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@ARTICLE{Heymann:906785,
author = {Heymann, Lisa and Weber, Moritz L. and Wohlgemuth, Marcus
and Risch, Marcel and Dittmann, Regina and Baeumer,
Christoph and Gunkel, Felix},
title = {{S}eparating the {E}ffects of {B}and {B}ending and
{C}ovalency in {H}ybrid {P}erovskite {O}xide
{E}lectrocatalyst {B}ilayers for {W}ater {E}lectrolysis},
journal = {ACS applied materials $\&$ interfaces},
volume = {14},
number = {12},
issn = {1944-8244},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2022-01692},
pages = {14129–14136},
year = {2022},
abstract = {The Co–O covalency in perovskite oxide cobaltites such as
La1–xSrxCoO3 is believed to impact the electrocatalytic
activity during electrochemical water splitting at the anode
where the oxygen evolution reaction (OER) takes place.
Additionally, space charge layers through band bending at
the interface to the electrolyte may affect the electron
transfer into the electrode, complicating the analysis and
identification of true OER activity descriptors. Here, we
separate the influence of covalency and band bending in
hybrid epitaxial bilayer structures of highly OER-active
La0.6Sr0.4CoO3 and undoped and less-active LaCoO3. Ultrathin
LaCoO3 capping layers of 2–8 unit cells on La0.6Sr0.4CoO3
show intermediate OER activity between La0.6Sr0.4CoO3 and
LaCoO3 evidently caused by the increased surface Co–O
covalency compared to single LaCoO3 as detected by X-ray
photoelectron spectroscopy. A Mott–Schottkyanalysis
revealed low flat band potentials for different LaCoO3
capping layer thicknesses, indicating that no limiting
extended space charge layer exists under OER conditions as
all catalyst bilayer films exhibited hole accumulation at
the surface. The combined X-ray photoelectron spectroscopy
and Mott–Schottky analysis thus enables us to
differentiate between the influence of the covalency and
intrinsic space charge layers, which are indistinguishable
in a single physical or electrochemical characterization.
Our results emphasize the prominent role of transition metal
oxygen covalency in perovskite electrocatalysts and
introduce a bilayer approach to fine-tune the surface
electronic structure.},
cin = {PGI-7 / PGI-10 / JARA-FIT},
ddc = {600},
cid = {I:(DE-Juel1)PGI-7-20110106 / I:(DE-Juel1)PGI-10-20170113 /
$I:(DE-82)080009_20140620$},
pnm = {5233 - Memristive Materials and Devices (POF4-523) / DFG
project 167917811 - SFB 917: Resistiv schaltende
Chalkogenide für zukünftige Elektronikanwendungen:
Struktur, Kinetik und Bauelementskalierung "Nanoswitches"
(167917811)},
pid = {G:(DE-HGF)POF4-5233 / G:(GEPRIS)167917811},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000787374700013},
doi = {10.1021/acsami.1c20337},
url = {https://juser.fz-juelich.de/record/906785},
}