Mechanism of photocatalytic water oxidation on small TiO2 nanoparticles

Chemical Science
Mikko MuuronenFilipp Furche

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.

References

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Oct 6, 2016·The Journal of Physical Chemistry Letters·Jordan C VincentFilipp Furche

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Citations

Jun 18, 2017·The Journal of Physical Chemistry Letters·Yulun HanDmitri S Kilin
Jun 9, 2017·The Journal of Physical Chemistry. a·Johannes EhrmaierWolfgang Domcke
Aug 3, 2017·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Neepa T Maitra
Feb 14, 2020·Nanomaterials·Shahin Homaeigohar
May 18, 2020·The Journal of Chemical Physics·Sree Ganesh BalasubramaniJason M Yu
Jul 18, 2018·Nature Communications·Yue LuMan-Ling Sui
Jul 26, 2019·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Constantin A WalentaUeli Heiz
Nov 11, 2020·The Journal of Chemical Physics·Shane M Parker, Colin J Schiltz
Jun 20, 2017·Journal of Chemical Theory and Computation·Enrico BerardoMartijn A Zwijnenburg
May 17, 2018·Chemical Reviews·Rachel Crespo-Otero, Mario Barbatti
Aug 5, 2017·Journal of the American Chemical Society·Annapaola Migani, Lluís Blancafort
Sep 1, 2021·The Journal of Physical Chemistry Letters·Lionel Lacombe, Neepa T Maitra

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Methods Mentioned

BETA
fluorescence microscopy

Software Mentioned

BOMD
NAMD
Turbomole

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