Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution View Full Text


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

2017-05

AUTHORS

Alexis Grimaud, Oscar Diaz-Morales, Binghong Han, Wesley T. Hong, Yueh-Lin Lee, Livia Giordano, Kelsey A. Stoerzinger, Marc T. M. Koper, Yang Shao-Horn

ABSTRACT

Understanding how materials that catalyse the oxygen evolution reaction (OER) function is essential for the development of efficient energy-storage technologies. The traditional understanding of the OER mechanism on metal oxides involves four concerted proton-electron transfer steps on metal-ion centres at their surface and product oxygen molecules derived from water. Here, using in situ 18O isotope labelling mass spectrometry, we provide direct experimental evidence that the O2 generated during the OER on some highly active oxides can come from lattice oxygen. The oxides capable of lattice-oxygen oxidation also exhibit pH-dependent OER activity on the reversible hydrogen electrode scale, indicating non-concerted proton-electron transfers in the OER mechanism. Based on our experimental data and density functional theory calculations, we discuss mechanisms that are fundamentally different from the conventional scheme and show that increasing the covalency of metal-oxygen bonds is critical to trigger lattice-oxygen oxidation and enable non-concerted proton-electron transfers during OER. More... »

PAGES

457

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/nchem.2695

DOI

http://dx.doi.org/10.1038/nchem.2695

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1050615355

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/28430191


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