A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol
Апстракт
Non-heme (L)Fe-III and (L)Fe-III-O-Fe-III(L) complexes (L=1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)-ethan-1-amine) underwent reduction under irradiation to the Fe-II state with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and DFT studies support a mechanism in which irradiation results in charge-transfer excitation of a Fe-III-mu-O-Fe-III complex to generate [(L)Fe-IV=O](2+) (observed transiently during irradiation in acetonitrile), and an equivalent of (L)Fe-II. Under aerobic conditions, irradiation accelerates reoxidation from the Fe-II to the Fe-III state with O-2, thus closing the cycle of methanol oxidation to methanal.
Кључне речи:
diiron complexes / iron / oxidation / photochemistry / reaction mechanismsИзвор:
Angewandte Chemie (International Edition), 2018, 57, 12, 3207-3211Издавач:
- Wiley-V C H Verlag Gmbh, Weinheim
Финансирање / пројекти:
- Рационални дизајн и синтеза биолошки активних и координационих једињења и функционалних материјала, релевантних у (био)нанотехнологији (RS-MESTD-Basic Research (BR or ON)-172035)
- SolCat - Shedding light on catalyst systems for a brighter future with green oxidation chemistry (EU-FP7-279549)
- Center for Information Technology of the University of Groningen
- Labex ARCANE [ANR-11-LABX-003]
- Chinese Scholarship Council (CSC)
- COST association action ECOSTBio (STSM) [CM1305, 38503]
DOI: 10.1002/anie.201712678
ISSN: 1433-7851
PubMed: 29334586
WoS: 000426759900036
Scopus: 2-s2.0-85042067927
Колекције
Институција/група
Hemijski fakultet / Faculty of ChemistryTY - JOUR AU - Chen, Juan AU - Stepanović, Stepan AU - Draksharapu, Apparao AU - Gruden-Pavlović, Maja AU - Browne, Wesley R. PY - 2018 UR - https://cherry.chem.bg.ac.rs/handle/123456789/2104 AB - Non-heme (L)Fe-III and (L)Fe-III-O-Fe-III(L) complexes (L=1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)-ethan-1-amine) underwent reduction under irradiation to the Fe-II state with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and DFT studies support a mechanism in which irradiation results in charge-transfer excitation of a Fe-III-mu-O-Fe-III complex to generate [(L)Fe-IV=O](2+) (observed transiently during irradiation in acetonitrile), and an equivalent of (L)Fe-II. Under aerobic conditions, irradiation accelerates reoxidation from the Fe-II to the Fe-III state with O-2, thus closing the cycle of methanol oxidation to methanal. PB - Wiley-V C H Verlag Gmbh, Weinheim T2 - Angewandte Chemie (International Edition) T1 - A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol VL - 57 IS - 12 SP - 3207 EP - 3211 DO - 10.1002/anie.201712678 ER -
@article{ author = "Chen, Juan and Stepanović, Stepan and Draksharapu, Apparao and Gruden-Pavlović, Maja and Browne, Wesley R.", year = "2018", abstract = "Non-heme (L)Fe-III and (L)Fe-III-O-Fe-III(L) complexes (L=1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)-ethan-1-amine) underwent reduction under irradiation to the Fe-II state with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and DFT studies support a mechanism in which irradiation results in charge-transfer excitation of a Fe-III-mu-O-Fe-III complex to generate [(L)Fe-IV=O](2+) (observed transiently during irradiation in acetonitrile), and an equivalent of (L)Fe-II. Under aerobic conditions, irradiation accelerates reoxidation from the Fe-II to the Fe-III state with O-2, thus closing the cycle of methanol oxidation to methanal.", publisher = "Wiley-V C H Verlag Gmbh, Weinheim", journal = "Angewandte Chemie (International Edition)", title = "A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol", volume = "57", number = "12", pages = "3207-3211", doi = "10.1002/anie.201712678" }
Chen, J., Stepanović, S., Draksharapu, A., Gruden-Pavlović, M.,& Browne, W. R.. (2018). A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol. in Angewandte Chemie (International Edition) Wiley-V C H Verlag Gmbh, Weinheim., 57(12), 3207-3211. https://doi.org/10.1002/anie.201712678
Chen J, Stepanović S, Draksharapu A, Gruden-Pavlović M, Browne WR. A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol. in Angewandte Chemie (International Edition). 2018;57(12):3207-3211. doi:10.1002/anie.201712678 .
Chen, Juan, Stepanović, Stepan, Draksharapu, Apparao, Gruden-Pavlović, Maja, Browne, Wesley R., "A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol" in Angewandte Chemie (International Edition), 57, no. 12 (2018):3207-3211, https://doi.org/10.1002/anie.201712678 . .