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@ARTICLE{Staropoli:821019,
      author       = {Staropoli, Mariapaola and Raba, Andreas and Hövelmann,
                      Claas H. and Krutyeva, Margarita and Allgaier, J. and
                      Appavou, Marie-Sousai and Keiderling, Uwe and Stadler,
                      Florian J. and Pyckhout-Hintzen, Wim and Wischnewski,
                      Andreas and Richter, Dieter},
      title        = {{H}ydrogen {B}onding in a {R}eversible {C}omb {P}olymer
                      {A}rchitecture: {A} {M}icroscopic and {M}acroscopic
                      {I}nvestigation},
      journal      = {Macromolecules},
      volume       = {49},
      number       = {15},
      issn         = {1520-5835},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {FZJ-2016-06276},
      pages        = {5692 - 5703},
      year         = {2016},
      abstract     = {In this work, an investigation of the hydrogen-bonding
                      mechanism in a transiently branched comb-like polymer system
                      in the melt is reported. The system under investigation
                      consists of a polybutylene oxide (PBO)-based backbone,
                      randomly functionalized with thymine (thy) groups, in
                      combination with shorter PBO graft chains,
                      end-functionalized with diaminotriazine (DAT) groups. The
                      functional groups are able to associate through hydrogen
                      bonding. The heterocomplementary association of these groups
                      leads to the formation of a transiently branched comb-like
                      polymer system. Since recently virtually exclusive
                      heterocomplementary association could be observed in the
                      supramolecular association of telechelically modified
                      oligomeric PEG chains, here we aim to extend the
                      supramolecular assembly mechanism toward branched
                      structures. The present work combines small angle neutron
                      scattering (SANS) experiments on a selectively labeled
                      system with macroscopic dynamics measured in linear rheology
                      response. The association of thy- and DAT-modified
                      components was studied as a function of temperature and
                      composition. The scattering function reveals the formation
                      of a block copolymer and can be exclusively attributed to
                      heterocomplementary association of the hydrogen-bonding
                      groups. Scattering functions of nonfunctionalized blends are
                      also reported as references and evidence the change in the
                      microstructure induced by the heterocomplementary
                      association. All scattering profiles were described by means
                      of the random phase approximation (RPA) formalism from which
                      the average aggregation number, i.e., comb arm functionality
                      and the equilibrium association constant could be determined
                      directly in the melt state as a function of temperature. On
                      the other hand, rheological measurements were performed in
                      the melt state to study the influence of the reversible
                      bonds on the macroscopic dynamics of the polymer system. The
                      rheology data are in good agreement with the SANS results
                      and confirm the transient comb-like branched architecture.
                      The supramolecular association exhibits characteristic
                      bonding times of the groups in the order of 1 s at −25 °C
                      and therefore makes the thy–DAT pair an ideal candidate
                      for the development of responsive materials that combine
                      permanent and transient linkages for novel applications and
                      self-healing properties.},
      cin          = {JCNS (München) ; Jülich Centre for Neutron Science JCNS
                      (München) ; JCNS-FRM-II / Neutronenstreuung ; JCNS-1 /
                      JCNS-2},
      ddc          = {540},
      cid          = {I:(DE-Juel1)JCNS-FRM-II-20110218 /
                      I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-2-20110106},
      pnm          = {6215 - Soft Matter, Health and Life Sciences (POF3-621) /
                      6G15 - FRM II / MLZ (POF3-6G15) / 6G4 - Jülich Centre for
                      Neutron Research (JCNS) (POF3-623)},
      pid          = {G:(DE-HGF)POF3-6215 / G:(DE-HGF)POF3-6G15 /
                      G:(DE-HGF)POF3-6G4},
      experiment   = {EXP:(DE-MLZ)KWS2-20140101},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000381320300039},
      doi          = {10.1021/acs.macromol.6b00978},
      url          = {https://juser.fz-juelich.de/record/821019},
}