Executive Summary : | "The proposal aims to develop a heterogeneous metal-free pyridinic nitrogen-doped carbon material for hydrogenation and dehydrogenation reactions in sustainable chemical synthesis. With the world's growing population of over 9 billion people by 20501, the demand for ecologically and economically sustainable use of resources is increasing. Transition metal-catalyzed hydrogenation and dehydrogenation reactions are homogeneous, making reusable non-metal heterogeneous catalysis more comprehensible. Catalysis is one of the twelve principles of green chemistry, and this proposal focuses on using hetero atom modified carbon material as a reusable catalyst for hydrogenation and dehydrogenation reactions. Nitrogen-doped carbon material is particularly interested due to its numerous applications, including electrocatalysis for oxygen reduction reactions. The proposal uses the biocatalytic borrowing hydrogen concept by Turner et al., which uses carbon-nitrogen unsaturated bonds for hydrogen shuttles. The pyridine nucleotides' hydride transferability can be traced to their simple pyridine core, which oscillates between an aromatic pyridinium ion and a dearomatized dihydropyridine (DHP). The carbon material is post-functionalized with a hetero atom precursor to obtain DHPs and OHDs, with the preparation methods optimized to achieve the required properties.
The proposal also explores new approaches towards reductive amination of carbonyls and transfer hydrogenation of imines and enamines, which can be applied in sustainable synthesis of pharmaceuticals (APIs synthesis). The proposal also discusses C-C and C-N bond formations via borrowing hydrogen and their applications in sustainable synthesis of pharmaceuticals." |