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

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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. / Pittkowski, R.; Divanis, S.; Klementová, M. et al.
In: ACS Catalysis, Vol. 11, No. 2, 15.01.2021, p. 985-997.

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Pittkowski R, Divanis S, Klementová M, Nebel R, Nikman S, Hoster H et al. Engendering Unprecedented Activation of Oxygen Evolution via Rational Pinning of Ni Oxidation State in Prototypical Perovskite: Close Juxtaposition of Synthetic Approach and Theoretical Conception. ACS Catalysis. 2021 Jan 15;11(2):985-997. Epub 2021 Jan 6. doi: 10.1021/acscatal.0c04733

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@article{0a4b96cd30734f6382b61385a47018fd,
title = "Engendering Unprecedented Activation of Oxygen Evolution via Rational Pinning of Ni Oxidation State in Prototypical Perovskite: Close Juxtaposition of Synthetic Approach and Theoretical Conception",
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. {\textcopyright} 2021 American Chemical Society. All rights reserved.",
keywords = "DFT, electrocatalysis, oxygen evolution, rational catalyst design, Catalyst activity, Chemical activation, Lanthanum compounds, Nanocrystalline materials, Nanocrystals, Nickel, Oxidation, Oxygen, Perovskite, Surface structure, Freeze-drying synthesis, Local coordination, Oxygen evolution, Perovskite structures, Rational optimization, Structural motifs, Synthetic approach, Synthetic procedures, Nickel compounds",
author = "R. Pittkowski and S. Divanis and M. Klementov{\'a} and R. Nebel and S. Nikman and H. Hoster and S. Mukerjee and J. Rossmeisl and P. Krtil",
note = "This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright {\textcopyright} 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",
year = "2021",
month = jan,
day = "15",
doi = "10.1021/acscatal.0c04733",
language = "English",
volume = "11",
pages = "985--997",
journal = "ACS Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "2",

}

RIS

TY - JOUR

T1 - Engendering Unprecedented Activation of Oxygen Evolution via Rational Pinning of Ni Oxidation State in Prototypical Perovskite

T2 - Close Juxtaposition of Synthetic Approach and Theoretical Conception

AU - Pittkowski, R.

AU - Divanis, S.

AU - Klementová, M.

AU - Nebel, R.

AU - Nikman, S.

AU - Hoster, H.

AU - Mukerjee, S.

AU - Rossmeisl, J.

AU - Krtil, P.

N1 - 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

PY - 2021/1/15

Y1 - 2021/1/15

N2 - 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.

AB - 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.

KW - DFT

KW - electrocatalysis

KW - oxygen evolution

KW - rational catalyst design

KW - Catalyst activity

KW - Chemical activation

KW - Lanthanum compounds

KW - Nanocrystalline materials

KW - Nanocrystals

KW - Nickel

KW - Oxidation

KW - Oxygen

KW - Perovskite

KW - Surface structure

KW - Freeze-drying synthesis

KW - Local coordination

KW - Oxygen evolution

KW - Perovskite structures

KW - Rational optimization

KW - Structural motifs

KW - Synthetic approach

KW - Synthetic procedures

KW - Nickel compounds

U2 - 10.1021/acscatal.0c04733

DO - 10.1021/acscatal.0c04733

M3 - Journal article

VL - 11

SP - 985

EP - 997

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 2

ER -