Three complexes comprising ferrocenyl‐2‐pyridylimine and three d10 transition metal centers viz. Zn (II), Cd (II), and Hg (II) having formula [M (FcCH=NCH2(2‐py)] (M = Zn (II) (Zn‐Fc), Cd (II) (Cd‐Fc), and Hg (II) (Hg‐Fc); Fc = Ferrocene) are synthesized and their characterization have been done using microanalytical technique, FT‐IR and NMR spectroscopic methods. The optimized molecular geometries for all the three ferrocene‐based complexes revealed that the coordination geometries around the d10‐metal centers are distorted tetrahedral. The application of these complexes as sensitizers and co‐sensitizers/co‐adsorbents have been assessed in dye sensitized solar cells (DSSCs). Amid the three co‐sensitizers/co‐adsorbent based the DSSC set‐ups, the assembly fabricated using Zn‐Fc/N719 displayed superior performance with 5.71 ± 0.04% efficiency (η) indicating enhancement in the DSSC performance than to the set‐up constructed using solely N719 (η = 4.20 ± 0.05%).
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