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000189818 1001_ $$0P:(DE-HGF)0$$aGonzález-Gaitano, Gustavo$$b0$$eCorresponding Author
000189818 245__ $$aModulating the Self-Assembly of Amphiphilic X-Shaped Block Copolymers with Cyclodextrins: Structure and Mechanisms
000189818 260__ $$aWashington, DC$$bACS Publ.$$c2015
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000189818 520__ $$aInclusion complexes between cyclodextrins and polymers—so-called pseudopolyrotaxanes (PPR)—are at the origin of fascinating supramolecular structures, which are finding increasing uses in biomedical and technological fields. Here we explore the impact of both native and a range of modified cyclodextrins (CD) on the self-assembly of X-shaped poly(ethylene oxide)–poly(propylene oxide) block copolymers, so-called Tetronics or poloxamines, by focusing on Tetronic 904 (T904, Mw 6700). The effects are markedly dependent on the type and arrangement of the substituents on the macrocycle. While native CDs drive the formation of a solid PPR, most substituted CDs induce micellar breakup, with dimethylated β-CD (DIMEB) having the strongest impact and randomly substituted CDs a much weaker disruptive effect. Using native α-CD as a “molecular trap”, we perform competitive binding experiments—where two types of CDs thread together onto the polymer chains—to establish that DIMEB indeed has the highest propensity to form an inclusion complex with the polymer, while hydroxypropylated CDs do not thread. 1D 1H NMR and ROESY experiments confirm the formation of a soluble PPR with DIMEB in which the CD binds preferentially to the PO units, thus providing the drive for the observed demicellization. A combination of dynamic light scattering (DLS) and small-angle neutron scattering (SANS) is used to extract detailed structural parameters on the micelles. A binding model is proposed, which exploits the chemical shifts of selected protons from the CD in conjunction with the Hill equation, to prove that the formation of the PPR is a negatively cooperative process, in which threaded DIMEBs hamper the entrance of subsequent macrocycles.
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000189818 65017 $$0V:(DE-MLZ)GC-1602-2016$$2V:(DE-HGF)$$aPolymers, Soft Nano Particles and  Proteins$$x2
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000189818 7001_ $$0P:(DE-HGF)0$$aMüller, Céline$$b1
000189818 7001_ $$0P:(DE-Juel1)130905$$aRadulescu, Aurel$$b2$$ufzj
000189818 7001_ $$0P:(DE-HGF)0$$aDreiss, Cécile A.$$b3
000189818 773__ $$0PERI:(DE-600)2005937-1$$a10.1021/acs.langmuir.5b00334$$gVol. 31, no. 14, p. 4096 - 4105$$n14$$p4096 - 4105$$tLangmuir$$v31$$x1520-5827$$y2015
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