This study investigates single-pass dimethyl ether synthesis at mild pressure conditions using novel bifunctional catalysts based on indium-modified formulations and incorporating Ni, Cu, Pt, and Pd as active metals. Additionally, the substitution of the conventional HZSM-5 zeolite with 4A zeolite as the dehydration component was evaluated. Although 4A zeolite exhibited lower dehydration activity, it contributed to an overall improvement in DME selectivity. The incorporation of secondary metals into the In2O3-ZrO2 formulation reduced catalytic activity but enhanced selectivity, ultimately increasing DME yield. The formation of by-products such as light olefins and methane was significantly dependent on the metal used: Ni, Pt, and Pd reduced olefin production, though Ni promoted excessive methane formation across the whole temperature range. Notably, the Pt-based catalyst completely suppressed by-product formation across the temperature range studied. While the In2O3-ZrO2-based catalysts generally displayed lower space–time yields than the commercial reference, they achieved comparable performance at 280 °C. Due to their superior selectivity, these formulations are promising for developing even better performing catalysts, to be excellent candidates in industrial processes, where the operation with recycle loops requires a high product purity.
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