Muuronen, M;
Parker, SM;
Berardo, E;
Le, A;
Zwijnenburg, MA;
Furche, F;
(2017)
Mechanism of photocatalytic water oxidation on small TiO2 nanoparticles.
Chemical Science
, 8
(3)
pp. 2179-2183.
10.1039/c6sc04378j.
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Abstract
We present the first unconstrained nonadiabatic molecular dynamics (NAMD) simulations of photocatalytic water oxidation by small hydrated TiO2 nanoparticles using Tully surface hopping and time-dependent density functional theory. The results indicate that ultrafast electron–proton transfer from physisorbed water to the photohole initiates the photo-oxidation on the S1 potential energy surface. The new mechanism readily explains the observation of mobile hydroxyl radicals in recent experiments. Two key driving forces for the photo-oxidation reaction are identified: localization of the electron–hole pair and stabilization of the photohole by hydrogen bonding interaction. Our findings illustrate the scope of recent advances in NAMD methods and emphasize the importance of explicit simulation of electronic excitations.
| Type: | Article |
|---|---|
| Title: | Mechanism of photocatalytic water oxidation on small TiO2 nanoparticles |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1039/c6sc04378j |
| Publisher version: | http://dx.doi.org/10.1039/c6sc04378j |
| Language: | English |
| Additional information: | Open Access Article. Published on 07 December 2016. Downloaded on 10/07/2017 11:37:40. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence |
| Keywords: | Science & Technology, Physical Sciences, Chemistry, Multidisciplinary, Chemistry, AQUEOUS SURROUNDINGS, MOLECULAR-DYNAMICS, OXYGEN EVOLUTION, RUTILE, ANATASE, PHOTOOXIDATION, SURFACE, TITANIA, ELECTRODES |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/1550540 |
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