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  Key role of chemistry versus bias in electrocatalytic oxygen evolution

Nong, H. N., Falling, L., Bergmann, A., Klingenhof, M., Tran, H. P., Spöri, C., et al. (2020). Key role of chemistry versus bias in electrocatalytic oxygen evolution. Nature, 587, 408-413. doi:10.1038/s41586-020-2908-2.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0007-7532-D Version Permalink: http://hdl.handle.net/21.11116/0000-0007-760A-A
Genre: Journal Article

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Nong, Hong Nhan1, 2, Author
Falling, Lorenz3, Author              
Bergmann, Arno4, Author              
Klingenhof, Malte1, Author
Tran, Hoang Phi1, Author
Spöri, Camillo1, Author
Mom, Rik3, Author              
Timoshenko, Janis4, Author              
Knop-Gericke, Axel2, 3, Author              
Picicinin, Simone5, Author
Pérez-Ramírez, Javier6, Author
Roldan Cuenya, Beatriz4, Author              
Schlögl, Robert2, 3, Author              
Strasser, Peter1, Author
Teschner, Detre2, 3, Author              
Jones, Travis3, Author              
Affiliations:
1Department of Chemistry, Chemical and Materials Engineering Division, The Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin, Berlin, Germany, ou_persistent22              
2Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
5Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche, CNR-IOM, Trieste, Italy, ou_persistent22              
6Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Zurich, Switzerland, ou_persistent22              

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 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 fuels. Electrocatalysts accelerate the reaction by facilitating the required electron transfer, 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 overpotential. Such behaviour emerges when the applied bias drives the reaction in line with the phenomenological Butler–Volmer theory, which focuses on electron transfer, enabling the use of Tafel analysis to gain mechanistic insight under quasi-equilibrium or steady-state assumptions. However, the charging of catalyst surfaces under bias also affects bond formation and rupture, 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.

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Language(s): eng - English
 Dates: 2020-11-142020-09-162020-11-182020-11-19
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41586-020-2908-2
 Degree: -

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Title: Nature
  Abbreviation : Nature
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: 7 Volume / Issue: 587 Sequence Number: - Start / End Page: 408 - 413 Identifier: ISSN: 0028-0836
CoNE: https://pure.mpg.de/cone/journals/resource/954925427238