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The phase behaviour of amphiphilic multiblock copolymers with a large numberof blocks in semidilute solutions is studied by lattice Monte Carlosimulations. The influence on the resulting structures of the concentration,the solvent quality and the ratio of hydrophobic to hydrophilic monomers in thechains has been assessed explicitely. Several distinct regimes are put inevidence. For poorly substituted (mainly hydrophilic) copolymers formation ofmicelles is observed, either isolated or connected by the hydrophilic moieties,depending on concentration and chain length. For more highly substituted chainslarger tubular hydrophobic structures appear which, at higher concentration,join to form extended hydrophobic cores. For both substitution ratios gelationis observed, but with a very different gel network structure. For the poorlysubstituted chains the gel consists of micelles cross-linked by hydrophilicblocks whereas for the highly substituted copolymers the extended hydrophobiccores form the gelling network. The interplay between gelation and phaseseparation clearly appears in the phase diagram. In particular, for poorlysubstituted copolymers and in a narrow concentration range, we observe asol-gel transition followed by an inverse gel-sol transition when increasingthe interaction energy. The simulation results are discussed in the context ofthe experimentally observed phase properties of methylcellulose, ahydrophobically substituted polysaccharide.

Micelle formation, gelation and phase separation of amphiphilic multiblock copolymers