%0 Journal Article
%A Baeumer, Christoph
%A Li, Jiang
%A Lu, Qiyang
%A Liang, Allen Yu-Lun
%A Jin, Lei
%A Martins, Henrique Perin
%A Duchoň, Tomáš
%A Glöß, Maria
%A Gericke, Sabrina M.
%A Wohlgemuth, Marcus A.
%A Giesen, Margret
%A Penn, Emily E.
%A Dittmann, Regina
%A Gunkel, Felix
%A Waser, R.
%A Bajdich, Michal
%A Nemšák, Slavomír
%A Mefford, J. Tyler
%A Chueh, William C.
%T Tuning electrochemically driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis
%J Nature materials
%V 20
%@ 1476-4660
%C Basingstoke
%I Nature Publishing Group
%M FZJ-2021-01373
%P 674–682
%D 2021
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%$ 33432142
%U <Go to ISI:>//WOS:000607023400007
%R 10.1038/s41563-020-00877-1
%U https://juser.fz-juelich.de/record/891112