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@ARTICLE{Kampmann:877280,
author = {Kampmann, Jonathan and Betzler, Sophia and Hajiyani,
Hamidreza and Häringer, Sebastian and Beetz, Michael and
Harzer, Tristan and Kraus, Jürgen and Lotsch, Bettina V.
and Scheu, Christina and Pentcheva, Rossitza and Fattakhova,
Dina and Bein, Thomas},
title = {{H}ow photocorrosion can trick you: a detailed study on
low-bandgap {L}i doped {C}u{O} photocathodes for solar
hydrogen production},
journal = {Nanoscale},
volume = {12},
number = {14},
issn = {2040-3372},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {FZJ-2020-02103},
pages = {7766 - 7775},
year = {2020},
abstract = {The efficiency of photoelectrochemical tandem cells is
still limited by the availability of stable low band gap
electrodes. In this work, we report a photocathode based on
lithium doped copper(II) oxide, a black p-type
semiconductor. Density functional theory calculations with a
Hubbard U term show that low concentrations of Li
(Li0.03Cu0.97O) lead to an upward shift of the valence band
maximum that crosses the Fermi level and results in a p-type
semiconductor. Therefore, Li doping emerged as a suitable
approach to manipulate the electronic structure of copper
oxide based photocathodes. As this material class suffers
from instability in water under operating conditions, the
recorded photocurrents are repeatedly misinterpreted as
hydrogen evolution evidence. We investigated the
photocorrosion behavior of LixCu1−xO cathodes in detail
and give the first mechanistic study of the fundamental
physical process. The reduced copper oxide species were
localized by electron energy loss spectroscopy mapping. Cu2O
grows as distinct crystallites on the surface of LixCu1−xO
instead of forming a dense layer. Additionally, there is no
obvious Cu2O gradient inside the films, as Cu2O seems to
form on all LixCu1−xO nanocrystals exposed to water. The
application of a thin Ti0.8Nb0.2Ox coating by atomic layer
deposition and the deposition of a platinum co-catalyst
increased the stability of LixCu1−xO against
decomposition. These devices showed a stable hydrogen
evolution for 15 minutes.},
cin = {IEK-1},
ddc = {600},
cid = {I:(DE-Juel1)IEK-1-20101013},
pnm = {131 - Electrochemical Storage (POF3-131)},
pid = {G:(DE-HGF)POF3-131},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:32215409},
UT = {WOS:000529531500029},
doi = {10.1039/C9NR10250G},
url = {https://juser.fz-juelich.de/record/877280},
}