Interfacial and Intercalated Carbonates: From Catalytic Interfaces to tuneable Layered Materials

Carbonates, in both their crystalline and amorphous forms, have been shown to play multifaceted roles across geological and synthetic environments. In this contribution, recent insights are presented into high-temperature interfacial carbonates (HT-CO₃) within CuO-ZnO-based catalyst systems, where carbonate species are retained after calcination and act as molecular anchors at metal oxide interfaces. Through the combination of vibrational spectroscopy and first-principles modelling, their strong binding energies have been determined, and their essential role in suppressing thermal sintering has been demonstrated. The concept of carbonate functionality is further extended to layered double hydroxides (LDHs) — synthetic analogues to natural hydrotalcite-like phases — in which carbonate ions are incorporated as interlayer anions to modulate material stability, reactivity, and ion-exchange capacity. By comparing these two chemically and structurally distinct systems, the versatility of carbonate species is emphasized, both in dynamic catalytic settings and in tuneable layered solids. A broader understanding of carbonate behaviour at the molecular scale is thereby contributed, with implications for geochemistry, nanomaterials design, and carbon management strategies.