Castellano R K, Clark R, Craig S L, Nuckolls C, Rebek J
The Skaggs Institute for Chemical Biology and Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road, La Jolla, CA 92037, USA.
Proc Natl Acad Sci U S A. 2000 Nov 7;97(23):12418-21. doi: 10.1073/pnas.97.23.12418.
Synthetic self-assembled systems combine responsiveness and reversibility with the ability to perform chemical tasks such as molecular recognition and catalysis. An unmet challenge is the construction of polymeric materials that, like nature's tubulin, are simultaneously reversible and capable of useful physical tasks. We report here a class of reversibly formed polymers that show covalent-polymer mechanical integrity in solution and in the solid state. Non-Newtonian, polymeric behavior is observed despite the low molecular weight of the individual subunits and the seemingly weak forces holding the assemblies together. These polymers assemble through self-complementary hydrogen bonding and by physical encapsulation of small molecules; accordingly, the emergent macroscopic structure and function can be controlled by appropriate chemical signals.
合成自组装系统将响应性和可逆性与执行诸如分子识别和催化等化学任务的能力结合起来。一个尚未解决的挑战是构建像天然微管蛋白一样同时具有可逆性且能够执行有用物理任务的聚合材料。我们在此报告一类可逆形成的聚合物,它们在溶液和固态中都表现出共价聚合物的机械完整性。尽管单个亚基的分子量较低且将组装体维系在一起的力看似较弱,但仍观察到了非牛顿型的聚合行为。这些聚合物通过自互补氢键以及小分子的物理包封进行组装;因此,可通过适当的化学信号来控制所呈现出的宏观结构和功能。