Gold(II) Porphyrins in Photoinduced Electron Transfer Reactions

Chemistry : a European Journal
Sebastian PreißKatja Heinze

Abstract

In the context of solar-to-chemical energy conversion, inspired by natural photosynthesis, the synthesis, electrochemical properties and photoinduced electron-transfer processes of three novel zinc(II)-gold(III) bis(porphyrin) dyads [ZnII (P)-AuIII (P)]+ are presented (P: tetraaryl porphyrin). Time-resolved spectroscopic studies indicated ultrafast dynamics (k ET 1 >1010  s-1 ) after visible-light excitation, which finally yielded a charge-shifted state [ZnII (P⋅+ )-AuII (P)]+ featuring a gold(II) center. The lifetime of this excited state is quite long due to a comparably slow charge recombination (k BET 2 ≈3×108  s-1 ). The [ZnII (P⋅+ )-AuII (P)]+ charge-shifted state is reductively quenched by amines in bimolecular reactions, yielding the neutral zinc(II)-gold(II) bis(porphyrin) ZnII (P)-AuII (P). The electronic nature of this key gold(II) intermediate, prepared by chemical or photochemical reduction, is elucidated by UV/Vis, X-band EPR, gold L3 -edge X-ray absorption near edge structure (XANES) and paramagnetic 1 H NMR spectroscopy as well as by quantum chemical calculations. Finally, the gold(II) site in ZnII (P)-AuII (P) is thermodynamically and kinetically competent to reduce an aryl azide to the corr...Continue Reading

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