Copper Gallium Aluminum Mixed Metal Oxides as new Alternative Catalyst Candidates for Efficient Conversion of Carbon Dioxide to Methanol and Dimethyl Ether

Converting CO2 with renewable hydrogen requires high-value products to be economically viable due to its inherent energy intensity and associated renewable energy costs. Direct hydrogenation of CO2 via exothermic reactions is appealing given volatile energy prices. Methanol is valuable due to its wide use in the chemical industry and as sustainable fuel component. Indium oxide-based catalysts have been actively researched for several years; however, the scarcity of indium and the need for platinum group metals drive the search for alternatives using more abundant and non-noble metals and metal oxides. Employing a protocol which unites Artificial intelligence boosted atomic scale modelling approaches, advanced synthesis, high-throughput catalytic testing and state of the art characterization, we have developed a Cu-Al-Ga system that produces methanol and dimethyl ether (in different ratios) at highly competitive performance characteristics. The elemental composition of the Cu-Al-Ga catalysts was optimized towards a low gallium content to favor economic feasibility. The final lead composition with around 1 wt.% Ga content showed high activity while the ratio between MeOH and DME can be precisely adjusted by the reaction conditions in terms of temperature and syngas composition. Even in CO2 rich syngas flows, the catalyst remains active and selective towards the primary products. In addition, we introduce an advanced simulation protocol for studying potential surface changes under reactive condition to shed light on potential dynamical active site formations and their impact on reaction mechanisms.