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

Baeumer, Christoph (author)
Stanford Linear Accelerator Center (SLAC),Stanford University,RWTH Aachen University
Li, Jiang (author)
Stanford Linear Accelerator Center (SLAC)
Lu, Qiyang (author)
Advanced Light Source, Berkeley,Stanford Linear Accelerator Center (SLAC),Westlake University,Stanford University
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Liang, Allen Yu Lun (author)
Stanford University,Stanford Linear Accelerator Center (SLAC)
Jin, Lei (author)
Jülich Research Centre
Martins, Henrique Perin (author)
Advanced Light Source, Berkeley
Duchoň, Tomáš (author)
Jülich Research Centre
Glöß, Maria (author)
Leibniz Institute for Surface Modification,Jülich Research Centre
Gericke, Sabrina M. (author)
Lund University,Lunds universitet,Förbränningsfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Combustion Physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,Lawrence Berkeley National Laboratory
Wohlgemuth, Marcus A. (author)
Jülich Research Centre
Giesen, Margret (author)
Jülich Research Centre
Penn, Emily E. (author)
Stanford University
Dittmann, Regina (author)
Jülich Research Centre
Gunkel, Felix (author)
Jülich Research Centre
Waser, Rainer (author)
RWTH Aachen University,Jülich Research Centre
Bajdich, Michal (author)
Stanford Linear Accelerator Center (SLAC)
Nemšák, Slavomír (author)
Advanced Light Source, Berkeley,Jülich Research Centre
Mefford, J. Tyler (author)
Stanford University,Stanford Linear Accelerator Center (SLAC)
Chueh, William C. (author)
Stanford University,Stanford Linear Accelerator Center (SLAC)
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 (creator_code:org_t)
2021-01-11
2021
English 9 s.
In: Nature Materials. - : Springer Science and Business Media LLC. - 1476-1122 .- 1476-4660. ; 20:5, s. 674-682
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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.

Subject headings

NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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