Journal of the American Chemical Society · 2021 · 273 citations · 42 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistryNanomaterialsCatalyst DesignElectrochemical CellsElectrochemical Energy ConversionElectrode MaterialsFuel CellsRedox-active MaterialsElectrochemical ConversionElectrochemical StabilityMetal-air BatteriesMetal-organic Framework CatalystsMetal-organic FrameworksOxygen Reduction CatalystsOxygen Reduction ReactionZinc-air Batteries
Platinum (Pt)-based-nanomaterials are currently the most successful catalysts for the oxygen reduction reaction (ORR) in electrochemical energy conversion devices such as fuel cells and metal-air batteries. Nonetheless, Pt catalysts have serious drawbacks, including low abundance in nature, sluggish kinetics, and very high costs, which limit their practical applications. Herein, we report the first rationally designed nonprecious Co–Cu bimetallic metal–organic framework (MOF) using a low-temperature hydrothermal method that outperforms the electrocatalytic activity of Pt/C for ORR in alkaline environments. The MOF catalyst surpassed the ORR performance of Pt/C, exhibiting an onset potential of 1.06 V vs RHE, a half-wave potential of 0.95 V vs RHE, and a higher electrochemical stability (ΔE1/2 = 30 mV) after 1000 ORR cycles in 0.1 M NaOH. Additionally, it outperformed Pt/C in terms of power density and cyclability in zinc-air batteries. This outstanding behavior was attributed to the unique electronic synergy of the Co−Cu bimetallic centers in the MOF network, which was revealed by XPS and PDOS.
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From molecules to solids with the DMol3 approach
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