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For realizing the commercialization of Li-metal batteries (LMBs), the discharge-blocking obstacles under ultra-low temperatures must be conquered besides the long-term reversibility. Nevertheless, commercial carbonate-based electrolytes are not only incompatible with the aggressive Li anode, but also have poor fluidity at low temperatures. The prevailing chain-ether-based electrolyte designing tactics, such as the common-used DME, improve the affinity with Li metal to some extent, but the multiple Lewis-acid binding sites of chain ethers are not conducive to the de-solvation of Li+. Herein, for the first time, the cheap cyclic-type tetrahydrofuran (THF) with ultra-low melting point and weak solvating power is adopted for designing an original THF-based localized saturated electrolyte (Tb-LSCE), demonstrating excellent adaptability for low-temperature LMBs. Computational and experimental evidence verify the original solvated structure is modified via the addition of fluorinated antisolvent, further contributing to the Li+-THF de-solvation. Therefore, equipped with Tb-LSCE, the assembled Li-NCM523 cells achieve powerful anti-polarization capability at low temperatures (73.3% discharge capacity retention at-30 degrees C). Furthermore, the unique solvated sheath structure of Tb-LSCE also regulates the interfacial chemistry and uniformity of Li depositing behavior, highlighted by the outstanding reversibility of Li-Li cells (a long lifespan of exceeding 1600 h at 30 degrees C and 1100 h at-30 degrees C, respectively) and Li-NCM523 cells (80.7%, 160 cycles) even remarkably stable operation within 50 cycles (ultra-high cathode loading of 19.7 mg cm-2). This work outlines a cheap and effective electrolyte design solution to activate the potential LMBs under practical conditions, especially those operated under cryogenic environments.
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ENERGY STORAGE MATERIALS
ISSN: 2405-8297
Year: 2023
Volume: 58
Page: 184-194
1 8 . 9
JCR@2023
1 8 . 9 0 0
JCR@2023
ESI Discipline: MATERIALS SCIENCE;
ESI HC Threshold:49
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 18
SCOPUS Cited Count: 18
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 3