Abstract

The development of inexpensive, earth abundant, and bioinspired oxygen evolution electrocatalysts that are easily accessible and scalable is a principal requirement with regard to the feasibility of water splitting for large-scale chemical energy storage. A unique, versatile, and scalable approach has been developed to fabricate manganese oxide films from single layers to multilayers with a controlled thickness and high reproducibility. The produced MnOx films are composed of small nanostructures that are assembled closely in the form of porous sponge-like layers. The films were investigated for the electrochemical oxygen evolution reaction in alkaline media and demonstrate a remarkable activity as well as a superior stability of over 60 h. To elucidate the catalytically active species, as well as the striking structural characteristics, the films were further examined in depth by using SEM, TEM, and X-ray photoelectron spectroscopy, as well as quasi in situ extended X-ray absorption fine structure and X-ray absorption near edge structure analysis. The MnOx catalyst films excel because of a favorably high fraction of Mn3+ ions that are retained even after operation at oxidizing potentials. Upon exposure to oxidizing potentials in strongly alkaline aqueous electrolyte, the catalyst material maintains its structural integrity at the nanostructural, morphological, and atomic level.

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