Natural deep eutectics solvents (NADES), owing to their high solvation capacity and nontoxicity, are actively being sought for many technological applications. Herein, we report a series of novel NADES based on choline chloride and plant-derived polyphenols. Most of the obtained phenolic NADES have a wide liquid range and high thermal stability above 150 °C. Among them, small-sized polyphenols, like pyrogallol, vanillyl alcohol, or gentisic acid, lead to low-viscosity liquids with ionic conductivities in the order of 10^-3 S cm^-1 at room temperature. Interestingly, polyphenols possess valuable properties as therapeutic agents, antioxidants, adhesives, or redox-active compounds, among others. Thus, we evaluated the potential of these novel NADES for two applications: bioadhesives and corrosion protection. The mixture of choline chloride-vanillyl alcohol (2:3 mol ratio) and gelatin resulted in a highly adhesive viscoelastic liquid (adhesive stress ≈ 135 kPa), affording shear thinning behavior. Furthermore, choline chloride-tannic acid (20:1) showed an extraordinary ability to coordinate iron ions, reaching excellent corrosion inhibitive efficiencies in mild steel protection.

Lithium batteries are in high demand in different technological fields. However, the operating temperature is required to be below 70 °C, and this limits their use in applications demanding high-energy rechargeable batteries that are able to operate at temperatures above 100 °C. Poly(ethylene oxide) (PEO) is, currently, the reference solid polymer electrolyte (SPE) employed in solid-state lithium batteries. However, the application of PEO at higher temperatures is restricted due to the loss of mechanical properties. In this article, we show that the polymer blending strategy of blending PEO with poly(l,l-lactide) (PLA) allows extending its use in batteries at high temperatures (100 °C). This improvement is due to the mechanical reinforcement of PEO solid electrolytes associated with the presence of PLA crystals. Thus, two solid electrolyte systems based on PEO/PLA blends with either a LiTFSI salt or a lithium single-ion polymer (poly(lithium-1-[3-(methacryloyloxy)propylsulfonyl]-1-(trifluoromethanesulfonyl)imide), PLiMTFSI) were investigated and compared. Differential scanning calorimetry (DSC) results indicate that regardless of the concentration of LiTFSI or PLiMTFSI in the blend, crystals of PLA are present with melting peaks at 160–170 °C and the lithium salt distributes preferentially in the PEO-rich amorphous phases. The ionic conductivity is negatively affected by the incorporation of PLA in the blends. However, at high temperatures (>70 °C), ionic conductivities of ∼10^–4 S cm^–1 were obtained for both systems. DMTA results showed that PLA addition increases the mechanical properties of the electrolytes, yielding storage modulus values of ∼10⁶ Pa for the PEO/PLA/LiTFSI blend and ∼10⁷ Pa or higher for the PEO/PLA/PLiMTFSI blend at high temperatures (100 °C). Finally, both ternary blends were compared in a symmetrical lithium battery at 100 °C, and the single-ion conducting PEO/PLA/PLiMTFSI system presented lower overpotentials, which is reflected in a lower polarization inside the lithium battery.

Electrochemical impedance spectroscopy (EIS) has been proposed as an in situ strategy for the analysis of materials properties applied in the study of lithium-ion batteries (LIBs). However, the number and physical nature of the processes occurring simultaneously, combined with the typical interpretation of EIS spectra make the study challenging. To make the EIS interpretation more inclusive, in this work a graphical Bode diagram deconvolution is proposed, utilizing time constants τ (R-CPE), associated with relaxation of the phenomena occurring in battery composite electrodes. Since the effect of the additives on the electrode composite is still controversial and difficult to analyze for other in situ techniques, the graphical strategy is first applied to a LiFePO ₄ cathode with PVDF as the binder, to discriminate the contribution of each τ during different state of charge (SOC). This is done by removing the influence of counter electrode using a commercial three-electrode set-up cell. Then, the same cathode was evaluated, but with a Single Lithium-Ion Conducting Binder (SLICB). The electrode modification was easily observed with the graphical analysis. The results show that SLICB improved the speed of the processes, moving them to high frequencies, given that the polymer provides a continuous supply of ions diminishing concentration polarization.

Solid-state lithium batteries are considered one of the most promising battery systems due to their high volumetric energy density and safety. Poly(ethylene oxide) (PEO) is the most commonly used solid polymer electrolyte in solid-state batteries. In this article, we introduce new polyphosphoester polymer electrolytes, which show improved flame retardant properties in comparison with PEO. For this purpose, new polyphosphoester copolymers were synthesized, including phosphoester, poly(ethylene glycol) (PEG) and UV cross-linkable vinyl units. Solid polymer electrolyte films based on polyphosphoester copolymers and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) were prepared by curing under UV-light. The crystallinity present in the copolymers due to the PEG segment decreases with the amount of salt in the electrolyte, as seen by DSC. Solid polymer electrolytes based on polyphosphoester copolymers show ionic conductivity values as high as 2 × 10⁻⁴ S cm⁻¹ at 70 °C. FTIR analysis showed that lithium cations complexed with phosphoester groups provoked an increase in the lithium transference number to 0.26 as compared to that of PEO 0.17. Pyrolysis flow combustion calorimetry (PCFC) or micro-calorimetry results demonstrated the improved flame retardancy of the polyphosphoesters in comparison to a reference PEO based polymer electrolyte. The selected polyphosphoester solid electrolyte was investigated in a solid-state lithium cell Li⁰/polymer electrolyte/LFP battery showing a specific capacity retention close to 80% and coulombic efficiency greater than 98% over 100 cycles at 70 °C.