“Tri-Solvent-in-Salt” Electrolytes for High-Performance Supercapacitors
Bibliographic record
Abstract
Electrolytes chemistry for high-performance supercapacitors (SCs) has been addressed recently, where solvents included in electrolyte composition dissolving or mixing the electrochemically active salts or ILs have been typically seen as a mere medium.[1] Specifically, attention regarding the achievement of high-performacne SCs has also been paid to, e.g., water-in-salt (WIS), solvent-in-salt (SIS), and bi-solvent-in-salt (BSIS) electrolytes, demonstrating that solvent molecules may indeed play a more active role.[2 - 4] In this presentation, we will talk about the design of a tri-solvent-in-salt (TSIS) electrolyte where every solvent contributed (with an IL, i.e., EMIMBF4) to the formation of an electrochemically active hydrogen bond (HB) complex structure. Raman and NMR spectroscopies, as well as molecular dynamic (MD) simulations, helped elucidate the ratio among all compounds (e.g., solvents and IL) in the HB complex structure that best works as an electrolyte. For instance, the eutectic mixture of H2O and dimethylsulfoxide (DMSO) in a 2 to 1 molar ratio primary HB complex structures with mixed EMIMBF4 offers a low melting point and low flammability, then add acetonitrile (CH3CN) in different molar ratios providing an improvement of the rate capability to the resulting electrolyte. As compared to other electrolytes, the TSIS electrolyte composed in a molality of 5.8 m (TSIS-5.8) showed the cost efficiency and exhibited a low self-extinction rate. Moreover, SCs operating with TSIS-5.8, at -70 °C and up to 2.7 V provided energy densities of ca. 49 and 18 Wh kg-1, respectively, power densities of 10,000 and 17,000 W kg-1, the capacitance retention of ca. 82% after 15,000 cycles at 4 A g-1 and a self-discharge as low as 22%. The use of ternary solvent mixtures combining different solvents in the proper molar ratios opens up an easy and low-cost path to design many new electrolytes in terms of non-flammability, non-toxicity, high electrical conductivity, and wide electrochemical stability window (ESW). Forthcoming research could use the knowledge provided by this work in terms of ions solvation and transport in TSIS electrolytes and explore the interfacial interactions between electrolyte and electrode material to determine their respective relevance in the performance of SCs. Keywords: tri-solvent-in-salt (TSIS), hydrogen bond, eutectic mixtures, supercapacitors Reference ： [1] F. Béguin, et al. Carbons and electrolytes for advanced supercapacitors. Adv. Mater., 26 (2014), 2219-2251. [2] Q. Dou, et al. Safe and high-rate supercapacitors based on an ‘‘Acetonitrile/Water in Salt’’ hybrid electrolyte. Energy Environ. Sci, 11 (2018), 3212-3219. [3] X. Lu, et al. Aqueous-Eutectic-in-Salt Electrolytes for High-Energy-Density Supercapacitors with an Operational Temperature Window of 100 °C, from −35 to +65 °C. ACS Appl. Mater. Interfaces 2020, 12, 26, 29181–29193. [4] X. Lu, et al. Aqueous Co-Solvent in Zwitterionic-based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors. ChemSusChem 2020, 13, 5983. [5] X. Lu, et al. EMIMBF4 in ternary liquid mixtures of water, dimethyl sulfoxide and acetonitrile as “tri-solvent-in-salt” electrolytes for high-performance supercapacitors operating at -70 °C. Energy Storage Mater., 40, (2021), 368-385.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.001 | 0.001 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.001 | 0.001 |
| Insufficient payload (model declined to judge) | 0.002 | 0.001 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".