Electrochemical conversion of carbon dioxide (CO2) to multi-carbon fuels and chemical feedstocks is important but remains challenging. Here we report the stabilization of Cu+ within a CuO-CeO2 interface for efficient...
The
development of highly active and selective electrocatalysts
with low cost and earth abundance for electrochemical CO2 reduction (ECR) remains an important area of interest. Here, we
report the modification of CuO with other metal (Bi, Sb, Cd, and Zr)
oxides to form bimetallic oxide nanocomposite catalysts exhibiting
efficient ECR. In particular, CuO-Sb2O3 nanoparticles
anchored on carbon black (CB) facilitated ECR selectively to CO at
low overpotentials, providing a CO faradaic efficiency (FE) of up
to 90.0% at −0.8 V versus reversible hydrogen electrode, in
contrast to individual CuO/CB and Sb2O3/CB,
which gave rise to CO FEs of less than 31.0%, outperforming many previously
reported catalysts. A strong interaction between CuO and Sb2O3 is found, which likely contributes to the enhanced
ECR activity.
Electrochemical CO2 transformation to high‐value ethylene (C2H4) at high currents and efficiencies is desired and yet remains a grand challenge. We show for the first time that coupling single Sb atoms and oxygen vacancies of CuO enable synergistic electrocatalytic reduction of CO2 to C2H4 at low overpotentials. Highly dispersed Sb atoms occupying metal substitutional sites of CuO are synthesized under mild conditions. The overall CO2 reduction faradaic efficiency (FE) reaches 89.3 ± 1.1% with an FE toward C2H4 exceeding 58.4% at a high‐current density of 500 mA/cm2. Addition of the p‐block metal is found to induce transformation of CuO from flakes to nanoribbons rich in nanoholes and oxygen vacancies, greatly enhancing CO2 adsorption and activation while suppressing hydrogen evolution. Further density functional theory calculations with in situ X‐ray diffraction reveal that combining Sb sites and oxygen vacancies prominently lessen the dimerization energy of adsorbed CO intermediate, thus boosting the conversion of CO2 to produce C2H4. This study provides a new perspective for promoting selective C–C coupling for electrochemical CO2 reduction.
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