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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Nature Publishing Group
2018
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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. |
first_indexed | 2024-09-23T08:57:51Z |
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id | mit-1721.1/119813 |
institution | Massachusetts Institute of Technology |
last_indexed | 2024-09-23T08:57:51Z |
publishDate | 2018 |
publisher | Nature Publishing Group |
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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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