Suppressing Reverse Processes in the Perylene Diimide/Strontium Titanate Z-Scheme Heterojunction for Efficient Photocatalytic Overall Water Splitting

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Abstract Photocatalytic overall water splitting is promising for sustainable H2 supply but is hindered by severe charge recombination and the reverse reaction. Herein, we design a novel organic/inorganic heterojunction by coupling π-conjugated perylene diimide polymer (PDIP) with aluminum-doped strontium titanate (SrTiO3:Al) to suppress these reverse processes for boosting photocatalytic H2 evolution. In situ characterizations reveal a direct Z-scheme charge transfer pathway between PDIP and SrTiO3:Al, which promotes high‑energy charge carrier separation and suppresses the reverse reaction by spatially segregating the H2 and O2 evolution sites onto SrTiO3:Al and PDIP, respectively. Further, combined with selective co-catalyst engineering for preventing H2 and O2 from contacting on the catalyst surface, these reverse processes are fundamentally suppressed. Consequently, the PDIP/SrTiO3:Al heterojunction exhibits substantially enhanced photocatalytic activity for overall water splitting, achieving an H2 evolution rate 11.8 times higher than that of pristine SrTiO3:Al. This dual-suppression strategy provides a validated blueprint for highly efficient solar-to-hydrogen conversion.

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