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J Am Chem Soc. 2011 Apr 6;133(13):4742-5. doi: 10.1021/ja2004494. Epub 2011 Mar 15.

Single-chain folding of polymers for catalytic systems in water.

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Institute for Complex Molecular Systems, Laboratory of Macromolecular and Organic Chemistry, Laboratory of Chemical Biology, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands.


Enzymes are a source of inspiration for chemists attempting to create versatile synthetic catalysts. In order to arrive at a polymeric chain carrying catalytic units separated spatially, it is a prerequisite to fold these polymers in water into well-defined compartmentalized architectures thus creating a catalytic core. Herein, we report the synthesis, physical properties, and catalytic activity of a water-soluble segmented terpolymer in which a helical structure in the apolar core is created around a ruthenium-based catalyst. The supramolecular chirality of this catalytic system is the result of the self-assembly of benzene-1,3,5-tricarboxamide side chains, while the catalyst arises from the sequential ruthenium-catalyzed living radical polymerization of the different monomers followed by ligand exchange. The polymers exhibit a two-state folding process and show transfer hydrogenation in water.

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