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

Robin P. Forslund, William G. Hardin, Xi Rong, Artem M. Abakumov, Dmitry Filimonov, Caleb T. Alexander, J. Tyler Mefford, Hrishikesh Iyer, Alexie M. Kolpak, Keith P. Johnston and Keith J. Stevenson ()
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Robin P. Forslund: The University of Texas at Austin
William G. Hardin: The University of Texas at Austin
Xi Rong: Massachusetts Institute of Technology
Artem M. Abakumov: Skolkovo Institute of Science and Technology
Dmitry Filimonov: Moscow State University
Caleb T. Alexander: The University of Texas at Austin
J. Tyler Mefford: The University of Texas at Austin
Hrishikesh Iyer: The University of Texas at Austin
Alexie M. Kolpak: Massachusetts Institute of Technology
Keith P. Johnston: The University of Texas at Austin
Keith J. Stevenson: Skolkovo Institute of Science and Technology

Nature Communications, 2018, vol. 9, issue 1, 1-11

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-05600-y

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