Carbon vacancies enriched carbon nitride nanotubes for Pd coordination environment optimization: Highly efficient...

The use of easily available solar energy to achieve pollutants efficient degradation and waste carbon resource CO₂ utilization under mild conditions is highly desired. Herein, novel carbon vacancies enriched nanotubes graphitic carbon nitride (SCNT-500) has been successfully fabricated via melamine (MA) supramolecular hydrogen-bonded self-assembly in the presence of H₂SO₄. Pd NPs loaded carbon vacancies enriched carbon nitride nanotubes (Pd/SCNT-500) were used for photocatalytic chlorophenols hydrodechlorination and CO₂ cycloaddition with styrene oxide. Up to 6.93 s^-1 4-chlorophenol hydrodechlorination TOF and obviously improved CO₂ cycloaddition efficiency could be realized with Pd/SCNT-500. The improved photocatalytic efficiency should be related to the morphology and carbon vacancies based Pd coordination environment optimization. Such as, the surface area increased nanotubes structure promoted light harvesting along with photoelectrons and holes generation; the carbon vacancies improved excited electrons capture, photoinduced carriers recombination inhibition along with substrates adsorption with electron rich Pd NPs. Mechanism studies not only demonstrated the important role of atomic hydrogen and Pd coordination environment optimization in the chlorophenols hydrodechlorination, but also confirmed the promotion ability of photogenerated electrons on CO₂ cycloaddition.