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@ARTICLE{Baeumer:891112,
author = {Baeumer, Christoph and Li, Jiang and Lu, Qiyang and Liang,
Allen Yu-Lun and Jin, Lei and Martins, Henrique Perin and
Duchoň, Tomáš and Glöß, Maria and Gericke, Sabrina M.
and Wohlgemuth, Marcus A. and Giesen, Margret and Penn,
Emily E. and Dittmann, Regina and Gunkel, Felix and Waser,
R. and Bajdich, Michal and Nemšák, Slavomír and Mefford,
J. Tyler and Chueh, William C.},
title = {{T}uning electrochemically driven surface transformation in
atomically flat {L}a{N}i{O}3 thin films for enhanced water
electrolysis},
journal = {Nature materials},
volume = {20},
issn = {1476-4660},
address = {Basingstoke},
publisher = {Nature Publishing Group},
reportid = {FZJ-2021-01373},
pages = {674–682},
year = {2021},
abstract = {Structure–activity relationships built on descriptors of
bulk and bulk-terminated surfaces are the basis for the
rational design of electrocatalysts. However,
electrochemically driven surface transformations complicate
the identification of such descriptors. Here we demonstrate
how the as-prepared surface composition of (001)-terminated
LaNiO3 epitaxial thin films dictates the surface
transformation and the electrocatalytic activity for the
oxygen evolution reaction. Specifically, the Ni termination
(in the as-prepared state) is considerably more active than
the La termination, with overpotential differences of up to
150 mV. A combined electrochemical, spectroscopic and
density-functional theory investigation suggests that this
activity trend originates from a thermodynamically stable,
disordered NiO2 surface layer that forms during the
operation of Ni-terminated surfaces, which is kinetically
inaccessible when starting with a La termination. Our work
thus demonstrates the tunability of surface transformation
pathways by modifying a single atomic layer at the surface
and that active surface phases only develop for select
as-synthesized surface terminations.},
cin = {PGI-7 / PGI-10 / JARA-FIT / PGI-6 / ER-C-1},
ddc = {610},
cid = {I:(DE-Juel1)PGI-7-20110106 / I:(DE-Juel1)PGI-10-20170113 /
$I:(DE-82)080009_20140620$ / I:(DE-Juel1)PGI-6-20110106 /
I:(DE-Juel1)ER-C-1-20170209},
pnm = {523 - Neuromorphic Computing and Network Dynamics
(POF4-523)},
pid = {G:(DE-HGF)POF4-523},
typ = {PUB:(DE-HGF)16},
pubmed = {33432142},
UT = {WOS:000607023400007},
doi = {10.1038/s41563-020-00877-1},
url = {https://juser.fz-juelich.de/record/891112},
}