Modulating the self-assembly of amphiphilic X-shaped block copolymers with cyclodextrins: structure and mechanisms

Langmuir : the ACS Journal of Surfaces and Colloids
Gustavo González-GaitanoCécile A Dreiss

Abstract

Inclusion 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 (1)H NMR and ROESY experiments confirm the formation of a soluble PPR with DIMEB in which the CD binds preferentially to the PO units, thus pr...Continue Reading

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Citations

May 6, 2015·Langmuir : the ACS Journal of Surfaces and Colloids·Gustavo González-GaitanoCécile A Dreiss
Jun 2, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Rafael Serra-GómezGustavo González-Gaitano
May 1, 2021·European Journal of Pharmaceutical Sciences : Official Journal of the European Federation for Pharmaceutical Sciences·Gabriel Bezerra Motta CâmaraFernanda Nervo Raffin
Dec 14, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Margarita ValeroCécile A Dreiss
Apr 18, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Joan Puig-RigallGustavo González-Gaitano
Sep 17, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Alae El HaitamiAurica Farcas
Nov 20, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Suresh Nayana LakshmiSharmistha Dutta Choudhury

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