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Hierarchical Z-scheme photocatalyst g-C3N4/Au/ZnIn2S4 was constructed and applied for highly enhanced visible-light photocatalytic NO removal and CO2 conversion.

Direct water splitting over photocatalysts is a prospective strategy to convert solar energy into hydrogen energy. Nevertheless, because of the undesirable electron accumulation at the surface, the overall water‐splitting efficiency is seriously restricted by the poor charge separation/transfer ability. Here, an all‐organic donor–acceptor (D‐A) system through crafting carbon rings units‐conjugated tubular graphitic carbon nitride (C‐TCN) is proposed. Through a range of characterizations and theoretical calculations, the incorporation of carbon rings units via continuous π‐conjugated bond builds a D‐A system, which can drive intramolecular charge transfer to realize highly efficient charge separation. More importantly, the tubular structure and the incorporated carbon rings units cause a significant downshift of the valence band, of which the potential is beneficial to the activation for O2 evolution. When serving as photocatalyst for overall water splitting, C‐TCN displays considerable performance with H2 and O2 production rates of 204.6 and 100.8 µmol g−1 h−1, respectively. The corresponding external quantum efficiency reaches 2.6% at 405 nm, and still remains 1.7% at 420 nm. This work demonstrates that the all‐organic D‐A system conceptualized from organic solar cell can offer promotional effect for overall water splitting by addressing the charge accumulation problem rooted in the hydrogen evolution reaction.

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Photocatalytic reduction of CO 2 provides an opportunity to reach carbon neutrality, by which CO 2 emissions from fuel consumption can be converted back to fuels. The challenge is to explore materials with high charge separation efficiency and effective CO 2 adsorption capacity to boost the photoreduction of CO 2 . Here we report that a 2D heterostructure comprised of Co 3 O 4 /2D g-C 3 N 4 (COCN) can provide enhanced photocatalytic reduction of CO 2 to CO, yielding a CO production rate of 419 μmol g −1 h −1 with a selectivity of 89.4%, which is 13.5 and 2.6 times higher than that of pure 2D g-C 3 N 4 and Co 3 O 4 . The enhanced photocatalytic performance arises from (i) enhanced light absorption ability and charge separation efficiency originating from the unique 2D heterostructure connected through specifically exposed facet interfaces and (ii) favorable CO 2 adsorption capacity. The study may provide insight for the establishment of a heterostructure-based photocatalytic system toward CO 2 reduction.