One‐Pot N‐Alkylation of Amines over Ni(II) Embedded Reusable Porous Organic Polymer via Borrowing Hydrogen Strategy

Abstract The first‐of‐its‐kind, one‐pot N ‐alkylation reaction of amines over Ni(II) impregnated porous organic polymer of highly dense N ‐rich skeleton is reported. The primeval Ni(II) decorated hollow spherical porous polymer is synthesized and employed in a series of catalytic reactions involving C−N bond formation. The catalytic reactions are optimised to yield the desired product highlighting the role of different substituents present on the reactants towards the overall selectivity and efficiency. The detailed reaction mechanism is corroborated with computation validating a three‐step arrow formalism viz . dehydrogenation of the alcohol, condensation with amines to generate the imine as intermediate followed by hydrogenation by a borrowing strategy to yield the final product. The role of the bare support material in the first step and that of the Ni(II) centres of the support material in the third step is marked as pivotal for the forward reaction to proceed with enriching sustainability and feasibility.