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Tuning electrochemically driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis

Baeumer, Christoph ; Li, Jiang ; Lu, Qiyang ; Liang, Allen Yu Lun ; Jin, Lei ; Martins, Henrique Perin ; Duchoň, Tomáš ; Glöß, Maria ; Gericke, Sabrina M. LU and Wohlgemuth, Marcus A. , et al. (2021) In Nature Materials 20(5). p.674-682
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... (More)

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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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Materials
volume
20
issue
5
pages
9 pages
publisher
Nature Publishing Group
external identifiers
  • pmid:33432142
  • scopus:85100211005
ISSN
1476-1122
DOI
10.1038/s41563-020-00877-1
language
English
LU publication?
yes
id
7be8cd32-7df9-4b06-8f27-0f51fc4d0689
date added to LUP
2021-12-28 13:55:41
date last changed
2024-04-20 19:35:44
@article{7be8cd32-7df9-4b06-8f27-0f51fc4d0689,
  abstract     = {{<p>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 LaNiO<sub>3</sub> 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 NiO<sub>2</sub> 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.</p>}},
  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, Rainer and Bajdich, Michal and Nemšák, Slavomír and Mefford, J. Tyler and Chueh, William C.}},
  issn         = {{1476-1122}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{674--682}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Materials}},
  title        = {{Tuning electrochemically driven surface transformation in atomically flat LaNiO<sub>3</sub> thin films for enhanced water electrolysis}},
  url          = {{http://dx.doi.org/10.1038/s41563-020-00877-1}},
  doi          = {{10.1038/s41563-020-00877-1}},
  volume       = {{20}},
  year         = {{2021}},
}