Recently, aluminum–graphite batteries using chloroaluminate
ionic liquid electrolytes have been shown to store charge with significant
pseudocapacitive contributions, features attractive for energy storage
systems that must function with high capacity retention and high specific
power at low temperatures. Herein, we present results toward rechargeable
aluminum–graphite batteries designed specifically for low-temperature
applications, focusing on electrolyte design to reduce the melting
point and enhance ion transport properties down to −40 °C.
Chloroaluminate ionic liquid electrolytes with mixtures of organic
cations, particularly imidazolium cations with different asymmetric
functional groups, were used to impart disorder, disrupt ion clustering,
and enhance low-temperature ion mobilities. Graphite cathodes with
higher pseudocapacitive contributions showed improved specific capacity
retention at lower temperatures, while aluminum anodes with higher
surface roughness reduced the nucleation energy for aluminum electrodeposition.
An aluminum–natural graphite battery with mixed imidazolium
cations was shown to exhibit 87% specific capacity retention at −20
°C and 10 mA g–1. Overall, the results demonstrate
multiple approaches to improve low-temperature aluminum battery performance
and illustrate electrochemical methods that quantify electrolyte properties
relevant to ion transport and clustering, which can be universally
translated into other battery systems.