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Journal Articles New Journal of Chemistry Year : 2022

Photoactive silicon surfaces functionalized with high-quality and redox-active platinum diimine complex monolayers

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Abstract

New platinum diimine dichloro (PtCl2) and dithiolene (Ptdithiolene) complexes have been synthesized and covalently bound to hydrogen-terminated, oxide-free silicon(111) surfaces using a two-step procedure. This immobilization route resulted in the formation of ca. 2.0-2.5 nm-thick densely packed and perfectly clean Pt complex monolayers with the expected structure of the grafted molecular chains. The surface coverages of the attached PtCl2 and Ptdithiolene were electrochemically estimated at 8.9 x 10(-11) and 7.5 x 10(-11) mol cm(-2), respectively, corresponding to 0.07 PtCl2 and 0.06 Ptdithiolene per surface silicon atom. The Pt complex-functionalized photoactive silicon surfaces showed under simulated sunlight a redox activity similar to that observed for the complexes in solution at a non-photoactive electrode. The two one-electron reduction processes centered on the bipyridine ligand were however observed at much less negative potentials, owing to the photovoltage generated at the silicon/monolayer interface. These modified photocathodes showed great promise for solar photoelectrocatalysis, as exemplified with the photoassisted electrocatalytic reduction of CO2. Based on the measured cathodic photocurrent densities, the Ptdithiolene-modified surface showed superior catalytic performance.
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Dates and versions

hal-03606054 , version 1 (11-03-2022)

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Bruno Fabre, Franck Camerel, Soraya Ababou-Girard. Photoactive silicon surfaces functionalized with high-quality and redox-active platinum diimine complex monolayers. New Journal of Chemistry, 2022, 46 (8), pp.3667-3673. ⟨10.1039/d1nj05805c⟩. ⟨hal-03606054⟩
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