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Diiron Dithiolate Complex Induced Helical Structure of Histone and Application in Photochemical Hydrogen Generation

Hu, Xiantao, Chen, Weijian, Li, Shuyi, Sun, Jian, Du, Ke, Xia, Qiuyu, Feng, Fude
ACS applied materials & interfaces 2019 v.11 no.22 pp. 19691-19699
aqueous solutions, calves, catalysts, histones, hydrogen production, hydrophobicity, lysine, moieties, photocatalysis, thymus gland
Very-lysine-rich calf thymus histone proteins form disordered structure and hydrophobic interaction-driven aggregates in weakly acidic solution. We reported that the conjugation of diiron dithiolate complex to the lysine residues induced formation of helical conformation and condensed nanoassemblies with a high loading capacity up to 18.7 wt %. The incorporated diiron dithiolate complex showed photocatalytic activity for hydrogen evolution in aqueous solutions, with a turnover number (based on [FeFe] catalyst moiety) up to 359 that was more than 6 times that of the free catalyst. The increase of helical conformation in proteins was well correlated to the increasing enhancement of photocatalytic activity. We demonstrated that the [FeFe]–hydrogenase-mimic biohybrid system based on the photocatalyst-induced protein conformational conversion and reassembly is efficient for hydrogen generation regardless of the relatively large size.