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Single-atom heterogeneous catalysts based on distinct carbon nitride scaffolds

National Science Review 2018年第5期5卷 642-652页

作者： Zupeng Chen evgeniya vorobyeva Sharon Mitchell Edvin Fako Nuúria López Sean M.Collins Rowan K.Leary Paul A.Midgley RolAND Hauert Javier Pérez-Ramírez Institute for Chemical and Bioengineering Department of Chemistry and Applied BiosciencesETHZurich Institute of Chemical Research of Catalonia (ICIQ) The Barcelona Institute of Science and Technology 3. Department of Materials Science and MetallurgyUniversity of Cambridge 4. EmpaSwiss Federal Laboratories for Materials Science and Technology

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 ***, 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.

关键词： single-atom heterogeneous catalysts carbon nitride scaffolds alkyne semi-hydrogenation density functional theory metal–host interaction

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