/mmc (194) MoC WC hp2 P-6m2 (187) Mo 3C 2 Cr 3C 2 op20 Pnma (62) Mo 2C β''-mo 2C hp3 P-3m1 (164) Mo 3C Fe 3C op16 Pnma (62) ScAl 3C 3 ScAl 3C 3 hp14 P6 3/mmc (194) Sc 3AlC CaTiO 3 cp5 Pm-3m (221) Sc 2AlC Cr 2AlC hp8 P6 3/mmc (194) Sc 3AlC 2 Ti 3SiC 2 hp12 P6 3/mmc (194) Sc 4AlC 3 Ti 4AlN 3 hp16 P6 3/mmc (194) Mo 3AlC CaTiO 3 cp5 Pm-3m (221) Mo 3Al 2C Mo 3Al 2C cp24 P4 132 (213) Mo 3Al 2C Mo 3Al 2C cp24 P4 132 (213) Mo 3Al 2C Mo 3Al 2C cp24 P4 132 (213) Mo 3Al 2C Mo 3Al 2C cp24 P4 132 (213) Mo 3Al 2C 0.75 Mo 3Al 2C cp24 P4 132 (213) Mo 2AlC Cr 2AlC hp8 P6 3/mmc (194) Mo 3AlC 2 Ti 3SiC 2 hp12 P6 3/mmc (194) Mo 4AlC 3 Ti 4AlN 3 hp16 P6 3/mmc (194) ScMo 2AlC 2 TiCr 2AlC 2 hp12 P6 3/mmc (194) MoSc 2AlC 2 TiCr 2AlC 2 hp12 P6 3/mmc (194) (Mo 2/3Sc 1/3) 2AlC (Mo 2/3Sc 1/3) 2AlC op48 Cmcm (63) (Mo 2/3Sc 1/3) 2AlC (Mo 2/3Sc 1/3) 2AlC ms48 C2/c (15)
11 Supplementary Table 2 Atomic structure and phase stability of (Mo2/3Sc1/3)2AlC assuming monoclinic (C2/c) or orthorhombic (Cmcm) symmetry. Last row lists the phase stability of each structure expressed in formation enthalpy ΔHcp calculated with respect to the identified set of the most competing phases, viz. ScMo2AlC2, Mo3Al, Sc3AlC and Mo3Al8. Space group C2/c (#15) Cmcm (#63) Z 4 4 a (Å) b (Å) c (Å) α β γ Sc 8f ( , , ) 8f (0.00, , ) Mo 8f ( , , ) 8f ( , , ) Al 8f ( , , ) 4e ( ) C 8f ( ) 4d (0.25, 0.25, 0.50) 16h ( , , ) 4c ( , , 0.25) 8g ( , , 0.25) 8e ( , 0.0, 0.0) 4b (0.0, 0.5, 0.0) ΔH cp (mev/atom)
12 Supplementary Table 3 Rietveld refinement of (Mo2/3Sc1/3)2AlC assuming monoclinic (C2/c) symmetry. From the Rietveld refinement of the XRD pattern shown in Fig. 1E the mass fractions of the different phases were: (Mo2/3Sc1/3)2AlC (84.9(5) wt.%), Mo3Al2C (7.5(1) wt.%), Mo3Al (7.1(1) wt.%) and Mo2C (0.5(1) wt.%). The total χ 2 value was 32. Space group C2/c (#15) a (Å) (1) b (Å) (1) c (Å) (2) α β (10) γ Sc 8f (0.9497(8) (17) (3)) Occupancy of Sc = 7.00 and Mo = f (0.2760(3) (10) (1)) Mo Occupancy of Mo = 7.00 and Sc = f (0.6102(4) (10) (1)) Occupancy of Mo = 7.00 and Sc = 1.00 Al C 8f (0.7562(9) (19) (7)) 4e ( (20) ) 8f ( ) 4e ( ) 12
13 Supplementary Table 4 XPS peak fitting of results shown in Supplementary Fig. 7 for d-mo1.33ctx paper. The numbers in brackets in column 2 and 3 are peak locations of Mo 3d3/2 and their full-widths at half maximum, FWHM, respectively. For peak assignment see Ref. 2 and Ref. 3 and references therein. Region BE [ev] a FWHM [ev] Fraction Assigned to Mo 3d 5/2 (3d 3/2) C 1s O 1s F 1s (232.5) 230.9(233.9) (235.2) (0.7) 0.8 (0.8) 1.6 (1.9) C-Mo-T x Mo +5 MoO 3 C-Mo-T x C-C CH x C-O COO MoO 3 C-Mo-O x C-Mo-(OH) x H 2O ads C-Mo-F x AlF 3 a Values in parenthesis correspond to the 3d 3/2 component. 13
14 Supplementary Table 5 Gravimetric capacitance values for two different thickness d-mo1.33c free-standing electrodes tested in a three-electrode Swagelok configuration in 1 M H2SO4. 3 µm-thick film 12 µm-thick film Gravimetric(F g -1 ) Volumetric (F cm -3 ) Gravimetric (F g -1 ) Volumetric (F cm -3 ) 2 mv s mv s mv s mv s mv s mv s mv s mv s mv s
15 Supplementary References 1. Ghidiu, M. et al. Ion-Exchange and Cation Solvation Reactions in Ti 3C 2 MXene. Chem. Mater. 28, (2016). 2. Halim, J. et al. Synthesis and characterization of 2D molybdenum carbide (MXene). Adv. Func. Mater. 26, (2016). 3. Halim, J. et al. X-ray photoelectron spectroscopy of select multi-layered transition metal carbides (MXenes). App. Surf. Sci. 362, (2016). 15
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