Carbon-based Single-atom Catalyst for Direct CO2 Hydrogenation to Fuel-range (C5+) Hydrocarbons

To address climate change and achieve carbon neutrality, innovative technologies are needed to convert CO2 into fuels and chemicals. Among the several strategies, the direct conversion of CO2 and green H2 into fuel-range hydrocarbons (C5+) presents a sustainable alternative to fossil-based processes, ensuring energy security, especially in hard-to-electrify sectors such as shipping and aviation. In general, this tandem process through the RWGS-FT pathway demands at least two different types of active sites in a catalytic system for the formation of primary intermediate CO and subsequent consumption through C-C coupling and chain growth. Although Fe, Co, and Ru-based nanomaterials are well studied for this process, they have critical limitations, including low CO formation, limited C5+ selectivity, and insufficient activity under mild conditions. The core of this proposal is to construct single-atom sites (Fe or Co) within doped/co-doped carbon that combines the advantages of single-metal dispersion for *CO formation and stabilization and dynamic aggregation and carburization under reaction conditions for obtaining high C5+ selectivity. Therefore, this research will focus on tailoring the coordination environment at the atomic scale for achieving C5+ selectivity beyond the ASF limit (48%).This work will adopt a multidisciplinary approach, integrating a simple catalyst synthesis strategy with advanced characterization and in-situ/operando spectroscopy studies. Special attention will be given to probe dynamic structural and electronic changes under reaction conditions. By establishing a structure-activity relationship, fundamental insights into how a single site and its structural evolution affect the catalytic performance will be achieved. The expected outcome of this project is to develop a robust and scalable single-atom catalyst for CO2 valorization, contributing to the EU's Green Deal goal and enhancing researchers’ skills in both catalysis and leadership.