Leveraging Molecular Architecture To Design New, All-Polymer Solid Electrolytes with Simultaneous Enhancement in Modulus and Ionic Conductivity

Abstract

The primary challenge regarding solid polymer electrolytes (SPEs) is the development of materials with enhanced mechanical modulus without sacrificing ionic conductivity. Here, we demonstrate that when stiff/rigid polymer nanoparticles that are thermodynamically miscible with a polymer are utilized in a blend with a liquid electrolyte, the elastic modulus and the ionic conductivity of the resulting SPEs increase compared to the linear polymer blend analogues. In particular, when poly­(methyl methacrylate), PMMA, nanoparticles, composed of high functionality star-shaped PMMA, were added to low molecular weight poly­(ethylene oxide), PEO, doped with bis­(trifluoromethane)­sulfonamide (LiTFSI), the resulting SPEs exhibit 2 orders of magnitude higher conductivity and 1 order of magnitude higher mechanical strength compared to their linear PMMA blend analogues. In addition, the former remain solidlike over an extended temperature range. Key to their performance is the morphology that stems from the ability of the PMMA nanoparticles to disperse within the liquid electrolyte host, allowing for the formation of a highly interconnected network of pure liquid electrolyte that leads to high ionic conductivity (comparable to that of the neat PEO electrolyte). The present strategy offers tremendous potential for the design of all-polymer electrolytes with optimized mechanical properties and ionic conductivity over a wide temperature window for advanced electrochemical devices.

Advances and Prospects of Sulfide All‐Solid‐State Lithium Batteries via One‐to‐One Comparison with Conventional Liquid Lithium Ion Batteries

“…Initial studies on the SEs for ASSLBs mainly focused on improving the ionic conductivity and the electrochemical/chemical stability. Many researchers developed oxide, sulfide‐based materials, and polymers . Recent research shows that the sulfide‐based SEs, especially LGPS‐type materials involving lithium, retained compatible ionic conductivity at room temperature, compared with the conventional carbonate‐based liquid electrolyte that was utilized in conventional LIBs.…”

Monochromatic “Photoinitibitor”‐Mediated Holographic Photopolymer Electrolytes for Lithium‐Ion Batteries

“…To improve the ionic conductivity, many strategies have been developed to suppress polymer crystallization. For instance, polymer blends, block copolymers, comb‐like polymers, and cross‐linked network polymers are designed toward the target . In addition, strategies such as replacing polymer matrices, employing new lithium salts, and loading plasticizers have been considered .…”

Effectively improved ionic conductivity of montmorillonite clay nanoplatelets incorporated nanocomposite solid polymer electrolytes for lithium ion-conducting devices

“…Among the various types of energy storing devices, the solid-state lithium-ion batteries (LIBs) have gained great success due to their promising commercial applications [1][2][3]. The overall performance of the LIBs depends on the synergic properties of the electrodes (anode and cathode) and the electrolyte material used in their design and development [4][5][6][7][8][9][10][11][12][13][14]. The electrolyte material acts as an ion conductor/separator between the electrodes and governs most of the electrochemical parameters of a battery including its high-performance and safer workability.…”

“…The electrolyte material acts as an ion conductor/separator between the electrodes and governs most of the electrochemical parameters of a battery including its high-performance and safer workability. The solid polymer electrolytes (SPEs) [6][7][8][9][10][11][12]14], inorganic solid electrolytes (ISEs) [13], hybrid solid polymer electrolytes (HSPEs) (i.e., inorganic materials incorporated nanocomposite solid polymer electrolytes (NSPEs) [15][16][17][18][19], and plasticized solid polymer electrolytes (PSPEs) [20][21][22][23]) are frequently used for the fabrication of high energy density rechargeable LIBs.…”

“…The relatively enhanced ionic conductivity, good flexibility, better electrode/electrolyte interface capability and excellent processability of the SPEs, NSPEs, and PSPEs are the main factors due to which these materials have been the topic of great interest for the researchers over the past few decades [6][7][8][9][10][11][12][15][16][17][18][19][20][21][22][23]. So far, a large number of polymers and their blends as base matrices, different lithium metal salts as ionic dopant, various liquid plasticizers (high dielectric constant polar liquids for increasing amorphous phase and degree of salt dissolution), and a large number of nanosized inorganic materials (for improving the physical and electrochemical performance and to prevent the growth of dendrites during cycling) have been used for the preparation of novel SPE, NSPE and PSPE materials.…”