High-Performance Lithium Metal Batteries with a Wide Operating Temperature Range in Carbonate Electrolyte by Manipulating Interfacial Chemistry

Abstract

Development of high-performance lithium metal batteries with a wide operating temperature range is highly challenging, especially in carbonate electrolyte. Herein, a multifunctional high-donor-number solvent, tris-(pyrrolidinophosphine) oxide (TPPO), is introduced into carbonate electrolyte to regulate both electrode−electrolyte interfaces. On the one hand, lithium nitrate can be easily dissolved in carbonate electrolyte because of the strong interaction between TPPO and Li + , resulting in the formation of a robust and ionic conductive Li 3 N-rich solid electrolyte interphase, which efficiently inhibits the formation of lithium dendrites. On the other hand, TPPO can be preferentially oxidized into an ultrathin and robust cathode electrolyte interphase, significantly suppressing electrolyte decomposition. As a result, the TPPO-containing electrolyte enables stable lithium stripping/plating cycling performance (1000 h at 3 mA cm −2 and 3 mAh cm −2 ). Furthermore, Li/LiFePO 4 cells exhibit stable cycling performance even at temperatures as high as 70 °C and as low as −15 °C, demonstrating their potential in temperature tolerance.

A quasi-intercalation reaction for fast sulfur redox kinetics in solid-state lithium–sulfur batteries

“…It is generally accepted that LiF and Li x N are good SEI components for inhibiting lithium dendrite growth because LiF has a high interfacial energy 33 and Li x N has a good ionic conductivity. 34 In contrast, organic and oxide SEI components are easily decomposed. 35 The higher molar ratio of carbon and oxygen in the lithium metal in the cell with the liquid electrolyte indicates the formation of an unstable SEI, which may lead to lithium dendrite growth (Fig.…”

A nonflammable electrolyte for ultrahigh-voltage (4.8 V-class) Li||NCM811 cells with a wide temperature range of 100 °C

“…11,12 Meanwhile, EC-based electrolytes are prone to being reduced on lithium metal, resulting in the formation of an inhomogeneous and unstable solid-electrolyte interphase (SEI), which leads to the formation of lithium dendrites, capacity fade and a low Coulombic efficiency (CE). [13][14][15] Designing novel electrolyte systems compatible with both high-voltage cathodes and lithium metal anodes by constructing both stable CEI and SEI seems the most promising strategy for constructing ultrahigh-voltage LMBs. In previous reports, high-concentration electrolytes, 16 localized high-concentration electrolytes, 12,17 sulfonamide-based electrolytes, 10 phosphatebased electrolytes, 18 fluorinated solvents, 11 additives, 19,20 and salts, 9,21 have been investigated in high-voltage LMBs.…”

“…11,12 Meanwhile, EC-based electrolytes are prone to being reduced on lithium metal, resulting in the formation of an inhomogeneous and unstable solid–electrolyte interphase (SEI), which leads to the formation of lithium dendrites, capacity fade and a low Coulombic efficiency (CE). 13–15…”

A perspective on energy chemistry of low-temperature lithium metal batteries

“…The sluggish diffusion kinetics of Li ions across the SEI results in rapid depletion of Li ions at the interface, triggering early initiation of Li dendrites at low temperatures (Figure 6(b)) [87] . Improving the ionic conductivity of SEI is critically important for the efficient operation of low-temperature Li metal anodes.…”