Imperial College London
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DrAnnaRegoutz

Faculty of Engineering, Department of Materials

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Contact

 

a.regoutz Website

 
 
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Location

 

2.M14Royal School of MinesSouth Kensington Campus

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Summary

 

Publications

Citation

BibTex format

@article{Moss:2021:10.1038/s41563-020-00868-2,
author = {Moss, B and Wang, Q and Butler, K and Grau-Crespo, R and Selim, S and Regoutz, A and Hisatomi, T and Godin, R and Payne, D and Kafizas, A and Domen, K and Steier, L and Durrant, J},
doi = {10.1038/s41563-020-00868-2},
journal = {Nature Materials},
pages = {511--517},
title = {Linking in situ charge accumulation to electronic structure in doped SrTiO3 reveals design principles for hydrogen-evolving photocatalysts},
url = {http://dx.doi.org/10.1038/s41563-020-00868-2},
volume = {20},
year = {2021}
}
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RIS format (EndNote, RefMan)

TY  - JOUR
AB  - Recently, high solar-to-hydrogen efficiencies were demonstrated using La and Rh co-doped SrTiO3 (La,Rh:SrTiO3) incorporated into a low-cost and scalable Z-scheme device, known as a photocatalyst sheet. However, the unique properties that enable La,Rh:SrTiO3 to support this impressive performance are not fully understood. Combining in situ spectroelectrochemical measurements with density functional theory and photoelectron spectroscopy produces a depletion model of Rh:SrTiO3 and La,Rh:SrTiO3 photocatalyst sheets. This reveals remarkable properties, such as deep flatband potentials (+2 V versus the reversible hydrogen electrode) and a Rh oxidation state dependent reorganization of the electronic structure, involving the loss of a vacant Rh 4d mid-gap state. This reorganization enables Rh:SrTiO3 to be reduced by co-doping without compromising the p-type character. In situ time-resolved spectroscopies show that the electronic structure reorganization induced by Rh reduction controls the electron lifetime in photocatalyst sheets. In Rh:SrTiO3, enhanced lifetimes can only be obtained at negative applied potentials, where the complete Z-scheme operates inefficiently. La co-doping fixes Rh in the 3+ state, which results in long-lived photogenerated electrons even at very positive potentials (+1 V versus the reversible hydrogen electrode), in which both components of the complete device operate effectively. This understanding of the role of co-dopants provides a new insight into the design principles for water-splitting devices based on bandgap-engineered metal oxides.
AU  - Moss,B
AU  - Wang,Q
AU  - Butler,K
AU  - Grau-Crespo,R
AU  - Selim,S
AU  - Regoutz,A
AU  - Hisatomi,T
AU  - Godin,R
AU  - Payne,D
AU  - Kafizas,A
AU  - Domen,K
AU  - Steier,L
AU  - Durrant,J
DO  - 10.1038/s41563-020-00868-2
EP  - 517
PY  - 2021///
SN  - 1476-1122
SP  - 511
TI  - Linking in situ charge accumulation to electronic structure in doped SrTiO3 reveals design principles for hydrogen-evolving photocatalysts
T2  - Nature Materials
UR  - http://dx.doi.org/10.1038/s41563-020-00868-2
UR  - https://www.nature.com/articles/s41563-020-00868-2
UR  - http://hdl.handle.net/10044/1/83393
VL  - 20
ER  -
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