Unlike conventional
electrode processing for Li-ion batteries, which uses the expensive
and highly toxic organic N-methyl-2-pyrrolidone (NMP)
solvent, aqueous processing simply employs deionized water as the
solvent. However, thick aqueous processed cathodes have been found
to crack during drying. In this study, the influence of electrode
drying temperature and thickness on cracking was investigated. LiNi1/3Mn1/3Co1/3O2 cathodes prepared
with a hydrophilic binder, modified styrene–butadiene rubber
(SBR), were coated at various thicknesses and dried at temperatures
ranging from 20 to 70 °C. Experiments revealed cracking worsens
with increased electrode thickness and elevated drying temperatures.
Cracks were formed during the capillarity-driven phase during drying.
Strong evaporation and weak diffusion played a critical role in the
nonuniform distribution of the inactive phase. Images of electrode
surfaces were processed to quantify crack dimensions and crack intensity
factor (CIF). The average crack length and width, as well as CIF,
increased with drying temperature and electrode thickness. Electrochemical
performance revealed a strong and negative correlation between the
crack density and performance in terms of specific capacity. Transport
limitations associated with the presence of cracks adversely affect
the advantage of high volume ratio of active materials in the thick
electrodes.