Department of Chemistry and Physics, Emmanuel College, 400 The Fenway, Boston, Massachusetts 02115, United States.
ACS Appl Mater Interfaces. 2023 Feb 8;15(5):6274-6282. doi: 10.1021/acsami.2c15626. Epub 2023 Jan 30.
Calcium materials, such as calcium carbonate, are produced in natural and industrial settings that range from oceanic to biomedical. An array of biological and biomimetic template molecules have been employed in controlling and understanding the mineralization reaction but have largely focused on small molecule additives or disordered polyelectrolytes. DNA aptamers are synthetic and programmable biomolecules with polyelectrolyte characteristics but with predictable and controllable secondary structure akin to native extracellular moieties. This work demonstrates for the first time the influence of DNA aptamers with known G-quadruplex structures on calcium carbonate mineralization. Aptamers demonstrate kinetic inhibition of mineral formation, sequence and pH-dependent uptake into the mineral, and morphological control of the primarily calcite material in controlled solution conditions. In reactions initiated from the complex matrix of ocean water, DNA aptamers demonstrated enhancement of mineralization kinetics and resulting amorphous material. This work provides new biomimetic tools to employ in controlled mineralization and demonstrates the influence that template secondary structure can have in material formation.
钙材料,如碳酸钙,是在从海洋到生物医学等各种自然和工业环境中产生的。人们已经使用了一系列生物和仿生模板分子来控制和理解矿化反应,但主要集中在小分子添加剂或无序聚电解质上。DNA 适体是具有聚电解质特性的合成和可编程生物分子,但具有类似于天然细胞外部分的可预测和可控的二级结构。这项工作首次证明了具有已知 G-四链体结构的 DNA 适体对碳酸钙矿化的影响。适体表现出对矿物形成的动力学抑制、序列和 pH 依赖性摄取进入矿物以及在受控溶液条件下对主要方解石材料的形态控制。在从海水的复杂基质中引发的反应中,DNA 适体表现出矿化动力学的增强和无定形物质的产生。这项工作提供了新的仿生工具来进行受控矿化,并证明了模板二级结构在材料形成中可能具有的影响。