Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides

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 Ru...

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Main Authors: 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.
Other Authors: Massachusetts Institute of Technology. Department of Mechanical Engineering
Format: Article
Published: Nature Publishing Group 2018
Online Access:http://hdl.handle.net/1721.1/119813
https://orcid.org/0000-0002-9286-1216
https://orcid.org/0000-0002-4347-0139
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author 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.
author2 Massachusetts Institute of Technology. Department of Mechanical Engineering
author_facet Massachusetts Institute of Technology. Department of Mechanical Engineering
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.
author_sort Forslund, Robin P.
collection MIT
description 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 La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±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⁻¹[subscript ox] 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.
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spelling mit-1721.1/1198132022-09-26T09:30:14Z Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides 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. Massachusetts Institute of Technology. Department of Mechanical Engineering Rong, Xi Kolpak, Alexie M. 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 La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±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⁻¹[subscript ox] 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. Robert A. Welch Foundation (Grant F-1529) Robert A. Welch Foundation (Grant F-1319) 2018-12-21T14:13:25Z 2018-12-21T14:13:25Z 2018-08 2017-09 2018-12-12T13:57:00Z Article http://purl.org/eprint/type/JournalArticle 2041-1723 http://hdl.handle.net/1721.1/119813 Forslund, Robin P. et al. “Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides.” Nature Communications 9, 1 (August 2018): 3150 © 2018 The Author(s) https://orcid.org/0000-0002-9286-1216 https://orcid.org/0000-0002-4347-0139 http://dx.doi.org/10.1038/s41467-018-05600-y Nature Communications Creative Commons Attribution 4.0 International License http://creativecommons.org/licenses/by/4.0/ application/pdf Nature Publishing Group Nature
spellingShingle 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 La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title_full Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title_fullStr Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title_full_unstemmed Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title_short Exceptional Electrocatalytic Oxygen Evolution via Tunable Charge Transfer Interactions in La[subscript 0.5]Sr[subscript 1.5]Ni[subscript 1−x]FexO[subscript 4±δ] Ruddlesden-Popper Oxides
title_sort exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in la subscript 0 5 sr subscript 1 5 ni subscript 1 x fexo subscript 4 δ ruddlesden popper oxides
url http://hdl.handle.net/1721.1/119813
https://orcid.org/0000-0002-9286-1216
https://orcid.org/0000-0002-4347-0139
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