Selective catalytic generation of hydrogen over covalent organic polymer supported Pd nanoparticles (COP-Pd)

[Display omitted] •A facile two-steps method is used for the preparation of Triazine-based COP.•Pd-loaded TA-COP was applied for H2 generation from formic acid dehydrogenation.•High hydrogen content was achieved under sonication and at higher temperature.•The Ea for the formic acid dehydrogenation was calculated to be 28.95 kJ/mol.•Pd-NPs@TA-COP showed high stability even after 7 repetitions. Formic acid (FA) has long been regarded as a cheap and non-toxic hydrogen storage material due to its effective production of hydrogen in mild conditions. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Here, a porous Triazine-based covalent organic polymer (TA-COP) was fabricated via the Schiff base condensation reaction. Then, experimental studies on palladium nanoparticles supported on a nitrogen-rich TA-COP substrate are combined for FA dehydrogenation to selective production of CO2 and H2 under mild conditions. The Pd(0)@TA ­ COP showed high catalytic activity (TOF up to 233 h−1) and high hydrogen selectivity for the dehydrogenation of FA at 328 K. Our study demonstrated that the synergistic effects between the nitrogen-rich TA-COP support and Pd nanoparticles play a critical role in the efficient catalytic dehydrogenation of formic acid. This work provides a feasible strategy to design high-performance COP-based heterogeneous catalysts for catalyzing formic acid dehydrogenation.