Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Kyoto 615-8510, Japan.
J Am Chem Soc. 2009 Apr 22;131(15):5580-5. doi: 10.1021/ja8098239.
Logic-gate operations displaying macroscopic outputs are promising systems for the development of intelligent soft materials that can perform effective functions in response to various input patterns. A supramolecular hydrogel comprising the phosphate-type hydrogelator 1 exhibits macroscopic gel-sol behavior in response to four distinct input stimuli: temperature, pH, Ca(2+), and light. We characterized this performance through microscopic, spectroscopic, and rheological measurements. On the basis of its multiple-stimulus responsiveness, we constructed gel-based supramolecular logic gates from hydrogelator 1 that demonstrated AND, OR, NAND, and NOR types of stimulus-responsive gel-sol behavior in the presence of various combinations of the four stimuli. Implementation of such logic-gate functions into semiwet soft materials (e.g., supramolecular hydrogels) is an important step toward the design of controlled drug delivery and release systems. Indeed, we demonstrate herein that one of our gel-based supramolecular logic gates is capable of holding and releasing bioactive substances in response to logic triggers. Furthermore, combining our supramolecular gel-based AND logic gate with a photoresponsive supramolecular gel could temporarily modulate the release rate of the bioactive substance.
逻辑门操作显示宏观输出是开发智能软材料的有前途的系统,这些软材料可以对各种输入模式做出有效响应。包含磷酸盐型水凝胶形成剂 1 的超分子水凝胶在响应四种不同输入刺激时表现出宏观的凝胶-溶胶行为:温度、pH 值、Ca(2+)和光。我们通过微观、光谱和流变学测量来表征这种性能。基于其多刺激响应性,我们从水凝胶形成剂 1 构建了基于凝胶的超分子逻辑门,在存在四种刺激的各种组合的情况下,该逻辑门表现出了 AND、OR、NAND 和 NOR 类型的刺激响应的凝胶-溶胶行为。将这种逻辑门功能实现到半湿软材料(例如超分子水凝胶)中是设计控制药物输送和释放系统的重要步骤。事实上,我们在此证明,我们的基于凝胶的超分子逻辑门之一能够根据逻辑触发器来保持和释放生物活性物质。此外,将我们的基于超分子凝胶的 AND 逻辑门与光响应超分子凝胶结合使用,可以暂时调节生物活性物质的释放速率。