Alternative Single‐Solvent Electrolytes Based on Cyanoesters for Safer Lithium‐Ion Batteries

Abstract

To identify alternative single-solvent-based electrolytes for application in lithium-ion batteries (LIBs), adequate computational methods were applied to screen specified physicochemical and electrochemical properties of new cyanoester-based compounds. Out of 2747 possible target compounds, two promising candidates and two structurally equivalent components were chosen. A constructive selection process including evaluation of basic physicochemical properties as well assessing the compatibility towards graphitic anodes was initiated to identify the most promising candidates. With addition of a film-forming additive in a low concentration, the most promising candidate showed an adequate long-term cycling stability with LiNi1/3 Mn1/3 Co1/3 O2 [NMC(111)] in a full-cell setup using graphite as anode material. The main advantages of the new electrolyte formulation are related to its good thermal behavior, especially with regard to safety in combination with satisfying electrochemical performance.

Predicting the Solubility of Sulfur: A COSMO‐RS‐Based Approach to Investigate Electrolytes for Li–S Batteries

“…COSMO‐RS combines a quantum chemical (DFT)‐based continuum solvation approach for a single molecule with statistical thermodynamics, and has already proven to be an effective and reliable screening tool in relation to pharmaceutical drugs, industrial separation thermodynamics, and ionic liquids . With regard to Li‐based battery development, and Li‐ion and Li‐air systems in particular, COSMO‐RS has so far mostly been used for screening large datasets (10 2 –10 5 ) of small molecules as potential electrolyte solvents . Basic electronic properties, such as ionization potentials and electron affinities, as well as physicochemical properties, such as viscosity and melting and boiling temperatures, were assessed as selection criteria.…”

“…With regard to Li‐based battery development, and Li‐ion and Li‐air systems in particular, COSMO‐RS has so far mostly been used for screening large datasets (10 2 –10 5 ) of small molecules as potential electrolyte solvents . Basic electronic properties, such as ionization potentials and electron affinities, as well as physicochemical properties, such as viscosity and melting and boiling temperatures, were assessed as selection criteria. The predictions have provided a sufficient qualitative ranking for a multi‐level approach or have been used in quantitative structure–property relationship (QSPR)‐based methods to find new electrolytes.…”

“…Basic electronic properties, such as ionization potentials and electron affinities, as well as physicochemical properties, such as viscosity and melting and boiling temperatures, were assessed as selection criteria. The predictions have provided a sufficient qualitative ranking for a multi‐level approach or have been used in quantitative structure–property relationship (QSPR)‐based methods to find new electrolytes.…”

Review of Electrolyte Additives for Ternary Cathode Lithium-ion Battery

“…其中 ECH 结构中引入烷氧基, 进一步提高其离子电导率. 随 后, 一系列烷氧基取代腈也被相继提出, 如 3MPN、 AND (78～79, 图 17) [43] 、MCA (80, 图 17) [183] 及 EGBE (81, 图 17) [ Figure 16 (a) Cathodic, when the functional group ''X'' in α-position to the vinylene group is electron-withdrawing, reduction induced polymerization of vinylene monomers is facilitated; (b) anodic, when the functional group ''Y'' in α-position to the vinylene group is electron-pushing, oxidation induced polymerization of vinylene monomers is promoted [178] 向腈类结构引入其它官能团, 可提高腈类电解液的 适用性. Liu 等 [189] 将-CN 替换为异氰酸, 得到 HDI (82, …”

Innovative, Non‐Corrosive LiTFSI Cyanoester‐Based Electrolyte for Safer 4 V Lithium‐Ion Batteries

“…In a recent publication, we disclosed the problems arising from the remote thermal safety properties of cyclic and linear organic carbonate‐based electrolytes. Subsequently, we suggested the utilization of an alternative solvent, namely methyl 3‐cyanopropanoate (MCP), as it significantly improves thermal properties of the LiPF 6 ‐based electrolyte . Even though LiPF 6 is the conducting salt of choice for LIBs in SOTA electrolytes, there are many drawbacks associated with its usage, including its low thermal stability, high instability towards water, and subsequent release of toxic and highly reactive decomposition products such as HF, PF 5 , or POF 3 as well as numerous organophosphates .…”