Photocatalysis is the most promising method for achieving artificial photosynthesis, but a bottleneck is encountered in finding materials that could efficiently promote the water splitting reaction. The nontoxicity, low cost, and versatility of photocatalysts make them especially attractive for this application. This study demonstrates that small amounts of α‐Fe 2 O 3 nanosheets can actively promote exfoliation of g‐C 3 N 4 , producing 2D hybrid that exhibits tight interfaces and an all‐solid‐state Z‐scheme junction. These nanostructured hybrids present a high H 2 evolution rate >3 × 10 4 µmol g ‐1 h ‐1 and external quantum efficiency of 44.35% at λ = 420 nm, the highest value so far reported among the family of g‐C 3 N 4 photocatalysts. Besides effectively suppressing the recombination of electron–hole pairs, this Z‐scheme junction also exhibits activity toward overall water splitting without any sacrificial donor. The proposed synthetic route for controlled production of 2D g‐C 3 N 4 ‐based structures provides a scalable alternative toward the development of highly efficient and active photocatalysts.
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