LaTaON2 porous single crystals (PSCs), integrating structural coherence and porous microstructures, will warrant promising photocatalytic performance. The absence of grain boundaries in PSCs ensures rapid photocarrier transportation from bulk to the surface, thereby mitigating photocarriers’ recombination. Porous microstructures not only provide ample reachable surface to host photochemical reactions but also reinforce photon-matter interactions by additional photon reflection/scattering. Here, we have synthesized LaTaON2 PSCs via a topotactic route and show significantly improved photocatalytic performance. Efficient water oxidation into O2 has been realized by LaTaON2 PSCs with an apparent quantum efficiency as high as 5.7% at 420 ± 20 nm. Stable overall water splitting into stoichiometric H2 and O2 has also been achieved in a Z-scheme setup using LaTaON2 PSCs as the O2 evolution photocatalyst. These results not only prove that PSCs facilitate photocarrier migrations, which in turn deliver exceptional photocatalytic performance, but also imply that PSCs are useful to reinvigorate conventional semiconductor photocatalysts toward efficient solar energy conversions.

The one-atom substitution (O, S, Se) strategy shows great importance in the design of D–A type organic porous conjugated polymers for photocatalytic hydrogen evolution.

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