Scholarlink

<p>The use of aqueous/non-aqueous biphasic electrolyte solutions in Li-based battery systems circumvents the limitations of poor reductive stability of aqueous electrolyte solutions, broadening their electrochemical stability window. However, aqueous/non-aqueous electrolytes suffer from biphasic mixing and high impedance when Li ions cross the biphasic interface. Here we propose the use of 12-crown-4 (12C4) and tetraglyme (G4) as lithium ionophores to form Li<sup>+</sup>(ionophore) nanoclusters in both non-aqueous and aqueous phases to overcome the interface challenges in biphasic electrolytes. The Li<sup>+</sup>(ionophore) nanoclusters have the H<sub>2</sub>O-excluding inner Li<sup>+</sup> solvation structure in non-polar 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE), allowing fast charge transport across the biphasic interface without solvent mixing or water shuttling. A tailored electrolyte formulation comprising the lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, 12C4, TTE and H<sub>2</sub>O solvents (labelled LiTFSI−12C4@TTE/H<sub>2</sub>O) demonstrates low impedance (2.7 Ω cm<sup>−</sup><sup>2</sup>) at the TTE/H<sub>2</sub>O interface and enabling 2,000 cycles of prelithiated graphite||LiFePO<sub>4</sub> coin cells at 850 mA g<sup>−1</sup> with an average Coulombic efficiency of 99.8%. Single-layer 22.5 mAh Li||LiMn<sub>2</sub>O<sub>4</sub> pouch cells using LiTFSI−12C4@TTE/H<sub>2</sub>O electrolyte with G4 delivered a stable discharge capacity of about 1.3 mAh cm<sup>−2</sup> for 80 cycles at 0.5 mA cm<sup>−2</sup>.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Li+(ionophore) nanoclusters engineered aqueous/non-aqueous biphasic electrolyte solutions for high-potential lithium-based batteries

  • 期刊论文

  • 发表日期：

    2025年4月8日

查看全文
  • Xiyue Zhang,
  • Travis P. Pollard,
  • Sha Tan,
  • Nan Zhang,
  • Jijian Xu,
  • Yijie Liu,
  • An L. Phan,
  • Weiran Zhang,
  • Fu Chen,
  • Chongyin Yang,
  • Enyuan Hu,
  • Xiao-Qing Yang,
  • Oleg Borodin,
  • Chunsheng Wang

摘要

The use of aqueous/non-aqueous biphasic electrolyte solutions in Li-based battery systems circumvents the limitations of poor reductive stability of aqueous electrolyte solutions, broadening their electrochemical stability window. However, aqueous/non-aqueous electrolytes suffer from biphasic mixing and high impedance when Li ions cross the biphasic interface. Here we propose the use of 12-crown-4 (12C4) and tetraglyme (G4) as lithium ionophores to form Li+(ionophore) nanoclusters in both non-aqueous and aqueous phases to overcome the interface challenges in biphasic electrolytes. The Li+(ionophore) nanoclusters have the H2O-excluding inner Li+ solvation structure in non-polar 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE), allowing fast charge transport across the biphasic interface without solvent mixing or water shuttling. A tailored electrolyte formulation comprising the lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, 12C4, TTE and H2O solvents (labelled LiTFSI−12C4@TTE/H2O) demonstrates low impedance (2.7 Ω cm−2) at the TTE/H2O interface and enabling 2,000 cycles of prelithiated graphite||LiFePO4 coin cells at 850 mA g−1 with an average Coulombic efficiency of 99.8%. Single-layer 22.5 mAh Li||LiMn2O4 pouch cells using LiTFSI−12C4@TTE/H2O electrolyte with G4 delivered a stable discharge capacity of about 1.3 mAh cm−2 for 80 cycles at 0.5 mA cm−2.