The thermal decomposition processes of coprecipitated Cu-Ni-Al and Cu-Ni-Fe hydroxides and the formation of the mixed oxide phases were followed by thermogravimetry and derivative thermogravimetry analysis (TG – DTG) and in situ X-ray diffraction (XRD) in a temperature range from 25 to 800 °C. The as-prepared samples exhibited layered double hydroxide (LDH) with a rhombohedral structure for the Ni-richer Al- and Fe-bearing LDHs and a monoclinic structure for the CuAl LDH. Direct precipitation of CuO was also observed for the Cu-richest Fe-bearing samples. After the collapse of the LDHs, dehydration, dehydroxylation, and decarbonation occurred with an overlapping of these events to an extent, depending on the structure and composition, being more pronounced for the Fe-bearing rhombohedral LDHs and the monoclinic LDH. The Fe-bearing amorphous phases showed higher reactivity than the Al-bearing ones toward the crystallization of the mixed oxide phases. This reactivity was improved as the amount of embedded divalent cations increased. Moreover, the influence of copper was effective at a lower content than that of nickel.
