Solid Polymer Electrolytes Based on Functionalized Tannic Acids from Natural Resources for All‐Solid‐State Lithium‐Ion Batteries

Abstract

Solid polymer electrolytes (SPEs) for all-solid-state lithium-ion batteries are prepared by simple one-pot polymerization induced by ultraviolet (UV) light using poly(ethylene glycol) methyl ether methacrylate (PEGMA) as an ion-conducting monomeric unit and tannic acid (TA)-based crosslinking agent and plasticizer. The crosslinking agent and plasticizer based on natural resources are obtained from the reaction of TA with glycidyl methacrylate and glycidyl poly(ethylene glycol), respectively. Dimensionally stable free-standing SPE having a large ionic conductivity of 5.6×10(-4) Scm(-1) at room temperature can be obtained by the polymerization of PEGMA into P(PEGMA) with a very small amount (0.1 wt %) of the crosslinking agent and 2.0 wt % of the plasticizer. The ionic conductivity value of SPE with a crosslinked structure is one order of magnitude larger than that of linear P(PEGMA) in the waxy state.

Sustainable Lignin‐Derived Cross‐Linked Graft Polymers as Electrolyte and Binder Materials for Lithium Metal Batteries

“…Cross‐linking of LPG by heat treatment during drying of the cathode was confirmed by FT‐IR spectroscopy and solubility testing in THF (Figure S8). Furthermore, the surface of the cathode was further coated with PPEGMA linear polymer synthesized by free radical polymerization (see Figure S9 for synthetic scheme and 1 H NMR spectroscopy, and GPC results for PPEGMA) by a direct solution casting method to soak the porous inner space of the cathode, thereby readily forming an ion‐conductive pathway for the facile ion conduction . Prior to the evaluation of cycling performance, the electrochemical stability of LPGP10 was verified by cyclic voltammetry (Figure S10).…”

“…The long‐term cycling performance of the cells with LPGP10 and Celgard was tested at a rate of 0.1 C at 60 °C. Since LPGP10 has relatively low ionic conductivity, the cell performance was tested at a low current density of 0.1 C, as for the other SPE cell systems . Higher discharge capacity values were obtained during 50 cycles in the case of the cell with LPGP10 compared to that of the cell with Celgard, and outstanding capacity retention after 50 cycles was observed with LPGP10 (98 %), presumably due to the formation of stable SEI layer as well as the suppression of lithium dendrite growth .…”

“…Furthermore, the mechanical stability of PEO and its derivatives should be further improved to achieve the durability and processing of the SPEs. Therefore, the increase of both ionic conductivity and mechanical stability of the SPEs simultaneously has been the main object in the field of SPEs, and various strategies, such as tailoring the polymer morphologies and adding the fillers or plasticizers, have been proposed.…”

A new composite solid electrolyte PEO/Li10GeP2S12/SN for all-solid-state lithium battery

“…Therefore, several approaches have been developed to increase the amorphous content in the PEO-based electrolytes for achieving higher Li + conductivities at room temperature [9]. J. C. Lee [10] developed a new SPE by polymerization induced by ultraviolet light using poly(ethylene glycol) methyl ether methacrylate (PEGMA) as an ion-conducting monomeric unit and tannic acid (TA)-based crosslinking agent and plasticizer. The all-solid-state battery using this new SPE at 60 C exhibited good capacity retention ($75%) after 50 cycles with a charge-discharge rate of 0.1C.…”

Dendrite Suppression by Synergistic Combination of Solid Polymer Electrolyte Crosslinked with Natural Terpenes and Lithium‐Powder Anode for Lithium‐Metal Batteries

“…Flat surfaces without any wrinkles and pores were observed from the surface SEM images of the SPEs (Figure S9), indicating that macroscopic phase separation or aggregation did not occur in this system . When the crosslinked SPEs were prepared using methacrylated tannic acid and poly(ethylene glycol) methyl ether methacrylate (PEGMA) according to our previous study, wrinkles and pores were observed on the surface of the SPEs caused by the phase separation of electrolyte components, because they are not miscible . This time, the crosslinked SPEs prepared using polysiloxane‐based BPT and terpene‐based crosslinker do not show any phase separation behavior, because relatively nonpolar limonene or geraniol can be mixed well in the nonpolar BPT domains.…”