4 research outputs found
Al(TFSI)<sub>3</sub> as a Conducting Salt for High-Voltage Electrochemical Double-Layer Capacitors
In
this study, we report for the first time about the use of aluminum
bisÂ(trifluoromethanesulfonyl)Âimide [AlÂ(TFSI)<sub>3</sub>] as conducting
salt for electrochemical double-layer capacitors (EDLCs). We show
that using this salt it is possible to realize highly concentrated
electrolytes, which are able to suppress the anodic dissolution of
the aluminum current collectors. Because of this ability, the use
of this electrolyte makes possible the realization of EDLCs that can
retain 80% of their initial performance after floating for 1500 h
at 3 V (which is comparable to âź5000000 cycles of charge and
discharge at 1 A g<sup>â1</sup>)
Structural Investigations on Lithium-Doped Protic and Aprotic Ionic Liquids
Solutions
of lithium bisÂ(trifluoromethanesulfonyl)Âimide (LiNTf<sub>2</sub>),
in four different [NTf<sub>2</sub>]<sup>â</sup>-based
ionic liquids, are extensively investigated as potential electrolytes
for lithium-ion batteries. Solvation of the [Li]<sup>+</sup> ions
in the ionic liquids and its impact on their physicochemical properties
are studied herein with the aid of molecular dynamics simulations.
The cationic components of the investigated liquids were systematically
varied so as to individually evaluate effects of specific structural
changes; increase in ring size, the addition of an alkyl chain and
absence of an acidic proton, on the solvation and mobility of the
[Li]<sup>+</sup> cations. The studied cations also allow for a direct
comparison between solutions of [Li]<sup>+</sup> salt in protic and
aprotic ionic liquids. Emphasis is laid on elucidating the interactions
between the [Li]<sup>+</sup> and [NTf<sub>2</sub>]<sup>â</sup> ions revealing slightly higher coordination numbers for the aprotic
solvent, benchmarked against experimental measurements. The study
suggests that the ionic liquids largely retain their structure upon
salt addition, with interactions within the liquids only slightly
perturbed. The rattling motion of the [Li]<sup>+</sup> cations within
cages formed by the surrounding [NTf<sub>2</sub>]<sup>â</sup> anions is examined by the analysis of [Li]<sup>+</sup> autocorrelation
functions. Overall, the solvation mechanism of [Li]<sup>+</sup> salt,
within the hydrogen-bonded network of the ionic liquids, is detailed
from classical and <i>ab initio</i> molecular dynamics simulations
Toward New Solvents for EDLCs: From Computational Screening to Electrochemical Validation
The development of innovative electrolytes
is a key aspect of improving
electrochemical double layer capacitors (EDLCs). New solvents, new
conducting salts as well as new ionic liquids need to be considered.
To avoid time-consuming âtrial and errorâ experiments,
it is desirable to ârationalizeâ this search for new
materials. An important step in this direction is the systematic application
of computational screening approaches. Via the fast prediction of
the properties of a large number of compounds, for instance all reasonable
candidates within a given compound class, such approaches should allow
to identify of the most promising candidates for subsequent experiments.
In this work we consider the toy system of all reasonable nitrile
solvents up to 12 heavy atoms. To investigate if our recently proposed
computational screening strategy is a feasible tool for the purpose
of rationalizing the search for new EDLC electrolyte materials, we
correlateî¸in the case of EDLCs for the first timeî¸computational
screening results with experimental findings. For this, experiments
are performed on those compounds for which experimental data is not
available from the literature. We find that our screening approach
is well suited to pick good candidates out of the set of all reasonable
nitriles, comprising almost 5000 compounds
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Insights into Bulk Electrolyte Effects on the Operative Voltage of Electrochemical Double-Layer Capacitors
Electrochemical
double-layer capacitors (EDLCs) are robust, high-power,
and fast-charging energy storage devices. Rational design of novel
electrolyte materials could further improve the performance of EDLCs.
Computational methods offer immense scope in aiding the development
of such materials. Trends in experimentally observed operative voltages
nevertheless remain difficult to predict and understand. We discuss
here the intriguing case of adiponitrile (ADN) versus 2-methyl-glutaronitrile
(2MGN) based electrolytes, which result in very different operative
voltages in EDLCs despite structural similarity. As a preliminary
step, bulk electrolyte effects on electrochemical stability are investigated
by <i>ab initio</i> molecular dynamics (AIMD) and static,
cluster-based quantum chemistry calculations