Journal Article

FZJ-2021-01373

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Tuning electrochemically driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis

Baeumer, C. (Corresponding author)FZJ* ; Li, J. ; Lu, Q. ; Liang, A. Y. ; Jin, L. ; Martins, H. P. ; Duchoň, T.FZJ* ; Glöß, M.FZJ* ; Gericke, S. M. ; Wohlgemuth, M. A.FZJ* ; Giesen, M.FZJ* ; Penn, E. E. ; Dittmann, R.FZJ* ; Gunkel, F.FZJ* ; Waser, R.FZJ* ; Bajdich, M. ; Nemšák, S.FZJ* ; Mefford, J. T. ; Chueh, W. C.

2021
Nature Publishing Group Basingstoke

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Please use a persistent id in citations: http://hdl.handle.net/2128/27751  doi:10.1038/s41563-020-00877-1

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.

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Contributing Institute(s):

1. Elektronische Materialien (PGI-7)
2. JARA Institut Green IT (PGI-10)
3. JARA-FIT (JARA-FIT)
4. Elektronische Eigenschaften (PGI-6)
5. Physik Nanoskaliger Systeme (ER-C-1)

Research Program(s):

1. 523 - Neuromorphic Computing and Network Dynamics (POF4-523) (POF4-523)

Appears in the scientific report 2021

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Database coverage:
; ; BIOSIS Previews ; Biological Abstracts ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 30 ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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