Research Projects

This project aims to develop innovative catalytic systems for the hydrogenation of challenging carbonyl derivatives, as well as CO₂, and CO to the corresponding C1 feedstocks and higher alcohols. The proposed heterogeneous catalysts employed in this project offer a hybrid approach, combining the mechanistic insights and selectivity of homogeneous catalysis with the robustness of heterogeneous systems. Our primary focus will be on the synthesis of various NHC-stabilized metal nanoparticles which will be utilized as catalysts. Several NHC ligand precursors incorporated with functionalities like amines, alcohols, and thiols will be synthesized (details see in other technical details). These functionalities, designed near metal nanoparticles, enhance coordination with carbonyl groups, therefore activation under mild conditions as well as facilitate the hydrogen activation via metal-ligand cooperation (MLC). The NHC ligands will then be incorporated into metal nanoparticles, which will be utilized for catalytic transformations. Using this strategy, initially, we will be focusing on the hydrogenation of various challenging carbonyl derivatives such as esters, amides, carbonates, and urea under mild reaction conditions. Next, our focus will be on the catalytic hydrogenation of CO₂. The catalytic hydrogenation of CO₂ can lead to their formal oxidation products such as formic acid (2 electron reduction), formaldehyde (4 electron reduction), and methanol (6 electron reduction) as well as higher alcohols, thus delivering a range of valuable chemicals and energy carriers. Our approach focuses on utilizing functionalized NHC-modified heterogeneous catalysts, designed for enhanced efficiency. The carbonyl functionality generated in situ from CO₂ can easily coordinate with the NHC-ligand backbone, enabling easy hydride transfer from the metal center to facilitate the reduction process. These catalysts, when combined with carefully selected additives, are expected to deliver selective different C1 products and higher alcohols with superior performance by achieving high turnover numbers, frequency, excellent selectivity, and robust recyclability, ensuring sustainable and practical catalytic processes. Furthermore, we aim to extend our protocol to explore the hydrogenation of carbon monoxide into methanol and higher alcohols, offering a sustainable approach to synthesize these vital molecules. Previous research on NHC-modified nanoparticles has demonstrated their potential for CO coordination, suggesting a high likelihood of successful CO activation in the presence of mild bases and alcoholic solvents. Building on these findings, we will investigate the hydrogenation of CO using our catalysts, focusing on two primary pathways: in-situ formed formate and formamide hydrogenation. By optimizing reaction conditions, such as temperature, pressure, and the choice of solvents, we will aim to achieve efficient conversion under mild conditions.