Wide-Temperature Range Lithium-Ion Batteries through Characterization of Surface Reactivity and Electrode/Electrolyte Interfacial Kinetics

Lithium-ion batteries (LIBs) are essential components of space travel, and they enable fundamental technologies such as space suits, satellite probes, rovers, drones, and handheld equipment. Commercial LIBs are typically operated between 15 degrees Celsius and 35 degrees Celsius, above which accelerated electrolyte decomposition and SEI growth occur, and below which sluggish reaction kinetics cause lithium plating leading to irreversible capacity fade and dendrite growth. To better utilize LIBs for crewed missions to the lunar surface and Mars’ moons, which experience temperatures well outside of these standard bounds of operation, it is necessary to characterize the surface reactivity and interfacial kinetics at the solid electrode/electrolyte interface (SEI) layer for more extreme temperatures. This research proposes to characterize the charge-transfer kinetics at the SEI, and the performance benefit of co-modified systems containing fluorinated electrolytes and preferentially-stable electrode coatings in LIBs tested over a wide temperature range of -60 degrees Celsius to 100 degrees Celsius. This will be accomplished using a three phase study, starting with the characterization of low temperature rate-limiting desolvation reactions, as well as the high temperature reactivity between the test electrolytes and their SEI layers, in order to better understand their mechanisms and how to mitigate them. Second, independent electrochemical analyses coupled with advanced materials characterization techniques will be utilized to explore the capability of artificial coatings to prevent surface reactivity, transition metal dissolution, and the formation of unfavorable SEI chemistries. Finally, these independent SEI mitigation techniques will be translated to LIB full cells for analysis of coupled modified-electrolyte and preferentially-stable coated-electrode systems. This research will help answer the fundamental knowledge gap concerning the degradation mechanisms during SEI formation, and simultaneously develop novel battery configurations that better enable NASA’s missions exploring the solar system and galaxy.

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