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Site-Selective Real-Time Observation of Bimolecular Electron Transfer in a Photocatalytic System Using L-Edge X-Ray Absorption Spectroscopy*.


ABSTRACT: Time-resolved X-ray absorption spectroscopy has been utilized to monitor the bimolecular electron transfer in a photocatalytic water splitting system. This has been possible by uniting the local probe and element specific character of X-ray transitions with insights from high-level ab initio calculations. The specific target has been a heteroleptic [IrIII (ppy)2 (bpy)]+ photosensitizer, in combination with triethylamine as a sacrificial reductant and Fe3(CO)12 as a water reduction catalyst. The relevant molecular transitions have been characterized via high-resolution Ir L-edge X-ray absorption spectroscopy on the picosecond time scale and restricted active space self-consistent field calculations. The presented methods and results will enhance our understanding of functionally relevant bimolecular electron transfer reactions and thus will pave the road to rational optimization of photocatalytic performance.

SUBMITTER: Britz A 

PROVIDER: S-EPMC8048488 | biostudies-literature | 2021 Apr

REPOSITORIES: biostudies-literature

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Site-Selective Real-Time Observation of Bimolecular Electron Transfer in a Photocatalytic System Using L-Edge X-Ray Absorption Spectroscopy*.

Britz Alexander A   Bokarev Sergey I SI   Assefa Tadesse A TA   Bajnóczi Èva G ÈG   Németh Zoltán Z   Vankó György G   Rockstroh Nils N   Junge Henrik H   Beller Matthias M   Doumy Gilles G   March Anne Marie AM   Southworth Stephen H SH   Lochbrunner Stefan S   Kühn Oliver O   Bressler Christian C   Gawelda Wojciech W  

Chemphyschem : a European journal of chemical physics and physical chemistry 20210316 7


Time-resolved X-ray absorption spectroscopy has been utilized to monitor the bimolecular electron transfer in a photocatalytic water splitting system. This has been possible by uniting the local probe and element specific character of X-ray transitions with insights from high-level ab initio calculations. The specific target has been a heteroleptic [Ir<sup>III</sup> (ppy)<sub>2</sub> (bpy)]<sup>+</sup> photosensitizer, in combination with triethylamine as a sacrificial reductant and Fe3(CO)12 as  ...[more]

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