Crystallized Poly(Triazine Imide) Decorated with Dynamically Coordinated Pd II Complex for Efficient Photocatalytic Overall Water Splitting

作者：Jiapeng Xu, Di Lu, Xinming Li, Renjie Li, Jing Zhang, Tianyou Peng · 发表于：ChemSusChem · 年份：2025 · DOI：10.1002/cssc.202500987 · 被引用次数：6 · 研究领域：Advanced Photocatalysis Techniques、Covalent Organic Framework Applications、Polyoxometalates: Synthesis and Applications

Exploring photocatalysts capable of overall water splitting without the need of sacrificial agents or external bias holds significant practical importance. Herein, crystallized poly(triazine imide) (cPTI) loaded with CoO x as oxygen evolution photocatalyst is decorated with (FFV) 2 PdCl 2 complex (FFV = Fluoflavin) for constructing a novel Z‐scheme heterojunction. The dynamic coordination between the Pd II ion and FFV ligands in (FFV) 2 PdCl 2 results in unsaturated Pd II active sites as the excellent hydrogen evolution photocatalyst. The resultant (FFV) 2 PdCl 2 /cPTI‐CoO x heterojunction delivers excellent overall water splitting activity with H 2 /O 2 yields up to 201/101 μmol h −1 under the illumination of Xe‐lamp and an apparent quantum yield of 19.8% at 365 nm. Mechanistic studies reveal that the Z‐scheme charge transfer mechanism in (FFV) 2 PdCl 2 /cPTI‐CoO x effectively promotes the photoinduced charge separation, while maintaining high redox capacity for overall water splitting. This work presents the first instance of integrating crystallized poly(triazine imide) with dynamically coordinated complex, paving a new way for manufacturing highly efficient overall water splitting system.