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@ARTICLE{GonzlezGaitano:189818,
      author       = {González-Gaitano, Gustavo and Müller, Céline and
                      Radulescu, Aurel and Dreiss, Cécile A.},
      title        = {{M}odulating the {S}elf-{A}ssembly of {A}mphiphilic
                      {X}-{S}haped {B}lock {C}opolymers with {C}yclodextrins:
                      {S}tructure and {M}echanisms},
      journal      = {Langmuir},
      volume       = {31},
      number       = {14},
      issn         = {1520-5827},
      address      = {Washington, DC},
      publisher    = {ACS Publ.},
      reportid     = {FZJ-2015-02836},
      pages        = {4096 - 4105},
      year         = {2015},
      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 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.},
      cin          = {JCNS (München) ; Jülich Centre for Neutron Science JCNS
                      (München) ; JCNS-FRM-II / Neutronenstreuung ; JCNS-1},
      ddc          = {670},
      cid          = {I:(DE-Juel1)JCNS-FRM-II-20110218 /
                      I:(DE-Juel1)JCNS-1-20110106},
      pnm          = {6G15 - FRM II / MLZ (POF3-6G15) / 6G4 - Jülich Centre for
                      Neutron Research (JCNS) (POF3-623)},
      pid          = {G:(DE-HGF)POF3-6G15 / G:(DE-HGF)POF3-6G4},
      experiment   = {EXP:(DE-MLZ)KWS2-20140101},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000353177200007},
      pubmed       = {pmid:25785814},
      doi          = {10.1021/acs.langmuir.5b00334},
      url          = {https://juser.fz-juelich.de/record/189818},
}