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A dissipative pathway for the structural evolution of DNA fibres
Nature Chemistry ( IF 19.2 ) Pub Date : 2021-08-09 , DOI: 10.1038/s41557-021-00751-w
Felix J Rizzuto 1 , Casey M Platnich 1 , Xin Luo 1 , Yao Shen 2 , Michael D Dore 1 , Christophe Lachance-Brais 1 , Alba Guarné 2 , Gonzalo Cosa 1 , Hanadi F Sleiman 1
Affiliation  

Biochemical networks interconnect, grow and evolve to express new properties as different chemical pathways are selected during a continuous cycle of energy consumption and transformation. In contrast, synthetic systems that push away from equilibrium usually return to the same self-assembled state, often generating waste that limits system recyclability and prevents the formation of adaptable networks. Here we show that annealing by slow proton dissipation selects for otherwise inaccessible morphologies of fibres built from DNA and cyanuric acid. Using single-molecule fluorescence microscopy, we observe that proton dissipation influences the growth mechanism of supramolecular polymerization, healing gaps within fibres and converting highly branched, interwoven networks into nanocable superstructures. Just as the growth kinetics of natural fibres determine their structural attributes to modulate function, our system of photoacid-enabled depolymerization and repolymerization selects for healed materials to yield organized, robust fibres. Our method provides a chemical route for error-checking, distinct from thermal annealing, that improves the morphologies and properties of supramolecular materials using out-of-equilibrium systems.



中文翻译:

DNA纤维结构进化的耗散途径

随着在能源消耗和转化的连续循环中选择不同的化学途径,生化网络相互连接、发展和发展以表达新的特性。相比之下,脱离平衡的合成系统通常会恢复到相同的自组装状态,通常会产生限制系统可回收性并阻止形成适应性网络的废物。在这里,我们展示了通过慢质子耗散进行的退火选择了由 DNA 和氰尿酸构建的纤维的其他难以接近的形态。使用单分子荧光显微镜,我们观察到质子耗散影响超分子聚合的生长机制,修复纤维内的间隙并将高度支化的交织网络转化为纳米电缆超结构。正如天然纤维的生长动力学决定其结构属性以调节功能一样,我们的光酸解聚和再聚合系统选择愈合材料以产生有组织、坚固的纤维。我们的方法提供了一种不同于热退火的错误检查化学途径,该方法使用失衡系统改善了超分子材料的形态和性能。

更新日期:2021-08-09
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