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This is a correction to the original manuscript. The original manuscript had missing text describing funding sources. 

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 °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 °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 °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. 

Abstract Confining molecules in the nanoscale environment can lead to dramatic changes of their physical and chemical properties, which opens possibilities for new applications. There is a growing interest in liquefied gas electrolytes for electrochemical devices operating at low temperatures due to their low melting point. However, their high vapor pressure still poses potential safety concerns for practical usages. Herein, we report facile capillary condensation of gas electrolyte by strong confinement in sub-nanometer pores of metal-organic framework (MOF). By designing MOF-polymer membranes (MPMs) that present dense and continuous micropore (~0.8 nm) networks, we show significant uptake of hydrofluorocarbon molecules in MOF pores at pressure lower than the bulk counterpart. This unique property enables lithium/fluorinated graphite batteries with MPM-based electrolytes to deliver a significantly higher capacity than those with commercial separator membranes (~500 mAh g⁻¹vs. <0.03 mAh g⁻¹) at −40 °C under reduced pressure of the electrolyte.