High Dispersed Pd Nanoparticles Anchored on Nanotubular Carbon Nitride for Hydrogen Production from Formic Acid

Abstract In this study, nanotubular carbon nitride (CN) was successfully synthesized via a supramolecular self‐assembly method using varied molar ratios of melamine (MA) to barbituric acid (BA). The resulting supported Pd catalysts demonstrated exceptional catalytic activity for hydrogen production through formic acid dehydrogenation, achieving an initial turnover frequency (TOF) of 1920.4 h −1 at 348 K. By systematically adjusting the MA:BA molar ratio, hydrothermal temperature, and reaction time, the chemical structure, morphology, and the type/content of nitrogen‐containing species in CN were tailored. Notably, the nature and distribution of nitrogen‐containing functional groups in nanotubular CN significantly modulated the electronic properties of Pd, thereby affecting the catalytic performance. The remarkable activity originated from the synergistic effect of Pd and pyrrolic N interactions, coupled with the small particle size and high dispersion of Pd nanoparticles.