Motivated
by the presence of metallic conductivity in the group
VI transition metal dichalcogenides, the supercapacitive performance
of the 1T phase of molybdenum (MoS2x
Se2(1–x)) sulfoselenides is explored.
Ultrahigh frequency response (∼1.4 kHz) along with excellent
electrochemical stability are exhibited by 1T MoS2x
Se2(1–x)-based supercapacitors.
The S:Se ratio in the mixed chalcogenide is shown to influence the
rate performance of the device. High areal capacitances of ∼450
μF cm–2 with short RC time
constants of ∼1.3–3.2 ms at 120 Hz are achieved in the
case of 1T MoSSe phase. The i–v characteristics are almost rectangular at very high scan rates of
∼1000 V s–1. Very stable gravimetric specific
capacitance of ∼36 F g–1 is retained for
several thousands of charge–discharge cycles leading to an
energy density of ∼12.1 Wh kg–1 at a specific
power of ∼842 W kg–1. The observed specific
power of ∼50 kW kg–1 at ∼1.5 Wh kg–1 energy density makes the sulfoselenide phase capacitors
attractive for high power applications without compromising on the
energy density.
We report on a systematic study of the structural, magnetic and transport properties of highpurity 1T-VS 2 powder samples prepared under high pressure. The results differ notably from those previously obtained by de-intercalating Li from LiVS 2 . First, no Charge Density Wave (CDW) is found by transmission electron microscopy down to 94 K. Though, ab initio phonon calculations unveil a latent CDW instability driven by an acoustic phonon softening at the wave vector q CDW ≈ (0.21,0.21,0) previously reported in de-intercalated samples. A further indication of latent lattice instability is given by an anomalous expansion of the V-S bond distance at low temperature.Second, infrared optical absorption and electrical resistivity measurements give evidence of non metallic properties, consistent with the observation of no CDW phase. On the other hand, magnetic susceptibility and NMR data suggest the coexistence of localized moments with metallic carriers, in agreement with ab initio band structure calculations. This discrepancy is reconciled by a picture of electron localization induced by disorder or electronic correlations leading to a phase separation of metallic and non-metallic domains in the nm scale. We conclude that 1T-VS 2 is at the verge of a CDW transition and suggest that residual electronic doping in Li de-intercalated samples stabilizes a uniform CDW phase with metallic properties.
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