Nature Communications · 2019 · 500 citations · 33 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistryReaction EngineeringCatalytic MaterialsElectrochemical CellsElectrochemical Energy ConversionElectrode MaterialsNanocatalysisRedox-active MaterialsCarbon Dioxide ElectroreductionCarbon Dioxide ReductionCarbon Dioxide Reduction CatalysisElectrocatalystsElectrocatalytic Carbon Dioxide ReductionElectrochemical ReductionNoble Metal CatalysisProduct Selectivity
Abstract Molecular catalysts that combine high product selectivity and high current density for CO 2 electrochemical reduction to CO or other chemical feedstocks are urgently needed. While earth-abundant metal-based molecular electrocatalysts with high selectivity for CO 2 to CO conversion are known, they are characterized by current densities that are significantly lower than those obtained with solid-state metal materials. Here, we report that a cobalt phthalocyanine bearing a trimethyl ammonium group appended to the phthalocyanine macrocycle is capable of reducing CO 2 to CO in water with high activity over a broad pH range from 4 to 14. In a flow cell configuration operating in basic conditions, CO production occurs with excellent selectivity (ca. 95%), and good stability with a maximum partial current density of 165 mA cm −2 (at −0.92 V vs. RHE), matching the most active noble metal-based nanocatalysts. These results represent state-of-the-art performance for electrolytic carbon dioxide reduction by a molecular catalyst.
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Visible-light-driven methane formation from CO2 with a molecular iron catalyst
Heng Rao, Luciana C. Schmidt, Julien Bonin et al. · Nature · 2017 · 1K citations
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