Assembling oppositely charged lock and key responsive colloids: A mesoscale analog of adaptive chemistry.
Assembling oppositely charged lock and key responsive colloids: A mesoscale analog of adaptive chemistry.
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DOI：
10.1126/sciadv.1700321
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发表时间：
2017-09
期刊：
影响因子：
13.6
通讯作者：
Crassous JJ
中科院分区：
文献类型：
--
作者：
Mihut AM;Stenqvist B;Lund M;Schurtenberger P;Crassous JJ
具有互补几何结构的相反带电的热响应粒子被组装成自适应的胶体分子。我们已经看到了胶体科学中的相当大的努力，以复制自然的成功策略，通过自组装来制造复杂的功能结构。这包括尝试设计胶体构建块及其分子间相互作用，例如创建定向分子相互作用、分子识别、主客体系统和特定结合的胶体类似物。我们证明，我们可以使用形状互补的相反带电的热响应粒子，如球形和碗形粒子，来实现外部可控的锁和钥匙自组装机制。可调静电相互作用的使用与这些构建块的依赖于温度的大小和形状以及van der Waals相互作用相结合，提供了对相互作用和自组装过程的选择性和专一性的精细控制。该机制的动态性质允许通过各种结构的可逆循环，范围从弱结构的稠密液体到通过温度和离子强度的变化而具有不同构型的定义良好的分子形状的团簇。我们将这种复杂而动态的自组装行为与相关的分子相互作用联系起来，如屏蔽库仑力和范德华力以及这两个构件的几何互补性，并在最近引入分子系统的适应性化学概念的背景下讨论了我们的发现。
Oppositely charged thermoresponsive particles with complementary geometries are assembled into adaptive colloidal molecules. We have seen a considerable effort in colloid sciences to copy Nature’s successful strategies to fabricate complex functional structures through self-assembly. This includes attempts to design colloidal building blocks and their intermolecular interactions, such as creating the colloidal analogs of directional molecular interactions, molecular recognition, host-guest systems, and specific binding. We show that we can use oppositely charged thermoresponsive particles with complementary shapes, such as spherical and bowl-shaped particles, to implement an externally controllable lock-and-key self-assembly mechanism. The use of tunable electrostatic interactions combined with the temperature-dependent size and shape and van der Waals interactions of these building blocks provides an exquisite control over the selectivity and specificity of the interactions and self-assembly process. The dynamic nature of the mechanism allows for reversibly cycling through various structures that range from weakly structured dense liquids to well-defined molecule-shaped clusters with different configurations through variations in temperature and ionic strength. We link this complex and dynamic self-assembly behavior to the relevant molecular interactions, such as screened Coulomb and van der Waals forces and the geometrical complementarity of the two building blocks, and discuss our findings in the context of the concepts of adaptive chemistry recently introduced to molecular systems.
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