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; Keith J Stevenson

doi:10.1038/s41467-018-05600-y

Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La_0.5Sr_1.5Ni_1-xFe_xO_4±δ Ruddlesden-Popper oxides

Nat Commun. 2018 Aug 8;9(1):3150. doi: 10.1038/s41467-018-05600-y.

Authors

Robin P Forslund¹, William G Hardin^{2

3}, Xi Rong⁴, Artem M Abakumov⁵, Dmitry Filimonov⁶, Caleb T Alexander⁷, J Tyler Mefford^{1

8}, Hrishikesh Iyer⁷, Alexie M Kolpak⁴, Keith P Johnston⁷, Keith J Stevenson⁹

Affiliations

¹ Department of Chemistry, The University of Texas at Austin, 1 University Station, Austin, TX, 78712, USA.
² Texas Materials Institute, The University of Texas at Austin, 1 University Station, Austin, TX, 78712, USA.
³ Exponent Failure Analysis Associates, 9 Strathmore Rd, Natick, MA, 01760, USA.
⁴ Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
⁵ Center for Electrochemical Energy Storage, Skolkovo Institute of Science and Technology, 3 Nobel Street, Moscow, 143026, Russia.
⁶ Department of Chemistry, Moscow State University, 1 Leninskiye Gory, Moscow, 119991, Russia.
⁷ McKetta Department of Chemical Engineering, The University of Texas at Austin, 1 University Station, Austin, TX, 78712, USA.
⁸ Department of Materials Science & Engineering, Stanford University, 496 Lomita Mall, Stanford, CA, 94305, USA.
⁹ Center for Electrochemical Energy Storage, Skolkovo Institute of Science and Technology, 3 Nobel Street, Moscow, 143026, Russia. K.Stevenson@skoltech.ru.

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 La_0.5Sr_1.5Ni_1-xFe_xO_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_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.

Publication types

Research Support, Non-U.S. Gov't