Data set for the journal article: The Spatial Distribution of Cobalt Phthalocyanine and Copper Nanocubes Controls the Selectivity towards C2 Products in Tandem Electrocatalytic CO2 Reduction
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Data set for the journal article: The coupling of CO-generating molecular catalysts with copper electrodes in tandem schemes is a promising strategy to boost the formation of multi-carbon products in the electrocatalytic reduction of CO<sub>2</sub>. While the spatial distribution of the two components is important, this aspect remains underexplored, especially for molecular-based tandem systems. Herein, we address this knowledge gap by studying tandem catalysts comprising Co-phthalocyanine (CoPc) and Cu nanocubes (Cu<sub>cub</sub>). In particular, we identify the importance of the relative spatial distributions of the two components on the performance of the tandem catalyst by preparing CoPc-Cu<sub>cub</sub>/C, wherein the CoPc and Cu<sub>cub</sub> share an interface, and CoPc-C/Cu<sub>cub</sub>, wherein the CoPc is loaded first on carbon black (C) before mixing with the Cu<sub>cub</sub>. The electrocatalytic measurements of these two catalysts show that the faradaic efficiency towards C<sub>2 </sub>products almost doubles for the CoPc-Cu<sub>cub</sub>/C, whereas it decreases by half for the CoPc-C/Cu<sub>cub</sub>, compared to the Cu<sub>cub</sub>/C. Our results highlight the importance of a direct contact between the CO-generating molecular catalyst and the Cu to promote C-C coupling, which hints at a surface transport mechanism of the CO intermediate between the two components of the tandem catalyst instead of a transfer via CO diffusion in the electrolyte followed by re-adsorption.



