Katla Sai Krishna, Lin Chenyu, Pérez-Mercader Juan
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138-1204.
Santa Fe Institute, Santa Fe, NM 87501.
Proc Natl Acad Sci U S A. 2025 Jun 3;122(22):e2412514122. doi: 10.1073/pnas.2412514122. Epub 2025 May 27.
We investigate mechanisms for the observed nonlinear growth in the number of polymer vesicles generated during a photo-Reversible Addition-Fragmentation Chain Transfer-based polymerization-induced self-assembly (PISA) reaction. Our experimental results reveal the presence of a self-reproduction process during which chemically active polymer protocells are chemically and autonomously generated in a light-stimulated one-pot reaction that starts from a homogeneous blend of non-self-assembling molecules and which, as observed microscopically, form vesicular objects that grow and multiply (reproduce) during irradiation with green light (530 nm) as the reaction proceeds. By using a filtration-based protocol, our experiments demonstrate that the self-reproduction process occurs concomitantly with the PISA process and results in a nonlinear increase in the number of polymer vesicles during photopolymerization which can only be ascribed to their reproduction via polymeric spores ejected from previously existing first-generation vesicles. The second and subsequent generations' vesicles also self-reproduce and continue the process of population growth.
我们研究了在基于光可逆加成-断裂链转移的聚合诱导自组装(PISA)反应中,所观察到的聚合物囊泡数量非线性增长的机制。我们的实验结果揭示了一种自我复制过程的存在,在此过程中,化学活性聚合物原细胞在光刺激的一锅反应中通过化学方式自主生成,该反应起始于非自组装分子的均匀混合物,并且如显微镜观察所示,随着反应进行,在绿光(530 nm)照射下形成囊泡状物体,这些物体在照射过程中生长并繁殖(复制)。通过基于过滤的实验方案,我们的实验表明自我复制过程与PISA过程同时发生,并导致光聚合过程中聚合物囊泡数量的非线性增加,这只能归因于它们通过从先前存在的第一代囊泡中喷出的聚合物孢子进行复制。第二代及后续代次的囊泡也会自我复制并继续种群增长过程。