Imperial College London
Portrait Picture

Professor James Durrant, CBE, FRS

Faculty of Natural Sciences, Department of Chemistry

Professor of Photochemistry
 
 
 
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Contact

 

+44 (0)20 7594 5321j.durrant Website

 
 
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Assistant

 

Miss Lisa Benbow +44 (0)20 7594 5883

 
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Location

 

G22CMolecular Sciences Research HubWhite City Campus

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Summary

 

Publications

Citation

BibTex format

@article{Mesa:2020:10.1038/s41557-019-0347-1,
author = {Mesa, Zamora C and Francas, Forcada L and Yang, KR and Garrido-Barros, P and Pastor, Hernandez E and Ma, Y and Kafizas, A and Rosser, TE and Mayer, MT and Reisner, E and Grätzel, M and Batista, VS and Durrant, J},
doi = {10.1038/s41557-019-0347-1},
journal = {Nature Chemistry},
pages = {82--89},
title = {Multihole water oxidation catalysis on hematite photoanodes revealed by operando spectroelectrochemistry and DFT},
url = {http://dx.doi.org/10.1038/s41557-019-0347-1},
volume = {12},
year = {2020}
}
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RIS format (EndNote, RefMan)

TY  - JOUR
AB  - Water oxidation is  the key kinetic  bottle neck  of photoelectrochemical  devices for fuel  synthesis. Despite advances  in the identification of  intermediates, elucidating the  catalytic  mechanism of this multi-redox reactionon metal-oxidephotoanodes 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 upon hematite.We  observe  that hematite  is  able  toaccess  a reaction  mechanism  third  order  in surface  hole  density,  assigned  to  equilibration between  three surface holes and M(OH)-O-M(OH) sites. This reaction exhibits a remarkably low activation energy (Ea~ 60 meV). Density functional theory is employedto determine the energetics of charge accumulation and O-O bond formation on a modelhematite 110 surface. The proposed mechanism shows parallels with  the  function  of  oxygen  evolving  complex  of  photosystem  II,and  provides  new  insights  to  the mechanism of heterogeneous water oxidation on a metal oxide surface.
AU  - Mesa,Zamora C
AU  - Francas,Forcada L
AU  - Yang,KR
AU  - Garrido-Barros,P
AU  - Pastor,Hernandez E
AU  - Ma,Y
AU  - Kafizas,A
AU  - Rosser,TE
AU  - Mayer,MT
AU  - Reisner,E
AU  - Grätzel,M
AU  - Batista,VS
AU  - Durrant,J
DO  - 10.1038/s41557-019-0347-1
EP  - 89
PY  - 2020///
SN  - 1755-4330
SP  - 82
TI  - Multihole water oxidation catalysis on hematite photoanodes revealed by operando spectroelectrochemistry and DFT
T2  - Nature Chemistry
UR  - http://dx.doi.org/10.1038/s41557-019-0347-1
UR  - https://www.nature.com/articles/s41557-019-0347-1
UR  - http://hdl.handle.net/10044/1/73601
VL  - 12
ER  -
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