Institut für Organische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569, Stuttgart, Germany.
Chemistry. 2019 Dec 2;25(67):15288-15294. doi: 10.1002/chem.201903631. Epub 2019 Oct 22.
Nanoscale assemblies of DNA strands are readily designed and can be generated in a wide range of shapes and sizes. Turning them into solids that bind biomolecules reversibly, so that they can act as active material in flow cells, is a challenge. Among the biomolecular ligands, cofactors are of particular interest because they are often the most expensive reagents of biochemical transformations, for which controlled release and recycling are desirable. We have recently described DNA triplex motifs that bind adenine-containing cofactors, such as NAD, FAD and ATP, reversibly with low micromolar affinity. We sought ways to convert the soluble DNA motifs into a macroporous solid for cofactor binding. While assemblies of linear and branched DNA motifs produced hydrogels with undesirable properties, long DNA triplexes treated with protamine gave materials suitable for flow cells. Using exchangeable cells in a flow system, thermally controlled loading and discharge were demonstrated. Employing a flow cell loaded with ATP, bioluminescence was induced through thermal release of the cofactor. The results show that materials generated from functional DNA structures can be successfully employed in macroscopic devices.
DNA 链的纳米级组装体可以很容易地设计，并可以生成各种形状和大小。将它们转化为可以可逆地结合生物分子的固体，使其能够在流动池中作为活性材料发挥作用，这是一个挑战。在生物分子配体中，辅因子特别有趣，因为它们通常是生化转化中最昂贵的试剂，需要控制其释放和回收。我们最近描述了 DNA 三螺旋基序，这些基序可以与包含腺嘌呤的辅因子（如 NAD、FAD 和 ATP）以低微摩尔亲和力可逆结合。我们寻求将可溶性 DNA 基序转化为用于辅因子结合的大孔固体的方法。虽然线性和支化 DNA 基序的组装体产生了具有不理想性质的水凝胶，但用鱼精蛋白处理的长 DNA 三螺旋体得到了适合流动池的材料。在流动系统中使用可交换的细胞，证明了热控制的加载和卸载。使用装有 ATP 的流动池，通过热释放辅因子诱导生物发光。结果表明，从功能 DNA 结构生成的材料可以成功地用于宏观器件中。
