The deployment of rechargeable batteries is crucial for the operation of advanced portable electronics and electric vehicles under harsh environment. However, commercial lithium‐ion batteries using ethylene carbonate electrolytes suffer from severe loss in cell energy density at extremely low temperature. Lithium metal batteries (LMBs), which use Li metal as anode rather than graphite, are expected to push the baseline energy density of low‐temperature devices at the cell level. Albeit promising, the kinetic limitations of standard cell chemistries under subzero operation condition inevitably hamper the cyclability of LMBs, resulting in a severe decline in plating/stripping reversibility and short‐circuit hazards due to the dendritic growth. Such performance degradation becomes more pronounced with decreasing temperature, ascribing to sluggish ion transport kinetics during charging/discharging processes which includes Li+ solvation/desolvation, ion transport through bulk electrolyte, as well as ion diffusion within solid electrolyte interphase and bulk electrode materials at low temperature. In this review, the critical limiting factors and challenges for low‐temperature ion transport behaviors are systematically reviewed and discussed. The strategies to enhance Li+ transport kinetics in electrolytes, electrodes, and electrolyte/electrode interface are comprehensively summarized. Finally, perspective on future research direction of low‐temperature LMBs toward practical applications is proposed.

Ion Transport Kinetics in Low‐Temperature 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. 

/pdf/tailoring-polymer-electrolyte-ionic-conductivity-for-1bu5m9ry.pdf

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

The low ionic conductivity of poly(ethylene oxide) (PEO)‐based polymer electrolytes at room temperature and the undesired lithium‐dendrite growth at Li|PEO interface impede their further application. Herein, a PEO polymer is regulated at the molecular level through a copper ion (Cu2+) coordination effect with both PEO and Li salts to achieve a high Li+ conductivity of 0.2 mS cm−1 and a transference number of 0.42 at 30 °C. Moreover, the Cu‐coordinated PEO electrolyte is neither sticky nor hygroscopic because the hydrophilic oxygen groups in PEO are terminated by Cu ions. Furthermore, the in situ formed F/Li‐rich inorganic layer induced by CuF2 additive accelerates Li+ transport kinetics and enables uniform Li+ deposition during Li plating/stripping. As a result, the Cu2+‐coordinated PEO electrolytes deliver a high critical current density of 1.5 mA cm−2 at 30 °C. An all‐solid‐state Li‐LiNi0.83Co0.12Mn0.05O2 (NCM83) battery with such a copper coordinated PEO electrolyte exhibits a long cycle life over 500 cycles with a capacity retention of 71% under 0.6 C at 30 °C. When the mass loading increases to a record high of 7 mg cm−2, the Li‐NCM83 cell delivers a high areal capacity of 1.07 mAh cm−2 under 0.1 C at 30 °C.

Enabling All‐Solid‐State Li Metal Batteries Operated at 30 °C by Molecular Regulation of Polymer Electrolyte

Solid-state lithium-metal batteries constructed by in-situ solidification of cyclic ether, are considered to be a critical strategy for the next generation of solid-state batteries with high energy density and safety. However, the poor thermal/electrochemical stability of linear polyethers and severe interfacial reactions limit its further development. Herein, in-situ ring-opening hybrid crosslinked polymerization is proposed for organic/inorganic hybrid polymer electrolyte (HCPE) with superior ionic conductivity of 2.22×10-3 S cm-1 at 30°C, ultrahigh Li+ transference number of 0.88, and wide electrochemical stability window of 5.2 V. These allow highly stable lithium stripping/plating cycling for over 1000 h at 1 mA cm-2 , which also reveal a well-defined interfacial stabilization mechanism. Thus HCPE endows assembled solid-state lithium-metal batteries with excellent long-cycle performance over 600 cycles at 2 C (25°C) and superior capacity retention of 92.1%. More importantly, our proposed non-combustible HCPE opens up a new frontier to promote the practical application of high safety and high energy density solid-state batteries via in-situ solidification. This article is protected by copyright. All rights reserved.

Hybrid Crosslinked Solid Polymer Electrolyte via In-Situ Solidification Enables High-Performance Solid-State Lithium Metal Batteries.

Polymer solid electrolytes for solid‐state batteries typically suffer from low ionic conductivity and low oxidative stability. Herein, a polymer electrolyte based on a polymerized ionic liquid and an ionic liquid plasticizer offering simultaneously a high room‐temperature ionic conductivity of 0.8 mS cm−1 and a high oxidative stability >5.0 V versus Li+/Li, is reported. The electrolyte is compatible with lithium metal and non‐flammable upon direct flame exposure. In symmetric lithium metal cells, the electrolyte enables stable lithium plating and stripping at 0.1 mA cm−2 with a capacity of 1 mAh cm−2 per half cycle for over 1700 h at 25 °C. Cells with a lithium metal anode cycled against a state‐of‐the‐art high‐energy uncoated layered LiNi0.8Mn0.1Co0.1O2 cathode achieve an initial capacity of 162 mA h g−1 and a capacity retention of 72% after 600 cycles to an upper cut‐off voltage of 4.4 V at 25 °C. Cells with a high‐voltage spinel LiMn1.5Ni0.5O4 cathode reach an initial capacity of 132 mAh g−1 and a capacity retention of 76% after 300 cycles to an upper cut‐off voltage of 5 V at 25 °C, confirming the high oxidative stability and technological potential of this electrolyte for high‐voltage solid‐state lithium metal batteries.

A Polymerized‐Ionic‐Liquid‐Based Polymer Electrolyte with High Oxidative Stability for 4 and 5 V Class Solid‐State Lithium Metal Batteries

In Situ Fabricated Quasi-Solid Polymer Electrolyte for High-Energy-Density Lithium Metal Battery Capable of Subzero Operation

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In Situ Fabricated Quasi-Solid Polymer Electrolyte for High-Energy-Density Lithium Metal Battery Capable of Subzero Operation