| Yazarlar (2) |
Prof. Dr. Emine Esra KASAPBAŞI
İstanbul Aydın Üniversitesi, Türkiye |
Myung-Hwan Whangbo
Nc State University, Amerika Birleşik Devletleri |
| Özet |
| Recently it was discovered that the iron coordination complex L(N4)Fe(II)(OTf)(2) (1) (L(N4) = neutral tetraazadendate ligand and OTf = OSO(2)CF(3)) and its analogues are efficient water oxidizing catalysts (WOCs) in aqueous acidic solution with excess amount of ceric(IV) ammonium nitrate (CAN), [Ce(IV)(NO(3))(6)](NH(4))(2), as sacrificial oxidants. The probable mechanism of water oxidation by these catalysts was explored on the basis of density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations for 1 as a representative WOC. We examined the conversion of 1 to the resting intermediate [L(N4)Fe(IV)(O)(OH(2))](2+) [2(IV)] as well as two catalytic cycles involving 2(IV): one proposed by Fillol et al. [Nat. Chem. 2011, 3, 1] in which the Fe oxidation states of the intermediate species vary from +2 to +5, and the alternative cycle in which they remain constant at +4. In addition, we investigated the role of the sacrificial oxidant CAN in driving the catalytic cycle. Our DFT and TD-DFT calculations confirm the experimental observation that 2(IV) is the resting species, and indicate that the catalytic cycle in which the Fe oxidation states of the intermediate species remain at +4 is energetically more favorable. |
| Anahtar Kelimeler |
| Makale Türü | Özgün Makale |
| Makale Alt Türü | SSCI, AHCI, SCI, SCI-Exp dergilerinde yayınlanan tam makale |
| Dergi Adı | Inorganic Chemistry |
| Dergi ISSN | 0020-1669 Wos Dergi Scopus Dergi |
| Dergi Tarandığı Indeksler | SSCI |
| Dergi Grubu | Q4 |
| Makale Dili | İngilizce |
| Basım Tarihi | 01-2012 |
| Cilt No | 51 |
| Sayı | 1 |
| Sayfalar | 10850 / 10855 |
| Doi Numarası | 10.1021/ic3013359 |
| Atıf Sayıları | |
| WoS | 20 |
| SCOPUS | 20 |
| Google Scholar | 27 |
