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Title: Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co 3O 4/La 0.3Sr 0.7CoO 3

Abstract

Surface lattice oxygen in transition-metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co 3O 4 /perovskite La 0.3Sr 0.7CoO 3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co 3O 4, leading to more inactive O 2- transformed into active O 2-x. Furthermore, the activated Co 3O 4/LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1];  [1]; ORCiD logo [1]
  1. Jilin Univ., Changchun (China)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1546793
Grant/Contract Number:  
AC02-76SF00515; 21427802; 21671076; 21621001; 21831003; 3102018bzc007; 10183201816
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Volume: 58; Journal Issue: 34; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; electron transfer; electronic structure; perovskite; spinels; surface lattice oxygen

Citation Formats

Wang, Xiyang, Pan, Ziye, Chu, Xuefeng, Huang, Keke, Cong, Yingge, Cao, Rui, Sarangi, Ritimukta, Li, Liping, Li, Guangshe, and Feng, Shouhua. Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co3O4/La0.3Sr0.7CoO3. United States: N. p., 2019. Web. doi:10.1002/anie.201905543.
Wang, Xiyang, Pan, Ziye, Chu, Xuefeng, Huang, Keke, Cong, Yingge, Cao, Rui, Sarangi, Ritimukta, Li, Liping, Li, Guangshe, & Feng, Shouhua. Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co3O4/La0.3Sr0.7CoO3. United States. https://doi.org/10.1002/anie.201905543
Wang, Xiyang, Pan, Ziye, Chu, Xuefeng, Huang, Keke, Cong, Yingge, Cao, Rui, Sarangi, Ritimukta, Li, Liping, Li, Guangshe, and Feng, Shouhua. Sat . "Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co3O4/La0.3Sr0.7CoO3". United States. https://doi.org/10.1002/anie.201905543. https://www.osti.gov/servlets/purl/1546793.
@article{osti_1546793,
title = {Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co3O4/La0.3Sr0.7CoO3},
author = {Wang, Xiyang and Pan, Ziye and Chu, Xuefeng and Huang, Keke and Cong, Yingge and Cao, Rui and Sarangi, Ritimukta and Li, Liping and Li, Guangshe and Feng, Shouhua},
abstractNote = {Surface lattice oxygen in transition-metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co3O4 /perovskite La0.3Sr0.7CoO3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co3O4, leading to more inactive O2- transformed into active O2-x. Furthermore, the activated Co3O4/LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.},
doi = {10.1002/anie.201905543},
url = {https://www.osti.gov/biblio/1546793}, journal = {Angewandte Chemie (International Edition)},
issn = {1433-7851},
number = 34,
volume = 58,
place = {United States},
year = {2019},
month = {6}
}

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Cited by: 5 works
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Works referenced in this record:

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journal, August 2000


Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
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Titanium dx y ferromagnetism at the LaAlO3/SrTiO3 interface
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Remarkable Oxygen-Evolution Activity of a Perovskite Oxide from the Ca 2− x Sr x Fe 2 O 6− δ Series
journal, January 2019


Activation of surface oxygen sites on an iridium-based model catalyst for the oxygen evolution reaction
journal, December 2016


Anionic redox processes for electrochemical devices
journal, January 2016


Redox activity of surface oxygen anions in oxygen-deficient perovskite oxides during electrochemical reactions
journal, January 2015


Real-time impedance monitoring of oxygen reduction during surface modification of thin film cathodes
journal, March 2017


Improved chemical and electrochemical stability of perovskite oxides with less reducible cations at the surface
journal, June 2016


Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures
journal, August 2008


Remarkable Oxygen-Evolution Activity of a Perovskite Oxide from the Ca 2− x Sr x Fe 2 O 6− δ Series
journal, January 2019


Co@Co 3 O 4 Encapsulated in Carbon Nanotube-Grafted Nitrogen-Doped Carbon Polyhedra as an Advanced Bifunctional Oxygen Electrode
journal, February 2016


Contrasting the Role of Ni/Al 2 O 3 Interfaces in Water–Gas Shift and Dry Reforming of Methane
journal, November 2017


Thermally stable single-atom platinum-on-ceria catalysts via atom trapping
journal, July 2016


Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution
journal, January 2017


O-K and Co-L XANES Study on Oxygen Intercalation in Perovskite SrCoO3-δ
journal, January 2010


Activating p-Blocking Centers in Perovskite for Efficient Water Splitting
journal, December 2018


A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3
journal, January 2013


    Works referencing / citing this record:

    Remarkable Oxygen-Evolution Activity of a Perovskite Oxide from the Ca 2− x Sr x Fe 2 O 6− δ Series
    journal, January 2019


    Co@Co 3 O 4 Encapsulated in Carbon Nanotube-Grafted Nitrogen-Doped Carbon Polyhedra as an Advanced Bifunctional Oxygen Electrode
    journal, February 2016


    Remarkable Oxygen-Evolution Activity of a Perovskite Oxide from the Ca 2− x Sr x Fe 2 O 6− δ Series
    journal, January 2019


    Activating p-Blocking Centers in Perovskite for Efficient Water Splitting
    journal, December 2018


    Interfaces in Heterogeneous Catalysts: Advancing Mechanistic Understanding through Atomic-Scale Measurements
    journal, February 2017


    Activation of Surface Oxygen Sites in a Cobalt-Based Perovskite Model Catalyst for CO Oxidation
    journal, July 2018


    O-K and Co-L XANES Study on Oxygen Intercalation in Perovskite SrCoO3-δ
    journal, January 2010


    Perovskite Oxides: Preparation, Characterizations, and Applications in Heterogeneous Catalysis
    journal, August 2014


    A Bifunctional Nonprecious Metal Catalyst for Oxygen Reduction and Water Oxidation
    journal, October 2010


    Contrasting the Role of Ni/Al 2 O 3 Interfaces in Water–Gas Shift and Dry Reforming of Methane
    journal, November 2017


    Catalytically Active Oxygen Species in La 1 - x Sr x CoO 3 - δ Studied by XPS and XAFS Spectroscopy
    journal, August 2000


    Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution
    journal, January 2017


    A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3
    journal, January 2013


    Redox activity of surface oxygen anions in oxygen-deficient perovskite oxides during electrochemical reactions
    journal, January 2015


    Activation of surface oxygen sites on an iridium-based model catalyst for the oxygen evolution reaction
    journal, December 2016


    Titanium dx y ferromagnetism at the LaAlO3/SrTiO3 interface
    journal, June 2013


    Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
    journal, July 2013


    Anionic redox processes for electrochemical devices
    journal, January 2016


    Improved chemical and electrochemical stability of perovskite oxides with less reducible cations at the surface
    journal, June 2016


    Real-time impedance monitoring of oxygen reduction during surface modification of thin film cathodes
    journal, March 2017


    Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures
    journal, August 2008


    Thermally stable single-atom platinum-on-ceria catalysts via atom trapping
    journal, July 2016


    Perovskites in catalysis and electrocatalysis
    journal, November 2017


    Enhanced catalytic activity of nanostructured, A-site deficient (La 0.7 Sr 0.3 ) 0.95 (Co 0.2 Fe 0.8 )O 3−δ for SOFC cathodes
    journal, January 2019