Nature Communications · 2022 · 485 citations · 67 references
Natural SciencesChemical EngineeringChemistryCatalysisInorganic ChemistryPhysical ChemistryCatalyst DesignCatalytic MaterialsCluster ChemistryFuel CellsRedox CatalysisRedox-active MaterialsCatalyst Structure - Activity RelationshipsElectron TransferElectron Transfer PathwaysOxygen Reduction CatalystsOxygen Reduction ReactionSingle-atom CatalystsSingle-site CatalystsTurnover Frequency
Abstract Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
67
VMD: Visual molecular dynamics
William Humphrey, Andrew Dalke, Klaus Schulten · Journal of Molecular Graphics · 1996 · 66.6K citations
Wenjie Jiang, Lin Gu, Li Li et al. · Journal of the American Chemical Society · 2016 · 1.8K citations
Natural Sciences, Chemical Engineering, Materials Science +17