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Abstract

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 elec-
troreduction 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.