Tracking an Fe V (O) Intermediate for Water Oxidation in Water.

Autor: Wei XZ; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Ding TY; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Wang Y; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Yang B; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Yang QQ; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Ye S; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China., Tung CH; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China., Wu LZ; Key Laboratory of Photochemical Conversion and Optoelectronic Materials, New Cornerstone Science Laboratory, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.; School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2023 Sep 04; Vol. 62 (36), pp. e202308192. Date of Electronic Publication: 2023 Jul 24.
DOI: 10.1002/anie.202308192
Abstrakt: High-valent iron-oxo species are appealing for conducting O-O bond formation for water oxidation reactions. However, their high reactivity poses a great challenge to the dissection of their chemical transformations. Herein, we introduce an electron-rich and oxidation-resistant ligand, 2-[(2,2'-bipyridin)-6-yl]propan-2-ol to stabilize such fleeting intermediates. Advanced spectroscopies and electrochemical studies demonstrate a high-valent Fe V (O) species formation in water. Combining kinetic and oxygen isotope labelling experiments and organic reactions indicates that the Fe V (O) species is responsible for O-O bond formation via water nucleophilic attack under the real catalytic water oxidation conditions.
(© 2023 Wiley-VCH GmbH.)
Databáze: MEDLINE
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