Key role of chemistry versus bias in electrocatalytic oxygen evolution

Hong Nhan Nong, Lorenz J. Falling, Arno Bergmann, Malte Klingenhof, Hoang Phi Tran, Camillo Spöri, Rik Mom, Janis Timoshenko, Guido Zichittella, Axel Knop-Gericke, Simone Piccinin, Javier Pérez-Ramírez, Beatriz Roldan Cuenya, Robert Schlögl, Peter Strasser, Detre Teschner () and Travis E. Jones ()
Additional contact information
Hong Nhan Nong: Technische Universität Berlin
Lorenz J. Falling: Fritz-Haber-Institute of the Max-Planck-Society
Arno Bergmann: Fritz-Haber-Institute of the Max-Planck-Society
Malte Klingenhof: Technische Universität Berlin
Hoang Phi Tran: Technische Universität Berlin
Camillo Spöri: Technische Universität Berlin
Rik Mom: Fritz-Haber-Institute of the Max-Planck-Society
Janis Timoshenko: Fritz-Haber-Institute of the Max-Planck-Society
Guido Zichittella: ETH Zurich
Axel Knop-Gericke: Max-Planck-Institute for Chemical Energy Conversion
Simone Piccinin: Consiglio Nazionale delle Ricerche, CNR-IOM
Javier Pérez-Ramírez: ETH Zurich
Beatriz Roldan Cuenya: Fritz-Haber-Institute of the Max-Planck-Society
Robert Schlögl: Max-Planck-Institute for Chemical Energy Conversion
Peter Strasser: Technische Universität Berlin
Detre Teschner: Max-Planck-Institute for Chemical Energy Conversion
Travis E. Jones: Fritz-Haber-Institute of the Max-Planck-Society

Nature, 2020, vol. 587, issue 7834, 408-413

Abstract: Abstract The oxygen evolution reaction has an important role in many alternative-energy schemes because it supplies the protons and electrons required for converting renewable electricity into chemical fuels1–3. Electrocatalysts accelerate the reaction by facilitating the required electron transfer4, as well as the formation and rupture of chemical bonds5. This involvement in fundamentally different processes results in complex electrochemical kinetics that can be challenging to understand and control, and that typically depends exponentially on overpotential1,2,6,7. Such behaviour emerges when the applied bias drives the reaction in line with the phenomenological Butler–Volmer theory, which focuses on electron transfer8, enabling the use of Tafel analysis to gain mechanistic insight under quasi-equilibrium9–11 or steady-state assumptions12. However, the charging of catalyst surfaces under bias also affects bond formation and rupture13–15, the effect of which on the electrocatalytic rate is not accounted for by the phenomenological Tafel analysis8 and is often unknown. Here we report pulse voltammetry and operando X-ray absorption spectroscopy measurements on iridium oxide to show that the applied bias does not act directly on the reaction coordinate, but affects the electrocatalytically generated current through charge accumulation in the catalyst. We find that the activation free energy decreases linearly with the amount of oxidative charge stored, and show that this relationship underlies electrocatalytic performance and can be evaluated using measurement and computation. We anticipate that these findings and our methodology will help to better understand other electrocatalytic materials and design systems with improved performance.

Date: 2020
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Citations: View citations in EconPapers (29)

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DOI: 10.1038/s41586-020-2908-2

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