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Two series of metallo‐(Zn(II), Mg(II), and Ru(II)) and free‐base phthalocyanines (Pcs) with a carboxyl anchoring group and well‐established bulky peripheral substituents (either tert‐butyl or bulky 2,6‐diisopropylphenoxy) were synthesized and tested as sensitizers in dye‐sensitized solar cells (DSSCs). The trend of photovoltaic efficiencies (PCEs) for free‐base and metallo Pcs followed the order Zn(II)Pc>Mg(II)Pc≫H2Pc...