Tailoring polymer electrolyte ionic conductivity for production of low- temperature operating quasi-all-solid-state lithium metal batteries

The stable operation of lithium-based batteries at low temperatures is critical for applications in cold climates. However, low-temperature operations are plagued by insufficient dynamics in the bulk of the electrolyte and at electrode|electrolyte interfaces. Here, we report a quasi-solid-state polymer electrolyte with an ionic conductivity of 2.2 × 10−4 S cm−1 at −20 °C. The electrolyte is prepared via in situ polymerization using a 1,3,5-trioxane-based precursor. The polymer-based electrolyte enables a dual-layered solid electrolyte interphase formation on the Li metal electrode and stabilizes the LiNi0.8Co0.1Mn0.1O2-based positive electrode, thus improving interfacial charge-transfer at low temperatures. Consequently, the growth of dendrites at the lithium metal electrode is hindered, thus enabling stable Li||LiNi0.8Co0.1Mn0.1O2 coin and pouch cell operation even at −30 °C. In particular, we report a Li||LiNi0.8Co0.1Mn0.1O2 coin cell cycled at −20 °C and 20 mA g−1 capable of retaining more than 75% (i.e., around 151 mAh g−1) of its first discharge capacity cycle at 30 °C and same specific current.