4.8 Article

Electrolyte design implications of ion-pairing in low-temperature Li metal batteries

期刊

ENERGY & ENVIRONMENTAL SCIENCE
卷 15, 期 4, 页码 1647-1658

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ee03422g

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资金

  1. NASA Space Technology Graduate Research Opportunity [80NSSC20K1174]
  2. Early Career Faculty grant from NASA's Space Technology Research Grants Program [ECF 80NSSC18K1512]
  3. NSF through the UC San Diego Materials Research Science and Engineering Center (UCSD MRSEC) [DMR-2011924]
  4. National Science Foundation [ECCS-1542148, ACI-1548562]

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In this study, we report the development of >4 V Li metal full cell batteries capable of charging and discharging at extremely low temperatures. By introducing cation/anion pairs in the electrolyte, significant improvements in the performance of the batteries were observed. This ion-pairing effect was found to enhance both the cathode and anode, resulting in improved Coulombic efficiencies and oxidative stability of the Li metal.
Lithium metal batteries are capable of pushing cell energy densities beyond what is currently achievable with commercial Li-ion cells and are the ideal technology for supplying power to electronic devices at low temperatures (<=-20 degrees C). To minimize the thermal management requirements of these devices, batteries capable of both charging and discharging at these temperatures are highly desirable. Here, we report >4 V Li metal full cell batteries (N/P = 2) capable of hundreds of stable cycles down to -40 degrees C, unambiguously enabled by the introduction of cation/anion pairs in the electrolyte. Via controlled experimental and computational investigations in electrolytes employing 1,2-dimethoxyethane as the solvating solvent, we observed distinct performance transitions in low temperature electrochemical performance, coincident with a shift in the Li+ binding environment. The performance advantages of heavily ion-paired electrolytes were found to apply to both the cathode and anode, providing Li metal Coulombic efficiencies of 98.9, 98.5, and 96.9% at -20, -40, and -60 degrees C, respectively, while improving the oxidative stability in support of >4 V cathodes. This work reveals a strong correlation between ion-pairing and low-temperature performance while providing a viable route to Li metal full batteries cycling under extreme conditions.

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