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.; Wohlgemuth, Marcus A.; Giesen, Margret; Penn, Emily E.; Dittmann, Regina; Gunkel, Felix; Waser, Rainer; Bajdich, Michal; Nemšák, Slavomír; Mefford, J. Tyler; Chueh, William C.

doi:10.1038/s41563-020-00877-1

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

Journal Article · Mon Jan 11 00:00:00 EST 2021 · Nature Materials

DOI:https://doi.org/10.1038/s41563-020-00877-1· OSTI ID:1767439

^[1]; Li, Jiang ^[2]; Lu, Qiyang ^[3];

^[4]; Jin, Lei ^[5]; Martins, Henrique Perin ^[6];

^[5]; Glöß, Maria ^[7];

^[8]; Wohlgemuth, Marcus A. ^[5];

^[5]; Penn, Emily E. ^[9]; Dittmann, Regina ^[5];

^[5]; Waser, Rainer ^[10];

^[2];

^[11]; Mefford, J. Tyler ^[12];

^[12]

Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); RWTH Aachen Univ. (Germany); Univ. of Twente, Enschede (Netherlands)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Westlake Univ., Hangzhou (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
Forschungszentrum Juelich (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Forschungszentrum Juelich (Germany); Leibniz Inst. of Surface Engineering (IOM), Leipzig (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lund Univ. (Sweden)
Stanford Univ., CA (United States)
RWTH Aachen Univ. (Germany); Forschungszentrum Juelich (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Forschungszentrum Juelich (Germany)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

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. In this work, 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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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); European Research Council (ERC); German Research Foundation (DFG)

Grant/Contract Number:: 713683; 796142; AC02-76SF00515; AC02-05CH11231; SC0014697; SFB917; ECCS-1542152

OSTI ID:: 1767439

Journal Information:: Nature Materials, Vol. 2021; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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