The multi-carbon (C2+) alcohols produced by electrochemical CO2 reduction, such as ethanol and n-propanol, are considered as indispensable liquid energy carriers. In most C-C coupling cases, however, the concomitant gaseous C2H4 product results in the low selectivity of C2+ alcohols. Here, we report rational construction of mesostructured CuO electrocatalysts, specifically mesoporous CuO (m-CuO) and cylindrical CuO (c-CuO), enables selective distribution of C2+ products. The m-CuO and c-CuO show similar selectivity towards total C2+ products (≥76 %), but the corresponding predominant products are C2+ alcohols (55 %) and C2H4 (52 %), respectively. The ordered mesostructure not only induces the surface hydrophobicity, but selectively tailors the adsorption configuration of *CO intermediate: m-CuO prefers bridged adsorption, whereas c-CuO favors top adsorption as revealed by in situ spectroscopies. Computational calculations unravel that bridged *CO adsorbate is prone to deep protonation into *OCH3 intermediate, thus accelerating the coupling of *CO and *OCH3 intermediates to generate C2+ alcohols; by contrast, top *CO adsorbate is apt to undergo conventional C-C coupling process to produce C2H4. This work illustrates selective C2+ products distribution via mesostructure manipulation, and paves a new path into the design of efficient electrocatalysts with tunable adsorption configuration of key intermediates for targeted products.
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Li et al. (2024) studied this question.
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