期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 127, 期 16, 页码 5928-5935出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja050713n
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Crystallographic analysis revealed that pyricline-palladium complexation is a good geometric match to the m-phenylene ethynylene (mPE) repeat unit and thus could serve as a reversible linking group to join oligomer segments together. A series of pyricline-terminated mPE oligomers were then synthesized and found to coordinate with palladium dichloride to give complexes effectively twice the length of the free oligomers. A quantitative analysis of these coordination equilibria by isothermal calorimetry found the ability of the pyricline end-group to form a coordination complex corresponded with their ability to fold. Oligomers that were able to form complexes of sufficient length to fold showed positive cooperativity based on experimental determination of their association constants with a palladium ion. We suggest that the additional free energy of complexation for the folded oligomers is analogous to chelation by multidentate ligands, but here the multidentate ligand is held together by supramolecular rather than covalent bonds.
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