Deconvoluting XPS Spectra of La-Containing Perovskites from First-Principles

Whitten, Ariel; Guo, Dezhou; Tezel, Elif; Denecke, Reinhard; Nikolla, Eranda; McEwen, Jean-Sabin

doi:10.1021/jacsau.4c00440

Deconvoluting XPS Spectra of La-Containing Perovskites from First-Principles

Journal Article · Tue Jul 23 00:00:00 EDT 2024 · JACS Au

DOI:https://doi.org/10.1021/jacsau.4c00440· OSTI ID:2480703

Whitten, Ariel ^[1]; Guo, Dezhou ^[1]; Tezel, Elif ^[2]; ^[3]; ^[4]; ^[5]

Washington State Univ., Pullman, WA (United States)
Wayne State Univ., Detroit, MI (United States)
Univ. of Leipzig (Germany)
Univ. of Michigan, Ann Arbor, MI (United States); Wayne State Univ., Detroit, MI (United States)
Washington State Univ., Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Perovskite-based oxides are used in electrochemical CO₂ and H₂O reduction in electrochemical cells due to their compositional versatility, redox properties and stability. However limited knowledge exists on the mechanisms driving these processes. Toward this understanding, herein we probe the core level binding energy shifts of water-derived adspecies (H, O, OH, H₂O) as well as the adsorption of CO₂ on LaCoO₃ and LaNiO₃ and we correlate the simulated peaks with experimental Temperature Programmed X-ray Photoelectron Spectroscopy (TPXPS) results. We find the strong adsorption of such chemical species can affect the antiferromagnetic ordering of LaNiO₃. The adsorption of such adspecies is further quantified through Bader and differential charge analyses. We find the higher O 1s core level binding energy peak for both LaCoO₃ and LaNiO₃ corresponds to adsorption of water-related species and CO₂, while the lower energy peak is due to lattice oxygen. We further correlate these DFT-based core level O 1s binding energies with the TPXPS measurements to quantify the decrease of the O 1s contribution due to desorption of adsorbates and the apparent increase of the lattice oxygen (both bulk and surface) with temperature. Finally, we quantify the influence of adsorbates on the La 4d, Co 2p and the Ni 3p core level binding energy shifts. This work demonstrates how theoretically generated XPS data can be utilized to predict species-specific binding energy shifts to assist in the deconvolution of the experimental results.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2480703

Report Number(s):: PNNL-SA--199847

Journal Information:: JACS Au, Journal Name: JACS Au Journal Issue: 8 Vol. 4; ISSN 2691-3704

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Deconvoluting XPS Spectra of La-Containing Perovskites from First-Principles

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