Abstract:The pursuit of high energy density enables lithium metal batteries (LMBs) to become the research hotpot again. However, the safety concerns including easy leakage and inflammability of the liquid electrolyte and the performance deterioration due to the uncontrollable Li dendrites growth in liquid electrolyte limit the further development of LMBs. Gel electrolyte, the most promising alternative for the commercial liquid electrolyte, is expected to solve the dilemma faced by the liquid electrolyte because of its… Show more
“…With the FEC plasticizer addition, the ionic conductivity has increased by dozens of times and the impedance drops down to 13 Ω at RT. The plasticizer tends to weaken the intermolecular forces between polymer molecules and thus the activity and mobility of polymer molecular chain increase, 37 on the other hand, introducing FEC plasticizer to PDOL also can promote the dissociation of Li salts and provide new ions conducting paths in plasticizer. 38 Because of the reasons above, ionic conductivity of the electrolyte is significantly improved by introducing FEC.…”
In-situ-polymerized solid-state electrolytes can significantly
improve the interfacial compatibility of Li metal batteries. Typically,
in-situ-polymerized 1,3-dioxolane electrolyte (PDOL) exhibits good
compatibility with Li metal. However, it still suffers from the narrow
electrochemical window (4.1 V), limiting the application of high-voltage
cathodes. Herein, a novel modified PDOL (PDOL-F/S) electrolyte with
an expanded electrochemical window of 4.43 V and a considerable ionic
conductivity of 1.95 × 10–4 S cm–1 is developed by introducing high-voltage stable plasticizers (fluoroethylene
carbonate and succinonitrile) to its polymer network. The space-confined
plasticizers are beneficial to construct a high-quality cathode–electrolyte
interphase, hindering the decomposition of lithium salts and polymers
in electrolytes at high voltage. The as-assembled Li|PDOL-F/S|LiCoO2 battery delivers superior cycling stability (capacity retention
of 80% after 400 cycles) at 4.3 V, superior to that of pristine PDOL
(3% after 120 cycles). This work provides new insights into the design
and application of high-voltage solid-state lithium metal batteries
by in situ polymerization.
“…With the FEC plasticizer addition, the ionic conductivity has increased by dozens of times and the impedance drops down to 13 Ω at RT. The plasticizer tends to weaken the intermolecular forces between polymer molecules and thus the activity and mobility of polymer molecular chain increase, 37 on the other hand, introducing FEC plasticizer to PDOL also can promote the dissociation of Li salts and provide new ions conducting paths in plasticizer. 38 Because of the reasons above, ionic conductivity of the electrolyte is significantly improved by introducing FEC.…”
In-situ-polymerized solid-state electrolytes can significantly
improve the interfacial compatibility of Li metal batteries. Typically,
in-situ-polymerized 1,3-dioxolane electrolyte (PDOL) exhibits good
compatibility with Li metal. However, it still suffers from the narrow
electrochemical window (4.1 V), limiting the application of high-voltage
cathodes. Herein, a novel modified PDOL (PDOL-F/S) electrolyte with
an expanded electrochemical window of 4.43 V and a considerable ionic
conductivity of 1.95 × 10–4 S cm–1 is developed by introducing high-voltage stable plasticizers (fluoroethylene
carbonate and succinonitrile) to its polymer network. The space-confined
plasticizers are beneficial to construct a high-quality cathode–electrolyte
interphase, hindering the decomposition of lithium salts and polymers
in electrolytes at high voltage. The as-assembled Li|PDOL-F/S|LiCoO2 battery delivers superior cycling stability (capacity retention
of 80% after 400 cycles) at 4.3 V, superior to that of pristine PDOL
(3% after 120 cycles). This work provides new insights into the design
and application of high-voltage solid-state lithium metal batteries
by in situ polymerization.
“…Consequently, the segmental mobility of the polymer is enhanced. [ 55,56 ] Furthermore, the incorporation of plasticizers with high‐dielectric constants facilitates the dissociation of the lithium salts. [ 57 ] These synergistic effects of enhanced segment mobility and increased charge carrier concentration further enhance the ion conduction of the polymer matrices.…”
Section: Intrinsic Characteristics and Li+ Conduction Mechanisms Of V...mentioning
Portable electronic devices and electric vehicles have become indispensable in daily life and caused an increasing demand for high‐performance lithium‐ion batteries (LIBs) with high‐energy‐density. This work compares the intrinsic characteristics and Li+ conduction mechanisms of various electrolytes, aiming at emphasizing their suitability for high‐energy‐density LIBs. Among all electrolytes, polymer‐based solid‐state electrolytes (SSEs) are the most promising candidates, as they demonstrate the most comprehensive properties. The advantages and disadvantages of commonly used polymer matrix materials of SSEs are discussed, along with typical approaches to address their limitations. As significant issues for high‐energy‐density and cycle stability, the development related to the cathode/electrolyte interfacial contact and wetting, interfacial electrochemical compatibility, and interfacial Li+ conduction in LIBs employing polymer‐based SSEs, as well as the anode/electrolyte interfacial chemical stability and lithium dendrite suppression are comprehensively reviewed and analyzed. Finally, perspectives on future research directions for developing high‐energy‐density LIBs are highlighted building upon the existing literature.
“…12,13 GEs deliver comparable ion conductive capacity to liquid electrolytes, while the risks of solvent leakage and fast evaporation are greatly reduced owing to the strong affinity between the gel networks and solvents. 14,15 Inside the GEs, the as-formed cross-linking network accounts for the elastic response and the solvent component contributes to the energy loss, which is responsible for their observable viscoelastic behaviour under imposed deformations. By fine-tuning the chemical compositions and hierarchical structures, the mechanical properties of the resultant gels can be broadly tuned and adapted to different service conditions.…”
The commercial proton exchange membranes (PEMs) impose high requirements on environmental humidity, which significantly narrows the applications of PEM-assembled fuel cells and raises costs for humidity maintenance. Herein, polyvinyl alcohol...
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