On Demand One-Pot Mild Preparation of Layered Double Hydroxides and Their Hybrid Forms: Advances through the Epoxide Route

Epoxide ring opening driven alkalinization process was explored with the aim of preparing layered double hydroxide (LDH) phases on demand, at room temperature. Employing iodide as nucleophilic agent, the precipitation reaction can be driven under much lower halide concentrations. This scenario favors the selective intercalation of concomitant bulky oxo anions as nitrate or perchlorate in the LDH products, allowing for the one-pot synthesis of an LDH able to delaminate in formamide. Even large dicarboxylic acids, ⁻O₂C-(CH₂)_n-CO₂ ⁻, with n up to 8, can be quantitively intercalated within the growing LDH phase, providing a versatile one-pot route for hybrid LDHs as well. Under the mild conditions employed, governed by a continuous pH rise from a starting acid condition, a M^II to M^*III ratio of 2 prevails, independently from the overall cationic composition. However, after moderate hydrothermal aging LDH phases bearing a cationic ratio higher than 2 could result. The solubility of a given chloride-containing M^II ₂M^*III LDH can be approximated as a linear combination of the solubility of the pure hydroxylated phases of the constitutive cations, M(OH)₂ and M^*(OH)₃.