Supercritical anti-solvent precipitation of amorphous, copper-zinc georgeite and acetate precursors for preparation of ambient-pressure water gas shift copper/zinc oxide catalysts

摘要

A series of copper-zinc acetate and zincian georgeite precursors have been produced by supercritical CO2 anti-solvent (SAS) precipitation as precursors to Cu/ZnO catalysts for the water gas shift (WGS) reaction. The amorphous materials were prepared by varying the water/ethanol volumetric ratio in the initial metal acetate solutions. Water addition promoted georgeite formation at the expense of mixed metal acetates, which are formed in the absence of the water co-solvent. Optimum SAS precipitation occurs without water to give high surface areas, whilst a high water content gives inferior surface areas and copper-zinc segregation. Calcination of the acetates is exothermic, producing a mixture of metal oxides with high crystallinity. However, thermal decomposition of zincian georgeite resulted in highly dispersed CuO and ZnO crystallites with poor structural order. The georgeite-derived catalysts give superior WGS performance in comparison to the acetate-derived catalysts, which is attributed to enhanced copper-zinc interactions that originate from the precursor.