Self-assembly of two-component gels: stoichiometric control and component selection.

[摘要]：Two-component systems capable of self-assembling into soft gel-phase materials are of considerable interest due to their tunability and versatility. This paper investigates two-component gels based on a combination of a L-lysine-based dendron and a rigid diamine spacer (1,4-diaminobenzene or 1,4-diaminocyclohexane). The networked gelator was investigated using thermal measurements, CD, NMR spectroscopy and small angle neutron scattering (SANS) giving insight into the macroscopic properties, nanostructure and mol.-scale organization. Surprisingly, all of these techniques confirmed that irresp. of the molar ratio of the components employed, the "solid-like" gel network always consisted of a 1:1 mixt. of dendron/diamine. Addnl., the gel network was able to tolerate a significant excess of diamine in the "liq.-like" phase before being disrupted. In the light of this observation, we investigated the ability of the gel network structure to evolve from mixts. of different arom. diamines present in excess. We found that these two-component gels assembled in a component-selective manner, with the dendron preferentially recognizing 1,4-diaminobenzene (> 70%), when similar competitor diamines (1,2- and 1,3-diaminobenzene) are present. Furthermore, NMR relaxation measurements demonstrated that the gel based on 1,4-diaminobenzene was better able to form a selective ternary complex with pyrene than the gel based on 1,4-diaminocyclohexane, indicative of controlled and selective p-p interactions within a three-component assembly. As such, the results in this paper demonstrate how component selection processes in two-component gel systems can control hierarchical self-assembly.

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