Ulusoy-Ghobadi, T. GamzeGhobadi, AmirBüyüktemiz, M.Akhüseyin Yıldız, E.Yıldız, D. B.Yağlıoğlu, H. G.Dede, Y.Özbay, Ekmel2021-02-282021-02-282020-021433-7851http://hdl.handle.net/11693/75649Herein, we establish a simple synthetic strategy affording a heterogeneous, precious metal‐free, dye‐sensitized photoelectrode for water oxidation, which incorporates a Prussian blue (PB) structure for the sensitization of TiO2 and water oxidation catalysis. Our approach involves the use of a Fe(CN)5 bridging group not only as a cyanide precursor for the formation of a PB‐type structure but also as an electron shuttle between an organic chromophore and the catalytic center. The resulting hetero‐functional PB‐modified TiO2 electrode demonstrates a low‐cost and easy‐to‐construct photoanode, which exhibits favorable electron transfers with a remarkable excited state lifetime on the order of nanoseconds and an extended light absorption capacity of up to 500 nm. Our approach paves the way for a new family of precious metal‐free robust dye‐sensitized photoelectrodes for water oxidation, in which a variety of common organic chromophores can be employed in conjunction with CoFe PB structures.EnglishDye-sensitizationPhotoelectrochemistryPrussian blueWater oxidationWater splittingArticle10.1002/anie.201914743