A Cocrystal Precursor Strategy for Carbon-Rich Graphitic Carbon Nitride toward High-Efficiency Photocatalytic Overall Water Splitting

Direct and efficient photocatalytic overall water splitting is crucial for the sustainable conversion and storage of renewable solar energy. Herein, we present the design of a carbon-rich graphitic carbon nitride (C(co)-C(3)N(4)), prepared from a layered molecular cocrystal precursor. The cocrystal microsheets were synthesized using a facile hydrothermal process. Following two-step thermal treatment and liquid exfoliation, the product maintains the 2D morphology owing to the toptactic transformation process. The C(co)-C(3)N(4) exhibits an enhanced photogenerated electron-hole separation, high charge transport capacity, and prolonged lifetime of the carriers, relative to the g-C(3)N(4) system. In the absence of any sacrificial reagent or co-catalyst, the C(co)-C(3)N(4) microsheets exhibit a high photocatalytic activity. The work presented in this report supplies a cocrystal route for the orderly molecular self-assembly of precursor materials to tailor the chemical compositions and electronic structures. Moreover, the generation of a highly efficient water-splitting photocatalyst has larger implications for sustainable energy applications.