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Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity
DOI:10.1038/s41467-021-26743-5.png)
Abstract
En 中文
To rationally design effective and stable catalysts for energy conversion applications, we need to understand how they transform under reaction conditions and reveal their underlying structure-property relationships. This is especially important for catalysts used in the electroreduction of carbon dioxide where product selectivity is sensitive to catalyst structure. Here, we present real-time electrochemical liquid cell transmission electron microscopy studies showing the restructuring of copper(I) oxide cubes during reaction. Fragmentation of the solid cubes, re-deposition of new nanoparticles, catalyst detachment and catalyst aggregation are observed as a function of the applied potential and time. Using cubes with different initial sizes and loading, we further correlate this dynamic morphology with the catalytic selectivity through time-resolved scanning electron microscopy measurements and product analysis. These comparative studies reveal the impact of nanoparticle re-deposition and detachment on the catalyst reactivity, and how the increased surface metal loading created by re-deposited nanoparticles can lead to enhanced C2+ selectivity and stability. Understanding the changes that occur in catalysts during reaction are key to the rational design. Here, the authors use electrochemical transmission electron microscopy and time-resolved product analysis to unveil how cubic copper oxide catalysts evolve during electrochemical CO2 reduction, linking their structural transformations with their selectivity.
Keywords:
CELL ELECTRON-MICROSCOPY
CARBON-DIOXIDE
GROWTH
DEGRADATION
CHALLENGES
CONVERSION
RESOLUTION
CHEMISTRY
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