ProtectingCopper Oxidation State via IntermediateConfinement for Selective CO2 Electroreduction to C2+ Fuels
2020
Selective and efficient
catalytic conversion of carbon dioxide
(CO2) into value-added fuels and feedstocks provides an
ideal avenue to high-density renewable energy storage. An impediment
to enabling deep CO2 reduction to oxygenates and hydrocarbons
(e.g., C2+ compounds) is the difficulty of coupling carbon–carbon
bonds efficiently. Copper in the +1 oxidation state has been thought
to be active for catalyzing C2+ formation, whereas it is
prone to being reduced to Cu0 at cathodic potentials. Here
we report that catalysts with nanocavities can confine carbon intermediates
formed in situ, which in turn covers the local catalyst
surface and thereby stabilizes Cu+ species. Experimental
measurements on multihollow cuprous oxide catalyst exhibit a C2+ Faradaic efficiency of 75.2 ± 2.7% at a C2+ partial current density of 267 ± 13 mA cm–2 and a large C2+-to-C1 ratio of ∼7.2.
Operando Raman spectra, in conjunction with X-ray absorption studies,
confirm that Cu+ species in the as-designed catalyst are
well retained during CO2 reduction, which leads to the
marked C2+ selectivity at a large conversion rate.
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