Carbon nitride (CN) has emerged as a promising photocatalyst,
recognized
for its visible-light sensitivity, high conduction band-edge position,
tunable electronic configuration, and environmental friendliness.
Despite these attributes, the practical application of CN is hindered
by challenges such as inefficient charge carrier separation, a narrow
light absorption range, and inherent n-type characteristics due to
nonstoichiometry. Here, we introduce a new postsynthetic functionalization
strategy that modifies CN with catechol quinone (CQ) to substantially
improve its photocatalytic performance through light-induced electron
polarization and extended light absorption. The key mechanism involves
promoted spatial charge separation at the CN–CQ interface,
leveraging the light-triggered oscillation of CQ between its electron
donor and acceptor states, corroborated by density functional theory
calculations. Moreover, CN–CQ conjugation broadens the photoactive
range of CN across the full spectrum of visible light due to lower-energy
electronic excitations arising from the midgap states introduced by
CQ. Under sunlight illumination, the CN–CQ conjugation increased
the photocatalytic activities of CN 2-fold for photochemical gold
ion reduction and hydrogen evolution. Our findings suggest that postsynthetic
functionalization with a redox-active moiety is a promising strategy
for enhancing the photocatalytic activity of CN.