Data set for the journal article: Tandem electrocatalytic CO2 reduction with Fe-porphyrins and Cu nanocubes enhances ethylene production

Copper-based tandem schemes have emerged as promising strategies to promote the formation
of multi-carbon products of the electrocatalytic CO2 reduction reaction. In such approaches,
the CO-generating component of the tandem catalyst increases the local concentration of CO
and thereby enhances the intrinsic carbon-carbon (C-C) coupling on copper. However, the
optimal characteristics of the CO-generating catalyst for maximizing eventual C2 production
are currently unknown. In this work, we developed tunable tandem catalysts comprising iron
porphyrin (Fe-Por), as the CO-generating component, and Cu nanocubes (Cucub) to understand
how the turnover frequency for CO (TOFCO) of the molecular catalysts impacts C-C coupling
on the Cu surface. First, we tuned the TOFCO of the Fe-Por by varying the number of orbitals
involved in the π-system. Then, by coupling these molecular catalysts with the Cucub, we
assessed the current densities and faradaic efficiencies, discovering that all of the designed Fe-
Por boost ethylene production. The most efficient Cucub/Fe-Por tandem catalyst was the one
including the Fe-Por with the highest TOFCO and exhibited a nearly 22-fold increase in the
ethylene selectivity and 100 mV positive shift of the onset potential with respect to the pristine
Cucub. These results reveal that coupling the TOFCO tunability of molecular catalysts along with
copper nanocatalysts opens up new possibilities towards the development of Cu-based catalysts
with enhanced selectivity for multi-carbon product generation at low overpotential.