Although numerous supported metal-oxide heterogeneous catalysts are effective for CO2 hydrogenation, it remains extremely challenging to achieve high C1 product selectivity. Specific structural features of metal-oxide heterogeneous catalysts are known to promote high CO2 hydrogenation activity, selectivity to a specific C1 product, or both. In particular, nanocatalysts derived from structured materials such as metal phyllosilicates (PS) often exhibit superior CO2 hydrogenation activity as compared to catalysts with conventional supports due to their unique structures. This work focuses on the synthesis and characterization of Cu-Zn phyllosilicates with tunable Cu:Zn compositions through a Reactive Laser Ablation in Liquid (RLAL) approach, a “green’’ technique that is being increasingly used to produce unique nanostructures with exotic metastable phases. The Cu-only nanocatalyst is comprised of Cu-PS fibrous structures supporting ~2 nm Cu2O clusters. Preliminary CO2 hydrogenation measurements performed on the Cu-PS catalyst resulted in 22–28% selectivity towards CH3OH, and 0.4–0.7% selectivity towards CH4, with the remaining product being CO. The addition of Zn did not alter the formation of the 2nm clusters or the Cu-PS structures and it prompted the formation of Zn-PS and ZnO phases. Preliminary results reveal Cu-Zn-PS samples have increased selectivity towards methanol (~50%). The effects of the addition of Zn on the Cu-PS active sites will be discussed.

Synthesis of Cu-Zn phyllosilicate catalysts for CO2 hydrogenation via fs-RLAL

ACS Fall 2021

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