Ultrathin Porous Carbon Nitride Bundles with an Adjustable Energy Band Structure toward Simultaneous Solar Photocatalytic Water Splitting and Selective Phenylcarbinol Oxidation

Angew Chem Int Ed Engl. 2021 Feb 23;60(9):4815-4822. doi: 10.1002/anie.202013753. Epub 2021 Jan 14.

Abstract

Actiniae-like carbon nitride (ACN) bundles were synthesized by the pyrolysis of an asymmetric supramolecular precursor prepared from L-arginine (L-Arg) and melamine. ACN has adjustable band gaps (2.25 eV-2.75 eV) and hollow microtubes with ultrathin pore walls, which enrich reaction sites, improve visible-light absorption and enhance charge separation. In the presence of phenylcarbinol, ACN exhibited excellent water-splitting ability (95.3 μmol h-1 ) and in the meanwhile phenylcarbinol was selectively oxidized to benzaldehyde (conversion of 90.9 %, selectivity of 99.7 %) under solar irradiation. For the concurrent reactions, 2 D isotope labeling, separation, and detection were conducted to confirm that the proton source of released hydrogen is water. The mechanism of water splitting and phenylcarbinol oxidation was also investigated.

Keywords: carbon nitride; phenylcarbinol oxidation; photocatalysis; supramolecular assembly; water splitting.