Encapsulation of cadmium selenide nanocrystals in biocompatible nanotubes: DFT calculations, X-ray diffraction investigations and confocal fluorescence imaging
| العنوان: | Encapsulation of cadmium selenide nanocrystals in biocompatible nanotubes: DFT calculations, X-ray diffraction investigations and confocal fluorescence imaging |
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| المؤلفون: | Calatayud, DG, Ge, H, Kuganathan, N, Mirabello, V, Jacobs, RMJ, Rees, NH, Stoppiello, CT, Khlobystov, AN, Tyrrell, RM, Como, ED, Pascu, SI |
| المساهمون: | European Research Council, Centre for Sustainable Chemical Technologies (UK), University of Bath |
| المصدر: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| بيانات النشر: | Wiley Open Access, 2018. |
| سنة النشر: | 2018 |
| مصطلحات موضوعية: | Density functional calculations, Functional and fluorescent biocompatible nanotube hybrids, Self-assembly, Beta-d-glucan encapsulation, Cadmium selenide functional nanohybrids |
| الوصف: | [EN] The encapsulation of CdSe nanocrystals within single‐walled carbon nanotube (SWNT) cavities of varying dimensions at elevated temperatures under strictly air‐tight conditions is described for the first time. The structures of CdSe nanocrystals under confinement inside SWNTs was established in a comprehensive study, combining both experimental and DFT theoretical investigations. The calculated binding energies show that all considered polymorphs [(3:3), (4:4), and (4:2)] may be obtained experimentally. The most thermodynamically stable structure (3:3) is directly compared to the experimentally observed CdSe structures inside carbon nanotubes. The gas‐phase DFT‐calculated energy difference between “free” 3:3 and 4:2 structures (whereby 3:3 models a novel tubular structure in which both Cd and Se form three coordination, as observed experimentally for HgTe inside SWNT, and 4:2 is a motif derived from the hexagonal CuI bulk structure in which both Cd and Se form 4 or 2 coordination) is surprisingly small, only 0.06 eV per formula unit. X‐ray powder diffraction, Raman spectroscopy, high‐resolution transmission electron microscopy, and energy‐dispersive X‐ray analyses led to the full characterization of the SWNTs filled with the CdSe nanocrystals, shedding light on the composition, structure, and electronic interactions of the new nanohybrid materials on an atomic level. A new emerging hybrid nanomaterial, simultaneously filled and beta‐d‐glucan coated, was obtained by using pristine nanotubes and bulk CdSe powder as starting materials. This displayed fluorescence in water dispersions and unexpected biocompatibility was found to be mediated by beta‐d‐glucan (a biopolymer extracted from barley) with respect to that of the individual inorganic material components. For the first time, such supramolecular nanostructures are investigated by life‐science techniques applied to functional nanomaterial characterization, opening the door for future nano‐biotechnological applications. This work was financially supported by the Science & Technologies Facilities Council, EPSRC Centre for Doctoral Training Centre for Sustainable Chemical Technologies at Bath, ERC Consolidator grant scheme (O2Sense to S.I.P.) and the University of Bath. The authors would also like to thank some former collaborators, Drs. Christoph Salzmann, Belen‐Ballesteros Perez, and Gerard Tobias for helpful discussions and their technical assistance with the initial stages of this research and training for the preliminary samples preparations. Chidambaram Kasimuthu and Gordon Lee are particularly acknowledged for help with some of the very preliminary initial tests and microscopy work during their short‐term stay in the S.I.P group at Oxford. Microscopy specialists of Oxford Nanotube Group, Prof John Hutchinson and Dr. Kerstin Jurkschat (Oxford Materials Department), are acknowledged for technical assistance with collection of some of the HRTEM data from initial batches, which proved batch‐to‐batch consistency. Dr. John Lowe is thanked for technical support with NMR. Prof. Malcolm Green FRS is thanked for invaluable discussions, training, support, and access to Oxford Nanotube Group facilities and expertise. The authors thank EPSRC National Service for Computational Chemistry Software and High‐Performance Computational facilities at Imperial College London for support and computational facilities. |
| وصف الملف: | |
| اللغة: | English |
| تدمد: | 2191-1363 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=dedup_wf_001::d448cf3eb54e55429d47f4c59075fe89 https://nottingham-repository.worktribe.com/file/908856/1/Calatayud_et_al-2018-ChemistryOpen.pdf |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.dedup.wf.001..d448cf3eb54e55429d47f4c59075fe89 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 21911363 |
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