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Seeing the key intermediates in bioinspired nonheme iron complex-catalyzed water oxidation
- Title
- Seeing the key intermediates in bioinspired nonheme iron complex-catalyzed water oxidation
- Authors
- Hong; Young Hyun; Lee; Yong-Min; Fukuzumi; Shunichi; Nam; Wonwoo
- Ewha Authors
- 남원우; Shunichi Fukuzumi; 이용민
- SCOPUS Author ID
- 남원우
; Shunichi Fukuzumi![scopus](/images/layout/icon2.png)
; 이용민![scopus](/images/layout/icon2.png)
![scopus](/images/layout/icon2.png)
![scopus](/images/layout/icon2.png)
- Issue Date
- 2024
- Journal Title
- Chem
- ISSN
- 2451-9308
- Citation
- Chem vol. 10, no. 6, pp. 1755 - 1765
- Keywords
- artificial photosynthesis; bioinorganic chemistry; key intermediates; oxygen evolution; photosystem II; reaction mechanism; SDG7: Affordable and clean energy; transient absorption spectroscopy; water oxidation
- Indexed
- SCIE; SCOPUS
![scopus](/images/layout/scopus2.gif)
- Document Type
- Article
- Abstract
- Inspired by the oxygen-evolving complex in photosystem II, the nature of intermediates and the oxygen–oxygen bond formation mechanism in photocatalytic water oxidation have been the topic of current research. Herein, we report that the key intermediates and the O–O bond formation step in the catalytic water oxidation by [RuIII(bpy)3]3+ or the excited state of 2,3-dichloro-5,6-dicyano-p-benzoquinone (3DDQ∗) with a nonheme iron complex, [FeII(dpaq)]+, were captured and identified. Especially, two keyintermediates, such as an iron(V)-oxo ([FeV(dpaq)(O)]2+ or [FeIV(dpaq cation radical)(O)]2+) and an iron(III)-hydroperoxo species ([FeIII(dpaq)(OOH)]+), were captured in the water oxidation reactions; [FeV(dpaq)(O)]2+ (or [FeIV(dpaq cation radical)(O)]2+) was detected using transient absorption spectroscopy in the oxidation of [FeIV(dpaq)(O)]+ by 3DDQ∗, whereas the formation of [FeIII(dpaq)(OOH)]+ was directly observed by reacting [FeIV(dpaq)(O)]+ with [RuIII(bpy)3]3+ or 3DDQ∗ in the presence of water. The evolution of O2 upon the oxidation of [FeIII(dpaq)(OOH)]+ by DDQ was also demonstrated in this study. © 2024 Elsevier Inc.
- DOI
- 10.1016/j.chempr.2024.01.027
- Appears in Collections:
- 자연과학대학 > 화학·나노과학전공 > Journal papers
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