4.6 Article

Rational Electrolyte Design to Form Inorganic-Polymeric Interphase on Silicon-Based Anodes

期刊

ACS ENERGY LETTERS
卷 6, 期 5, 页码 1811-1820

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c00514

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资金

  1. JSPS KAKENHI [20H05673]
  2. JST [JPMJPF2016]
  3. National Natural Science Foundation of China [22005108]
  4. Natural Science Foundation of Guangdong Province [2019A1515011460, 2019B1515120027]
  5. Guangdong Science and Technology Department [2020B0101030005, 2021A0505030063]
  6. Grants-in-Aid for Scientific Research [20H05673] Funding Source: KAKEN

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The research team designed a nonflammable cyclic phosphate-based electrolyte to adjust the component of the electrode/electrolyte interface, which enables the battery to maintain high elasticity and robustness even under high volume changes, achieving extremely high energy density and cycling stability.
Silicon-based materials have been regarded as the most promising anodes for high-energy batteries, when combined with high- voltage/capacity nickel-rich layered cathodes. However, challenges arise from unstable electrode/electrolyte interphases on the anode and cathode as well as from safety hazards associated with highly flammable commercial electrolytes. Herein, we rationally design a nonflammable cyclic phosphate-based electrolyte to tune the electrode/electrolyte interphase components by controlling the reduction of a cyclic phosphate and Li salt. This strategy enables the electrolyte to form a highly elastic, robust inorganic-polymeric interphase on microsized silicon-based anodes that can accommodate the immense volume changes. Furthermore, by generating a stable polymeric interphase on the surface of the cathode as well, a SiO vertical bar LiNi(0.6)Mn0.2Co(0.2)O(2) cell demonstrated an extremely high energy density of similar to 590 Wh.kg(-1) with 71.4% capacity retained over 300 cycles and high Coulombic efficiency of 99.9%. This interfacial regulation strategy is of vital importance for designing new electrolytes for high-energy-density batteries.

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