Novel processes are urgently needed to recycle critical
materials
(e.g., cobalt, lithium, nickel, and manganese) from spent lithium-ion
batteries (LIBs). These separations are vital both to meet growing
global demand and to mitigate a looming e-waste crisis. Currently,
to recover cobalt and lithium from spent LIBs, high temperatures and
organic solvents are used to separate Co2+ and Li+ in complex leaching and extraction processes. In contrast to using
expensive designer ligands or harmful organic solvents, this work
reveals that continuous membrane cascades are a promising aqueous-based
alternative to recover these critical materials and facilitate their
reuse. A superstructure optimization model that designs diafiltration
cascades to maximize material recovery and purity as a function of
membrane material performance and feed specifications is developed.
This approach enables the comparison of candidate membrane materials
by rapidly predicting the Pareto optimal trade-offs between the recovery
and purity of lithium and cobalt for bespoke cascade designs. For
example, the model predicts that, when deployed in an optimized two-stage
cascade configuration, a nanofiltration membrane with a modest selectivity
of 32 can be used to recover 95% Li+ and 99% Co2+ at 93 and 99.5 wt % purity, respectively. On the basis of analysis
of over 1000 Pareto optimal designs, six design heuristics for executing
binary separations using staged diafiltration cascades are proposed.
Moreover, by evaluating membrane materials in the context of optimized
diafiltration processes, this work quantifies the benefits of materials
improvements and shows that the greatest research opportunities for
membrane-based LIB recycling are at the device and systems scales.
More broadly, the optimization models represent a robust framework
for identifying the most effective way to deploy emerging materials
in integrated process systems. This transformative capability is widely
applicable to many of the separations needed to support sustainable
global development.