Sn-Decorated Cu/Cu2O Electrodes Enable Selective CO2 Reduction to Formic Acid under Realistic Flue Gas Streams.

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Theelectrochemical reductionofCO2 is typically investigatedunderpureCO2 feeds,butpracticaldeploymentmust addressmorecomplexanddilutesourcessuchasfluegases.Here, we studied Cu/Cu2O electrodes decorated with tin (Sn) synthesizedusing a scalable electrodepositionmethodandpost treatments under both pureCO2 and reactive nitrogen oxide containingsimulatedfluegas, towardformicacidsynthesis.Raman spectroscopyandAtomicForceMicroscopyanalysesrevealedthat flue gas exposure induces heterogeneous restructuring of the electrodewith surface roughening, surface carbonate formation, andlocalizedredepositionprocesses.Optimalcatalystperformance underpureCO2wasachievedwithintermediateSncoverageof3 minelectrodeposition, deliveringFaradaic efficiencies of 80%andproduction rates of 370μmol cm−2 h−1. Sn-modifiedCu2O electrodes alsoexhibitedhigh selectivity toward formic acidunder acidic gas containing simulatedflue gas, reachingFaradaic efficienciesof90%albeitatproductionratesof113μmolcm−2h−1,despitea10-foldreducedCO2partialpressure.Theseresults demonstratethat interfacialSn−CustructuresenabledselectiveCO2RRevenunderchallengingfeedconditions,pointingoutboth theopportunitiesandlimitationsof translatinglaboratory-scalecatalysts torealisticgasstreams.

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Plasma derived flue gas, Oxide derived copper, CO2 electroreduction

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