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Generation of maghemite nanocrystals from iron–sulfur centres
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Banerjee, Samya, Omlor, Andreas, Wolny, Juliusz A., Han, Yisong, Lermyte, Frederik, Godfrey, Amy, O'Connor, Peter B., Schünemann, Volker, Danaie, Mohsen and Sadler, Peter J. (2019) Generation of maghemite nanocrystals from iron–sulfur centres. Dalton Transactions, 48 (26). pp. 9564-9569. doi:10.1039/C9DT00514E ISSN 1477-9226.
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WRAP-generation-maghemite-nanocrystals-iron–sulfur-centres-Sadler-2019.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution 4.0. Download (3197Kb) | Preview |
Official URL: http://dx.doi.org/10.1039/C9DT00514E
Abstract
Iron oxide nano-crystals 0.1–1.1 μm in diameter were generated on sulfur-doped amorphous carbon surfaces by electron beam irradiation of the novel 13e− high-spin complex [Fe(4-methyl-1,2-benzenedithiolate)2][NHEt3] encapsulated in a triblock copolymer. Possible relevance to iron nano-mineralization from Fe–S ferredoxin proteins and iron dysregulation in neurological disorders is discussed. Graphical abstract: Generation of maghemite nanocrystals from iron–sulfur centres Iron is an essential element for mammals and, amongst many other functions, plays an important role in the human brain.1 Recent research has indicated a strong association between iron dysregulation and Alzheimer's disease (AD), although it is unknown how the chemical and magnetic state of iron is linked to AD pathogenesis.2–4 Reports from Collingwood et al., and Dobson et al., for example, have shown the presence of iron oxide as the mixed oxidation state mineral, magnetite (Fe3O4) in AD tissue, a possible source of redox-active iron, but it remains unclear how this kind of iron mineral forms in the tissue.5,6 These unsolved and important questions have led us to consider how atomic resolution microscopy might provide new insight into nanoscale iron mineralization. Recently we reported methodology for studies of the nano-mineralisation of osmium, gold, ruthenium and iridium from their respective 1,2-dicarba-closo-dodecarborane-1,2-dithiolate complexes encapsulated in polymer micelles upon electron beam irradiation.7–9 Here we report the synthesis and characterization of the novel 13e− iron(iii) complex [Fe(4-methyl-1,2-benzenedithiolate)2][NHEt3] (1), containing Fe–S bonds analogous to those in the ubiquitous iron–sulfur ferredoxin proteins. Importantly, recent research has indicated a strong relationship between neurodegenerative disorders and defective Fe–S clusters.10,11 We have characterized complex 1 using Mössbauer, Raman and far-infra red spectroscopy, and investigated the generation of iron nanocrystals from 1 encapsulated in a poly(ethylene glycol)-block-poly(propylene glycol)-block-poly(ethylene glycol) polymer (Scheme 1) by electron beam irradiation, and used electron energy-loss spectra (EELS) to identify the oxidation state of iron and its coordination environment in the nanocrystals.
Item Type: | Journal Article | |||||||||||||||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry T Technology > TA Engineering (General). Civil engineering (General) |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Engineering > Engineering Faculty of Science, Engineering and Medicine > Science > Physics |
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Library of Congress Subject Headings (LCSH): | Iron oxides , Nanocrystals , Maghemite, Microscopy | |||||||||||||||||||||
Journal or Publication Title: | Dalton Transactions | |||||||||||||||||||||
Publisher: | Royal Society of Chemistry | |||||||||||||||||||||
ISSN: | 1477-9226 | |||||||||||||||||||||
Official Date: | 14 July 2019 | |||||||||||||||||||||
Dates: |
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Volume: | 48 | |||||||||||||||||||||
Number: | 26 | |||||||||||||||||||||
Page Range: | pp. 9564-9569 | |||||||||||||||||||||
DOI: | 10.1039/C9DT00514E | |||||||||||||||||||||
Status: | Peer Reviewed | |||||||||||||||||||||
Publication Status: | Published | |||||||||||||||||||||
Access rights to Published version: | Restricted or Subscription Access | |||||||||||||||||||||
Date of first compliant deposit: | 20 June 2019 | |||||||||||||||||||||
Date of first compliant Open Access: | 26 June 2019 | |||||||||||||||||||||
RIOXX Funder/Project Grant: |
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