Electron Paramagnetic Resonance Monitoring of Predegradation Radical Generation in a Lithium Electrolyte.

Herein we present an innovative EPR spectroscopy approach complemented with computational modeling as a methodology for assessing a nonaqueous electrolyte behavior just before its massive degradation. As a proof of concept, we use the conventional lithium electrolyte (1 M LiPF in EC/DMC), which is utilized in current lithium-ion batteries. Through EPR, long-lived EC associates in amounts of 10-250 ppm were detected in a broad potential window (>2.

Molecular Engineering of Quinone-Based Nickel Complexes and Polymers for All-Organic Li-Ion Batteries.

All-organic Li-ion batteries appear to be a sustainable and safer alternative to the currently-used Li-ion batteries but their application is still limited due to the lack of organic compounds with high redox potentials toward Li/Li. Herein, we report a computational design of nickel complexes and coordination polymers that have redox potentials spanning the full voltage range: from the highest, 4.7 V, to the lowest, 0.

Redox Hyperactive MOF for Li, Na and Mg Storage.

To create both greener and high-power metal-ion batteries, it is of prime importance to invent an unprecedented electrode material that will be able to store a colossal amount of charge carriers by a redox mechanism. Employing periodic DFT calculations, we modeled a new metal-organic framework, which displays energy density exceeding that of conventional inorganic and organic electrodes, such as Li- and Na-rich oxides and anthraquinones. The designed MOF has a rhombohedral unit cell in which an Ni(II) node is coordinated by 2,5-dicyano--benzoquinone linkers in such a way that all components participate in the redox reaction upon lithiation, sodiation and magnesiation.

Rivalry at the Interface: Ion Desolvation and Electrolyte Degradation in Model Ethylene Carbonate Complexes of Li, Na, and Mg with PF on the LiTiO (111) Surface.

Spinel lithium titanate, LiTiO (LTO), emerges as a "universal" electrode material for Li-ion batteries and hybrid Li/Na-, Li/Mg-, and Na/Mg-ion batteries functioning on the basis of intercalation. Given that LTO operates in a variety of electrolyte solutions, the main challenge is to understand the reactivity of the LTO surface toward single- and dual-cation electrolytes at the molecular level. This study first reports results on ion desolvation and electrolyte solvent/salt degradation on an LTO surface by means of periodic DFT calculations.

Dual-Metal Electrolytes for Hybrid-Ion Batteries: Synergism or Antagonism?

The construction of hybrid metal-ion batteries faces a plethora of challenges. A critical one is to unveil the solvation/desolvation processes at the molecular level in electrolytes that ensure efficient transfer of several types of charge carriers. This study reports first results on simulations of mixed-ion electrolytes.