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In the pursuit of carbon neutrality, the catalytic hydrogenation of CO₂ using renewable H₂ is considered a promising route for the production of fuels and chemicals, while its integration with carbon capture and utilization processes (ICCU) provides an alternative and innovative approach for the synthesis of value-added products.¹ Even though the formation of C₁ molecules by CO/CO₂ hydrogenation is well established, the synthesis of C₂₊ products might be more attractive due to several advantages, such as a higher volumetric energy density.² In this work, structure-function relationships for the selective formation of C₂₊ products by CO₂ hydrogenation in direct and tandem reactions as well as the implementation of ICCU processes are investigated. Firstly, the chemical composition of spinel precursors AB₂₋ₓRhₓO₄ ((A,B) = Mn, Cu, Fe, Zn) is systematically varied, leading to differences in the activity and the products distribution (C₁ and C₂₊ oxygenates and hydrocarbons), which can be related to Rh⁰ exsolution and partial reduction of further spinel components as analyzed by NAP-XPS. Another approach is the development of nanostructured tandem core-shell catalysts for the stepwise conversion of CO₂-to-methanol and methanol-to-ethylene within the same operational window. Such rational design is guided by detailed operando investigations to elucidate the reaction pathway and reaction intermediates. In addition, CeO₂-supported metal particles are prepared by (co)precipitation as potential systems for ICCU. Attractive adsorption capacities under various CO₂ feeds (pure CO₂ and CO₂ from air), even at elevated temperatures (up to 200 ᵒC) are observed, as well as interesting catalytic performance in CO₂ hydrogenation reaction. The aforementioned findings suggest that the rational design of catalysts is essential in order to develop new hydrogenation routes for the utilization of CO₂.
1. Li, J., He,X., & Hu, R. Integrated Carbon Dioxide Capture and Utilization for the Production of CH₄, Syngas and Olefins over Dual-Function Materials. ChemCatChem 16, (2024).
2. Prieto, G. Carbon Dioxide Hydrogenation into Higher Hydrocarbons and Oxygenates: Thermodynamic and Kinetic Bounds and Progress with Heterogeneous and Homogeneous Catalysis. ChemSusChem. 10, 1056-1070 (2017).
