Single-atom heterogeneous catalysts based on distinct carbon nitride scaffolds
Zupeng Chen,Evgeniya Vorobyeva,Sharon Mitchell,Edvin Fako,Núria López,Sean M. Collins,Rowan K. Leary,Paul A. Midgley,Roland Hauert,Javier Pérez-Ramírez +9 more
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In this article, the authors demonstrate that palladium atoms can be effectively isolated on other carbon nitride scaffolds including linear melem oligomers and poly(triazine/heptazine imides).Abstract:
Carbon nitrides integrating macroheterocycles offer unique potential as hosts for stabilizing metal atoms due to their rich electronic structure. To date, only graphitic heptazine-based polymers have been studied. Here, we demonstrate that palladium atoms can be effectively isolated on other carbon nitride scaffolds including linear melem oligomers and poly(triazine/heptazine imides). Increased metal uptake was linked to the larger cavity size and the presence of chloride ions in the polyimide structures. Changing the host structure leads to significant variation in the average oxidation state of the metal, which can be tuned by exchange of the ionic species as evidenced by X-ray photoelectron spectroscopy and supported by density functional theory. Evaluation in the semi-hydrogenation of 2-methyl-3-butyn-2-ol reveals an inverse correlation between the activity and the degree of oxidation of palladium, with oligomers exhibiting the highest activity. These findings provide new mechanistic insights into the influence of the carbon nitride structure on metal stabilization.read more
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Single-Atom Catalysts across the Periodic Table.
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Defect engineering in earth-abundant electrocatalysts for CO2 and N2 reduction
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Computational Screening of Efficient Single‐Atom Catalysts Based on Graphitic Carbon Nitride (g‐C3N4) for Nitrogen Electroreduction
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Surface Coordination Chemistry of Atomically Dispersed Metal Catalysts.
TL;DR: This review will illustrate how the local and vicinal coordination species on different support systems act together with the dispersed catalytic metal center to determine the catalytic activity, selectivity, and stability of ADCs.
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