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A shuttle mechanism for molten-electrolyte lithium batteries

Technical Report ·
DOI:https://doi.org/10.2172/10105073· OSTI ID:10105073

The lithium-transport rates arising from a lithium shuttle mechanism (LSM) were examined by potentiometric control of a lithium-alloy electrode in a temperature range of 400 to 515{degrees}C in three electrolytes: LiCl-KCl, LiCl-LiBr-KBr, and LiF-LiCl-LiBr. Lithium transport in Li/FeS{sub x} cells by LSM was found to occur by diffusion of reduced lithium species across the separator layer, which was controlled by the Li-activity of the Li-alloy electrode. Solubility of lithium was strongly affected by electrolyte composition, especially K{sup +} content, which in turn regulated the lithium transport rate. As evidenced by LSM rates, the solubilized lithium would appear to form dimers (e.g. Li{sub 2}{sup +} or LiK{sup +}). The half-cell self-discharge rates, which were measured, correlate well with self-discharge rates in developmental cells ranging from 0.1 to 10 mA/cm{sup 2}. Innovative application of the LSM has led to the development of overcharge tolerant Li/FeS{sub x} cells. A bimodal self-discharge characteristic (a 20-fold increase toward the end of charge) results from a 150-250 mV step increase in lithium activity of a two-phase Li-alloy electrode (Li-Al plus Li-Al{sub 5}Fe{sub 2}). Three versions of the battery cell (100 cm{sup 2} separator area) have been demonstrated: LiAl+Li{sub 5}Al{sub 5}Fe{sub 2}(10% of capacity)/LiCl-LiBr-KBr(MgO)/FeS{sub 2}, as well as a FeS-type, (both operated at 400{degrees}C) and LiAl+Li{sub 5}Al{sub 5}Fe{sub 2}(10% of capacity)/LiF-LiCl-LiBr(MgO)/FeS (operated at 475{degrees}C). These cells exhibit a unique combination of overcharge capacity and extended trickle-charge tolerance at 2-5 mA/cm{sup 2}. Additionally, Li/FeS{sub 2} cells having overcharge tolerance have operated with stable performance for greater than 500 cycles. The overcharge tolerance rates are sufficient for battery cells to exhibit built-in charge/equalization capability by way of full-battery trickle charging.

Research Organization:
Argonne National Lab., IL (United States)
Sponsoring Organization:
USDOE, Washington, DC (United States)
DOE Contract Number:
W-31109-ENG-38
OSTI ID:
10105073
Report Number(s):
ANL/CMT/CP--79729; CONF-931024--5; ON: DE94002914
Country of Publication:
United States
Language:
English