Life-Like Materials and Systems, Department of Chemistry, University of Mainz, Duesbergweg 10-14, 55128, Mainz, Germany.
Present address: Department of Cancer Biology, Dana-Farber Cancer Institute and Wyss Institute for Biologically Inspired Engineering, Harvard Medical School, Boston, MA 02115, USA.
Angew Chem Int Ed Engl. 2022 Nov 7;61(45):e202208951. doi: 10.1002/anie.202208951. Epub 2022 Oct 7.
Liquid-liquid phase separation provides a versatile approach to fabricating cell-mimicking coacervates. Recently, it was discovered that phase separation of single-stranded DNA (ssDNA) allows for forming protocells and microgels in multicomponent systems. However, the mechanism of the ssDNA phase separation is not comprehensively understood. Here, we present mechanistic insights into the metal-dependent phase separation of ssDNA and leverage this understanding for a straightforward formation of all-DNA droplets. Two phase separation temperatures are found that correspond to the formation of primary nuclei and a growth process. Ca allows for irreversible, whereas Mg leads to reversible phase separation. Capitalizing on these differences makes it possible to control the information transfer of one-component DNA droplets and two-component core-shell protocells. This study introduces new kinetic traps of phase separating ssDNA that lead to new phenomena in cell-mimicking systems.
液-液相分离为制备细胞模拟凝聚提供了一种通用的方法。最近，人们发现单链 DNA（ssDNA）的相分离可以在多组分系统中形成原细胞和微凝胶。然而，ssDNA 相分离的机制尚未得到全面理解。在这里，我们提出了对 ssDNA 金属依赖性相分离的机制见解，并利用这一认识来直接形成全 DNA 液滴。发现了两个相分离温度，分别对应于初级核的形成和生长过程。Ca 允许不可逆相分离，而 Mg 则导致可逆相分离。利用这些差异，可以控制单组分 DNA 液滴和双组分核壳原细胞的信息传递。本研究介绍了 ssDNA 相分离的新动力学陷阱，这些陷阱导致了细胞模拟系统中的新现象。
