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Title: Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1–xFexO4±δ Ruddlesden-Popper oxides

Abstract

The electrolysis of water is of global importance to store renewable energy and the methodical design of next-generation oxygen evolution catalysts requires a greater understanding of the structural and electronic contributions that give rise to increased activities. Herein, we report a series of Ruddlesden–Popper La0.5Sr1.5Ni1–xFexO4±δ oxides that promote charge transfer via cross-gap hybridization to enhance electrocatalytic water splitting. Using selective substitution of lanthanum with strontium and nickel with iron to tune the extent to which transition metal and oxygen valence bands hybridize, we demonstrate remarkable catalytic activity of 10 mA cm–2 at a 360 mV overpotential and mass activity of 1930 mA mg–1ox at 1.63 V via a mechanism that utilizes lattice oxygen. This work demonstrates that Ruddlesden–Popper materials can be utilized as active catalysts for oxygen evolution through rational design of structural and electronic configurations that are unattainable in many other crystalline metal oxide phases.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [5];  [1];  [2];  [1]; ORCiD logo [3]
  1. The Univ. of Texas at Austin, Austin, TX (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Skolkovo Inst. of Science and Technology, Moscow (Russia)
  4. Moscow State Univ., Moscow (Russia)
  5. The Univ. of Texas at Austin, Austin, TX (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE
OSTI Identifier:
1543747
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Science & Technology; Other Topics

Citation Formats

Forslund, Robin P., Hardin, William G., Rong, Xi, Abakumov, Artem M., Filimonov, Dmitry, Alexander, Caleb T., Mefford, J. Tyler, Iyer, Hrishikesh, Kolpak, Alexie M., Johnston, Keith P., and Stevenson, Keith J. Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1–xFexO4±δ Ruddlesden-Popper oxides. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05600-y.
Forslund, Robin P., Hardin, William G., Rong, Xi, Abakumov, Artem M., Filimonov, Dmitry, Alexander, Caleb T., Mefford, J. Tyler, Iyer, Hrishikesh, Kolpak, Alexie M., Johnston, Keith P., & Stevenson, Keith J. Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1–xFexO4±δ Ruddlesden-Popper oxides. United States. https://doi.org/10.1038/s41467-018-05600-y
Forslund, Robin P., Hardin, William G., Rong, Xi, Abakumov, Artem M., Filimonov, Dmitry, Alexander, Caleb T., Mefford, J. Tyler, Iyer, Hrishikesh, Kolpak, Alexie M., Johnston, Keith P., and Stevenson, Keith J. Wed . "Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1–xFexO4±δ Ruddlesden-Popper oxides". United States. https://doi.org/10.1038/s41467-018-05600-y. https://www.osti.gov/servlets/purl/1543747.
@article{osti_1543747,
title = {Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1–xFexO4±δ Ruddlesden-Popper oxides},
author = {Forslund, Robin P. and Hardin, William G. and Rong, Xi and Abakumov, Artem M. and Filimonov, Dmitry and Alexander, Caleb T. and Mefford, J. Tyler and Iyer, Hrishikesh and Kolpak, Alexie M. and Johnston, Keith P. and Stevenson, Keith J.},
abstractNote = {The electrolysis of water is of global importance to store renewable energy and the methodical design of next-generation oxygen evolution catalysts requires a greater understanding of the structural and electronic contributions that give rise to increased activities. Herein, we report a series of Ruddlesden–Popper La0.5Sr1.5Ni1–xFexO4±δ oxides that promote charge transfer via cross-gap hybridization to enhance electrocatalytic water splitting. Using selective substitution of lanthanum with strontium and nickel with iron to tune the extent to which transition metal and oxygen valence bands hybridize, we demonstrate remarkable catalytic activity of 10 mA cm–2 at a 360 mV overpotential and mass activity of 1930 mA mg–1ox at 1.63 V via a mechanism that utilizes lattice oxygen. This work demonstrates that Ruddlesden–Popper materials can be utilized as active catalysts for oxygen evolution through rational design of structural and electronic configurations that are unattainable in many other crystalline metal oxide phases.},
doi = {10.1038/s41467-018-05600-y},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Wed Aug 08 00:00:00 EDT 2018},
month = {Wed Aug 08 00:00:00 EDT 2018}
}

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