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  4. Multihole water oxidation catalysis on haematite photoanodes revealed by operando spectroelectrochemistry and DFT
 
research article

Multihole water oxidation catalysis on haematite photoanodes revealed by operando spectroelectrochemistry and DFT

Mesa, Camilo A.
•
Francas, Laia
•
Yang, Ke R.
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January 1, 2020
Nature Chemistry

Water oxidation is the key kinetic bottleneck of photoelectrochemical devices for fuel synthesis. Despite advances in the identification of intermediates, elucidating the catalytic mechanism of this multi-redox reaction on metal-oxide photoanodes remains a significant experimental and theoretical challenge. Here, we report an experimental analysis of water oxidation kinetics on four widely studied metal oxides, focusing particularly on haematite. We observe that haematite is able to access a reaction mechanism that is third order in surface-hole density, which is assigned to equilibration between three surface holes and M(OH)-O-M(OH) sites. This reaction exhibits low activation energy (E-a approximate to 60meV). Density functional theory is used to determine the energetics of charge accumulation and O-O bond formation on a model haematite (110) surface. The proposed mechanism shows parallels with the function of the oxygen evolving complex of photosystem II, and provides new insights into the mechanism of heterogeneous water oxidation on a metal oxide surface. The oxidation of water remains the kinetic bottleneck of solar-to-fuel synthesis. Now, spectroelectrochemical evidence together with density functional theory calculations show that charge accumulation determines the reaction mechanism on metal-oxide photoanodes. These insights reveal features that are common to the mechanisms of water oxidation carried out by other inorganic and biological systems.

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Type
research article
DOI
10.1038/s41557-019-0347-1
Web of Science ID

WOS:000504734200015

Author(s)
Mesa, Camilo A.
Francas, Laia
Yang, Ke R.
Garrido-Barros, Pablo
Pasto, Ernest
Ma, Yimeng
Kafizas, Andreas
Rosser, Timothy E.
Mayer, Matthew T.
Reisner, Erwin
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Date Issued

2020-01-01

Publisher

NATURE PUBLISHING GROUP

Published in
Nature Chemistry
Volume

12

Issue

1

Start page

82

End page

89

Subjects

Chemistry, Multidisciplinary

•

Chemistry

•

o-o bond

•

quantum mechanics/molecular mechanics

•

oxygen-evolving complex

•

rate law analysis

•

photosystem-ii

•

nanostructured alpha-fe2o3

•

surface

•

kinetics

•

photooxidation

•

recombination

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LPI  
Available on Infoscience
March 3, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/166873
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