Understanding solvothermal crystallization of mesoporous anatase beads by in situ synchrotron PXRD and SAXS

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dc.contributor.authorXia, Fen_AU
dc.contributor.authorChen, DHen_AU
dc.contributor.authorScarlett, NVYen_AU
dc.contributor.authorMadsen, ICen_AU
dc.contributor.authorLau, Den_AU
dc.contributor.authorLeoni, Men_AU
dc.contributor.authorIlavsky, Jen_AU
dc.contributor.authorBrand, HEAen_AU
dc.contributor.authorCaruso, RAen_AU
dc.date.accessioned2021-12-08T19:48:25Zen_AU
dc.date.available2021-12-08T19:48:25Zen_AU
dc.date.issued2014-07-07en_AU
dc.date.statistics2021-11-12en_AU
dc.description.abstractSubmicrometer-sized mesoporous anatase (TiO2) beads have shown high efficiency as electrodes for dye-sensitized solar cells and are recoverable photocatalysts for the degradation of organic pollutants. The detailed mechanism for crystallization of the amorphous TiO2/hexadecylamine (HDA) hybrid beads occurring during the solvothermal process needs to be understood so that reaction parameters can be rationally refined for optimizing the synthesis. In this work, the solvothermal crystallization was monitored by in situ synchrotron powder X-ray diffraction (PXRD) and synchrotron small-angle X-ray scattering (SAXS) techniques. In situ PXRD provided crystallization curves, as well as the time evolution of anatase crystallite mean size and size distribution, and in situ SAXS provided complementary information regarding the evolution of the internal bead structure and the formation of pores during the course of the solvothermal process. By exploring the effects of temperature (140-180 °C), bead diameter (300 and 1150 nm), bead internal structure, and solvent composition (ethanol and ammonia concentrations) on this process, the crystallization was observed to progress 3-dimensionally throughout the entire bead due to solvent entrance after an initial fast partial dissolution of HDA from the nonporous precursor bead. On the basis of the kinetic and size evolution results, a 4-step crystallization process was proposed: (1) an induction period for precursor partial dissolution and anatase nucleation; (2) continued precursor dissolution accompanied by anatase nucleation and crystal growth; (3) continued precursor dissolution accompanied by only anatase crystal growth; and (4) complete crystallization with no significant Ostwald ripening. © 2014 American Chemical Society.en_AU
dc.description.sponsorshipThe CSIRO Office of the Chief Executive (OCE) Postdoctoral and Science Leader Schemes are acknowledged for financial support. This research was undertaken on the powder diffraction and small- and wide-angle X-ray scattering beamlines at the Australian Synchrotron, Victoria, Australia (beam time awards AS113/PD/4160 and AS131/SAXSFI/5984), through the Science and Industry Endowment Fund Special Research Program–Synchrotron Science. The authors wish to thank Dr. Wei Li, Dr. Nathan Webster, Dr. Xingdong Wang, Mr. Jingchao Song, Mr. Zaiquan Xu, Dr. Justin Kimpton, Dr. Stephen Mudie, and Dr. Nigel Kirby for assistance with synchrotron data collection. R.A.C. acknowledges the Australian Research Council for a Future Fellowship (FT0990583). Dr. Simon Crawford is thanked for ultramicrotoming samples in preparation for TEM characterization. The Melbourne Advanced Microscopy Facility at The University of Melbourne is acknowledged for electron microscopy access.en_AU
dc.identifier.citationXia, F., Chen, D., Scarlett, N. V., Madsen, I. C., Lau, D., Leoni, M., Ilavsky, J., Brand, H. E. A. & Caruso, R. A. (2014). Understanding solvothermal crystallization of mesoporous anatase beads by in situ synchrotron PXRD and SAXS. Chemistry of Materials, 26(15), 4563-4571. doi:10.1021/cm501810xen_AU
dc.identifier.issn0897-4756en_AU
dc.identifier.issue15en_AU
dc.identifier.journaltitleChemistry of Materialsen_AU
dc.identifier.pagination4563-4571en_AU
dc.identifier.urihttps://doi.org/10.1021/cm501810xen_AU
dc.identifier.urihttps://apo.ansto.gov.au/dspace/handle/10238/12390en_AU
dc.identifier.volume26en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectX-ray diffractionen_AU
dc.subjectSynchrotronsen_AU
dc.subjectCrystallizationen_AU
dc.subjectOxidesen_AU
dc.subjectMineralsen_AU
dc.subjectDelayed neutron precursorsen_AU
dc.titleUnderstanding solvothermal crystallization of mesoporous anatase beads by in situ synchrotron PXRD and SAXSen_AU
dc.typeJournal Articleen_AU
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