Multifunctional Catalyst Combination for the Direct Conversion of CO2 to Propane

Adrian Ramirez; Pierfrancesco Ticali; Davide Salusso; Tomas Cordero-Lanzac; Samy Ould-Chikh; Christian Ahoba-Sam; Aram L Bugaev; Elisa Borfecchia; Sara Morandi; Matteo Signorile; Silvia Bordiga; Jorge Gascon; Unni Olsbye

doi:10.1021/jacsau.1c00302

Multifunctional Catalyst Combination for the Direct Conversion of CO₂ to Propane

JACS Au. 2021 Sep 2;1(10):1719-1732. doi: 10.1021/jacsau.1c00302. eCollection 2021 Oct 25.

Affiliations

¹ KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology, Thuwal 23955, Saudi Arabia.
² Department of Chemistry, NIS Center and INSTM Reference Center, University of Turin, Turin 10125, Italy.
³ SMN Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, Oslo N-0315, Norway.
⁴ The Smart Materials Research Institute, Southern Federal University, Sladkova 178/24, Rostov-on-Don 344090, Russian Federation.

Abstract

The production of carbon-rich hydrocarbons via CO₂ valorization is essential for the transition to renewable, non-fossil-fuel-based energy sources. However, most of the recent works in the state of the art are devoted to the formation of olefins and aromatics, ignoring the rest of the hydrocarbon commodities that, like propane, are essential to our economy. Hence, in this work, we have developed a highly active and selective PdZn/ZrO₂+SAPO-34 multifunctional catalyst for the direct conversion of CO₂ to propane. Our multifunctional system displays a total selectivity to propane higher than 50% (with 20% CO, 6% C₁, 13% C₂, 10% C₄, and 1% C₅) and a CO₂ conversion close to 40% at 350 °C, 50 bar, and 1500 mL g^-1 h^-1. We attribute these results to the synergy between the intimately mixed PdZn/ZrO₂ and SAPO-34 components that shifts the overall reaction equilibrium, boosting CO₂ conversion and minimizing CO selectivity. Comparison to a PdZn/ZrO₂+ZSM-5 system showed that propane selectivity is further boosted by the topology of SAPO-34. The presence of Pd in the catalyst drives paraffin production via hydrogenation, with more than 99.9% of the products being saturated hydrocarbons, offering very important advantages for the purification of the products.