Oxygen evolution reaction electrocatalysis on SrIrO3grown using molecular beam epitaxy

Tang, Runbang;Nie, Yuefeng;Kawasaki, Jason K.;Kuo, Ding-Yuan;Suntivich, Jin;et.al.
(2016) Journal of Materials Chemistry A — (2016)

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Authors
  • Tang, RunbangDepartment of Materials Science and Engineering, Cornell University, Ithaca, New York, USA
    Author
  • Nie, YuefengDepartment of Materials Science and Engineering, Cornell University, Ithaca, New York, USA
    Author
  • Kawasaki, Jason K.Laboratory of Atomic and Solid State Physics, Cornell University, Ithaca, New York, USA
    Author
  • Kuo, Ding-YuanDepartment of Materials Science and Engineering, Cornell University, Ithaca, New York, USA
    Author
  • Petretto, GuidoUCLouvain
    Author
  • Hautier, GeoffroyUCLouvain
    Author
  • Rignanese, Gian-Marcoorcid-logoUCLouvain
    Author
  • Suntivich, JinDepartment of Materials Science and Engineering, Cornell University, Ithaca, New York, USA
    Author
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Abstract
Electrochemical generation of oxygen via the oxygen evolution reaction (OER) is a key enabling step for many air-breathing electrochemical energy storage devices. IrO2 (Ir4+: 5d5) ranks among the most active known OER catalysts. However, it is unclear how the environment of the Ir4+ oxygen-coordination octahedra affects the OER electrocatalysis. Herein, we present the OER kinetics on a single-crystal, epitaxial SrIrO3(100)p perovskite oxide synthesized using molecular-beam epitaxy on a DyScO3(110) substrate. We find that by switching the host structure of the Ir4+ oxygen-coordination octahedra from corner- and edge-sharing rutile (IrO2) to purely corner-sharing perovskite (SrIrO3), the OER activity increases by more than an order of magnitude. We explain our finding with the correlated, semimetal electronic structure of SrIrO3; our density functional theory calculations reveal that the adsorption energetics on SrIrO3 depends sensitively on the electron-electron interaction, whereas for IrO2, it depends rather weakly. This finding suggests the importance of correlations on the OER and the design of future transition metal oxide electrocatalysts.
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Tang, R., Nie, Y., Kawasaki, J. K., Kuo, D.-Y., Petretto, G., Hautier, G., Rignanese, G.-M., Shen, K. M., Schlom, D. G., & Suntivich, J. (2016). Oxygen evolution reaction electrocatalysis on SrIrO3grown using molecular beam epitaxy. Journal of Materials Chemistry A. Published. https://doi.org/10.1039/C5TA09530A (Original work published 2016)