Chemical & Biomolecular Engineering, Johns Hopkins University, Baltimore, MD, 21218, USA.
Our Lady of Lourdes High School, Poughkeepsie, NY, 12603, USA.
Nat Commun. 2020 Nov 27;11(1):6057. doi: 10.1038/s41467-020-19882-8.
Crystallization is a ubiquitous means of self-assembly that can organize matter over length scales orders of magnitude larger than those of the monomer units. Yet crystallization is notoriously difficult to control because it is exquisitely sensitive to monomer concentration, which changes as monomers are depleted during growth. Living cells control crystallization using chemical reaction networks that offset depletion by synthesizing or activating monomers to regulate monomer concentration, stabilizing growth conditions even as depletion rates change, and thus reliably yielding desired products. Using DNA nanotubes as a model system, here we show that coupling a generic reversible bimolecular monomer buffering reaction to a crystallization process leads to reliable growth of large, uniformly sized crystals even when crystal growth rates change over time. Buffering could be applied broadly as a simple means to regulate and sustain batch crystallization and could facilitate the self-assembly of complex, hierarchical synthetic structures.
结晶是一种普遍存在的自组装方式，可以将物质组织成比单体单元大几个数量级的长度尺度。然而，结晶非常难以控制，因为它对单体浓度极其敏感，而单体浓度会随着单体在生长过程中耗尽而变化。活细胞使用化学反应网络来控制结晶，这些网络通过合成或激活单体来补偿单体的消耗，从而调节单体浓度，即使在耗尽率发生变化的情况下，也能稳定生长条件，从而可靠地生成所需的产物。在这里，我们使用 DNA 纳米管作为模型系统，表明将通用的可逆双分子单体缓冲反应与结晶过程耦合，即使在晶体生长速率随时间变化的情况下，也能可靠地生长出大尺寸、均匀尺寸的晶体。缓冲可以作为一种简单的方法广泛应用于调节和维持批处理结晶，并可以促进复杂的、层次化的合成结构的自组装。
