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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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Dynamic Confinement Approach for High Metal Loading Single-Atom Catalysts Based on Covalent Organic Frameworks.

Kyung Seob Song^1,2, Murad Najafov^1,2, José Manuel González Acosta^3,4

¹Department of Chemistry, University of Fribourg, Chemin du Musee 9, Fribourg, 1700, Switzerland.

Angewandte Chemie (International Ed. in English)

|January 2, 2026

Summary

This summary is machine-generated.

This study introduces a new method for creating ultra-high metal loading single-atom catalysts (SACs) using palladium polyphthalocyanine covalent organic frameworks (COFs). The dynamic confinement strategy ensures catalyst stability and high performance in continuous flow reactions.

Keywords:

Flow chemistry Heterogeneous catalysis Platinum group metals Porous materials

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Area of Science:

Materials Science
Catalysis
Nanotechnology

Background:

Single-atom catalysts (SACs) provide well-defined active sites but face challenges in achieving high metal loadings without aggregation.
Developing stable SACs with high metal content is crucial for advanced catalytic applications.

Purpose of the Study:

To develop a synthetic strategy for ultra-high metal loading single-atom catalysts.
To investigate the use of palladium polyphthalocyanine covalent organic frameworks (COFs) for high-performance catalysis.
To explore the role of dynamic confinement in stabilizing single-atom catalysts.

Main Methods:

Synthesized palladium polyphthalocyanine COFs using a mixed metal ionothermal approach with PdCl2/ZnCl2 or PdCl2/ZnCl2/NaCl.
Employed theoretical simulations to understand the dynamic confinement of palladium atoms within the COF framework.
Evaluated catalyst performance under continuous flow conditions over 24 hours.

Main Results:

Achieved ultra-high palladium loadings up to 22.2 wt% in COFs with atomically dispersed Pd ions.
Demonstrated that the crystalline framework dynamically confines Pd atoms, preventing dimerization and ensuring long-term stability.
Catalysts exhibited stable performance with yields up to 90% in continuous flow reactions.

Conclusions:

The developed synthetic strategy enables ultra-high metal loading SACs.
Dynamic confinement within crystalline organic supports is key to achieving stable and high-performing SACs.
This work sets a new benchmark for SACs and offers a promising approach for catalyst design.