Please use this identifier to cite or link to this item:
http://hdl.handle.net/2445/114944
Title: | When anatase nanoparticles become bulk-like: properties of realistic TiO2 nanoparticles in the 1-6 nm size range from all electron relativistic density functional theory based calculations |
Author: | Lamiel Garcia, Josep Oriol Ko, Kyoung Chul Lee, Jin Yong Bromley, Stefan Thomas Illas i Riera, Francesc |
Keywords: | Diòxid de titani Nanopartícules Teoria del funcional de densitat Titanium dioxide Nanoparticles Density functionals |
Issue Date: | 1-Apr-2017 |
Publisher: | American Chemical Society |
Abstract: | All electron relativistic density functional theory (DFT) based calculations using numerical atom-centered orbitals have been carried out to explore the relative stability, atomic, and electronic structure of a series of stoichiometric TiO2 anatase nanoparticles explicitly containing up to 1365 atoms as a function of size and morphology. The nanoparticles under scrutiny exhibit octahedral or truncated octahedral structures and span the 1-6 nm diameter size range. Initial structures were obtained using the Wulff construction, thus exhibiting the most stable (101) and (001) anatase surfaces. Final structures were obtained from geometry optimization with full relaxation of all structural parameters using both generalized gradient approximation (GGA) and hybrid density functionals. Results show that, for nanoparticles of a similar size, octahedral and truncated octahedral morphologies have comparable energetic stabilities. The electronic structure properties exhibit a clear trend converging:to the bulk values as the size of the nanoparticles increases but with a marked influence of the density functional employed. Our results suggest that electronic structure properties, and hence reactivity, for the largest anatase nanoparticles considered in this study will be similar to those exhibited by even larger mesoscale particles or by bulk systems. Finally, we present compelling evidence that anatase nanoparticles become effectively bulklike when reaching a size of similar to 20 nm diameter. |
Note: | Versió postprint del document publicat a: https://doi.org/10.1021/acs.jctc.7b00085 |
It is part of: | Journal of Chemical Theory and Computation, 2017, vol. 13, num. 4, p. 1785-1793 |
URI: | http://hdl.handle.net/2445/114944 |
Related resource: | https://doi.org/10.1021/acs.jctc.7b00085 |
ISSN: | 1549-9618 |
Appears in Collections: | Articles publicats en revistes (Ciència dels Materials i Química Física) Publicacions de projectes de recerca finançats per la UE |
Files in This Item:
File | Description | Size | Format | |
---|---|---|---|---|
673122.pdf | 1.41 MB | Adobe PDF | View/Open |
Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.