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  • HH100_ACS_catalysis_LaNi4_Pittkowski_Hoster_Krtil

    Rights statement: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.0c04733

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    Embargo ends: 6/01/22

    Available under license: CC BY-NC: Creative Commons Attribution-NonCommercial 4.0 International License

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Engendering Unprecedented Activation of Oxygen Evolution via Rational Pinning of Ni Oxidation State in Prototypical Perovskite: Close Juxtaposition of Synthetic Approach and Theoretical Conception

Research output: Contribution to journalJournal articlepeer-review

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  • R. Pittkowski
  • S. Divanis
  • M. Klementová
  • R. Nebel
  • S. Nikman
  • H. Hoster
  • S. Mukerjee
  • J. Rossmeisl
  • P. Krtil
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<mark>Journal publication date</mark>15/01/2021
<mark>Journal</mark>ACS Catalysis
Issue number2
Volume11
Number of pages13
Pages (from-to)985-997
Publication StatusPublished
Early online date6/01/21
<mark>Original language</mark>English

Abstract

Rational optimization of the OER activity of catalysts based on LaNiO3 oxide is achieved by maximizing the presence of trivalent Ni in the surface structure. DFT investigations of the LaNiO3 catalyst and surface structures related to it predict an improvement in the OER activity for these materials to levels comparable with the top of the OER volcano if the La content is minimized while the oxidation state of Ni is maintained. These theoretically predicted structures of high intrinsic OER activity can be prepared by a templated spray-freeze freeze-drying synthesis followed by a simple postsynthesis exfoliation-like treatment in acidic media. These nanocrystalline LaNiO3-related materials confirm the theoretical predictions, showing a dramatic improvement in OER activity. The exfoliated surfaces remain stable in OER catalysis, as shown by an in-operando ICP-OES study. The unprecedented OER activation of the synthesized LaNiO3-based materials is related to a close juxtaposition of the theoretical conception of ideal structural motifs and the ability to engender such motifs using a unique synthetic procedure, both principally related to stabilization and pinning of the Ni oxidation state within the local coordination environment of the perovskite structure. © 2021 American Chemical Society. All rights reserved.

Bibliographic note

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.0c04733