Abstract
Noble metal oxides such as ruthenium dioxide are highly active electrocatalysts for anodic reactions in acidic electrolytes, but dissolution during electrochemical operation impedes wide-scale application in renewable energy technologies. Improving the fundamental understanding of the dissolution dynamics of application-relevant morphologies such as nanocrystals is critical for grid-scale implementation of these materials. Herein we report the nanoscale heterogeneity observed via liquid phase transmission electron microscopy during ruthenium dioxide nanocrystal dissolution under oxidizing conditions. Single-crystalline ruthenium dioxide nanocrystals enabled direct observation of dissolution along different crystallographic facets, allowing an unprecedented direct comparison of crystal facet stability. The nanoscale observations revealed substantial heterogeneity in the relative stability of crystallographic facets across different nanocrystals, attributed to nanoscale strains present in these crystals. These findings highlight the importance of nanoscale heterogeneity in determining macroscale properties such as electrocatalyst stability and provide a characterization methodology that can be integrated into next-generation electrocatalyst discovery efforts.
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Supplementary Movie 1
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In-situ TEM movie montage of (111)-tipped RuO2 nanocrystals in graphene liquid cells prepared with 25 mM FeCl3, 25 mM MgCl2, and 100 mM HCl exposed to an electron dose of 2,000 e- Å–2 s-1.
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Supplementary Movie 2
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In-situ TEM movie montage of (001)-tipped RuO2 nanocrystals in graphene liquid cells prepared with 25 mM FeCl3, 25 mM MgCl2, and 100 mM HCl exposed to an electron dose of 2,000 e- Å–2 s-1.
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Supplementary Movie 3
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In-situ TEM movie montage of RuO2 nanocrystals in graphene liquid cells prepared with 50 mM MgCl2 and 100 mM HCl exposed to an electron dose of 2,000 e- Å–2 s-1.
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Supplementary weblinks
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Data from: "Dissolution heterogeneity observed in anisotropic ruthenium dioxide nanocrystals via liquid-phase transmission electron microscopy"
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Duke Research Data Repository
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