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}
}
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 -