Cooperative Lithium Sorption in Doped Layered Double Hydroxides Is Modulated by Colloidal (Dis)Assembly

Lithium–aluminum layered double hydroxides (LDHs) selectively sorb lithium from brines, concentrating and purifying this critical element for subsequent conversion to active battery components. Lithium ion partitioning into lattice vacancies within the LDH structure is enhanced with iron doping. However, process leads a highly coupled set of intercalation interactions whose mechanisms are challenging assess in situ. Here, we show that modulates size- shape-dependent composition LDHs imposes powerful control on sorption processes complex fluids. We observe fundamental units layers aluminum ferrihydrite nanoclusters (dis)assemble form at least five distinct particle types influence capacity cyclability. Importantly, controlled by feedbacks arising dynamic interconversion planar stacks scrolls layers, which exchange lithium, water, other species (un)rolling due similar energy scales hydration, sorption, deformation. Under appropriate redox conditions, cycling efficiency stability can be optimized range concentrations found many natural brines.