Herein, we have demonstrated the design and synthesis of a novel Ni-immobilized MOF as heterogeneous catalyst for the dehydrogenation of N-heterocycles. A series of five and six-membered N-heteroarenes bearing one or more heteroatoms were synthesized in up to 98 % yield (>
33 examples). Late stage functionalization to the synthesis of β-glucuronides inhibitor, antimalarial drug quinine, and the nonsteroidal anti-inflammatory drug (NSAID) indomethacin were obtained under milder reactions conditions. A series of mechanistic studies revealed the detection of H