The excellent photocatalytic overall water splitting activity of TpPa-1-COF excited via MOF derived FeP-PC and α-Fe2O3 dual cocatalysts

Novel Fe-MOF-derived α-Fe2O3 and FeP-PC was designed and adopted as dual co-catalysts to facilitate the separation and utilization efficiency of charge carriers and activate the overall water splitting performance of the ketoenamine based TpPa-1-COF, with both the porous α-Fe2O3 and FeP-PC acting as the framework supporting to effectively prevent the agglomeration of TpPa-1-COF during the fabrication and photocatalytic process. Meanwhile, the construction of Z-scheme heterostructures and the connection of covalent bonds in the interface of α-Fe2O3/TpPa-1-COF/FeP-PC effectively facilitate the separation and transport of charge. Consequently, the optimal α-Fe2O3/TpPa-1-COF/FeP-PC excites very competitive photocatalytic H2 (97.45 μmol h−1 g−1) and O2 (48.68 μmol h−1 g−1) release rates, respectively, in comparison with most COFs and even some C3N4 based photocatalyst. [Display omitted] •α-Fe2O3 as an oxidation co-catalyst endow with sufficient oxidation sites to promote oxygen evolution kinetics.•FeP-PC is identified as a reduction co-catalyst to accelerate hydrogen evolution and accelerate the interface charge transfer.•The connection of covalent bonds in heterostructures effectively facilitate the separation and transport of charge.•The porous α-Fe2O3 and FeP-PC acting as the framework supporting could effectively prevent the agglomeration of TpPa-1-COF.•Optimal heterostructures excited competitive photocatalytic overall water splitting efficiency. Covalent organic frameworks (COFs) as an emerging porous material have exhibited excellent application prospects in the field of photocatalysis. Nevertheless, the overall water splitting using solar energy by COF-based photocatalysts remains a huge challenge due to the rapid charge recombination and insufficient redox catalytic capacity. Herein, for the first time, the novel Fe-MOF-derived α-Fe2O3 and FeP-PC was designed and adopted as dual co-catalysts to facilitate the separation and utilization efficiency of charge carriers and activate the overall water splitting performance of the ketoenamine based TpPa-1-COF, with both the porous α-Fe2O3 and FeP-PC acting as the framework supporting to effectively prevent the agglomeration of TpPa-1-COF during the fabrication and photocatalytic process. Meanwhile, the construction of Z-scheme heterostructures and the connection of covalent bonds in the interface of α-Fe2O3/TpPa-1-COF/FeP-PC effectively facilitate the separation and transport of charge. Consequently, the opti