Carbonyl-based negative electrodes have received considerable interest in the domain of rechargeable lithium batteries, owing to their superior feasibility in structural design, enhanced energy density, and good environmental sustainability. Among which, lithium terephthalate (LiTPA) has been intensively investigated as a negative electrode material in the past years, in light of its relatively stable discharge plateau at low potentials (ca. 1.0 V vs Li/Li+) and high specific capacity (ca. 290 mAh g-1). However, its cell performances are severely limited owing to the poor quality of the solid-electrolyte-interphase (SEI) layer generated therein. Here, we report the utilization of lithium bis(fluorosulfonyl)imide (LiFSI) as an electrolyte salt for forming a Li-ion permeable SEI layer on the LiTPA electrode and subsequently improving the cyclability and rate performance of the LiTPA-based cells. Our results show that, differing from the reference electrolyte containing the lithium hexafluorophosphate (LiPF6) salt, the electrochemical reductions of the FSI- anions occur prior to the lithiation processes of LiTPA electrode, which is capable of building an inorganic-rich SEI layer containing lithium fluoride (LiF) and lithium sulfate (Li2SO4). Consequently, the lithium metal (Li°)||LiTPA cell shows significantly improved cycling performance than the LiPF6-based reference cell. This work provides useful insight into the reductive processes of the FSI- anions on negative electrodes, which could spur the deployment of highly sustainable and high-energy rechargeable lithium batteries.
Keywords: carbonyl-based electrode; liquid electrolytes; lithium bis(fluorosulfonyl)imide; organic batteries; solid-electrolyte interphases.