As the preliminary synthetic analogs of living cells, protocells with life-like features serve as a versatile platform to explore the origin of life. Although protocells constructed from multiple components have been developed, the transition of primitive cellular compartments toward structural complexity and advanced function remains a scientific challenge. Herein, a programmable pathway is established to exploit a simple chemistry to construct structural transition of protocell models from emulsion droplets, nanocapsules to molecularly crowded droplets. The transitional process toward distinct cell-like compartments is driven by interfacial self-assembly of simple components and regulated by physicochemical cues (e.g., mechanical force, solvent evaporation, acid/base equilibrium) triggered dynamic covalent chemistry. These protocell models are further studied by comparing their compartmentalization behavior, sequestration efficiency, and the ability to enrich biomolecules (e.g., enzyme and substrate) toward catalytic reaction or biological activity within the compartments. The results showcase physiochemical cues-driven programmable transition of life-like compartments toward functionalization, and offer a new step toward the design of living soft materials.

中文翻译：

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通过物理化学线索触发的界面动态共价化学指导合成原始细胞模型的转变

作为活细胞的初步合成类似物，具有类似生命特征的原始细胞可作为探索生命起源的多功能平台。尽管已经开发出由多种成分构成的原始细胞，但原始细胞区室向结构复杂性和高级功能的转变仍然是一项科学挑战。在这里，建立了一个可编程的途径，利用一种简单的化学方法来构建从乳液液滴、纳米胶囊到分子拥挤液滴的原细胞模型的结构转变。向不同细胞样隔室的过渡过程由简单组分的界面自组装驱动，并由物理化学信号（例如机械力、溶剂蒸发、酸/碱平衡）触发的动态共价化学调节。这些原始细胞模型通过比较它们的区室化行为、隔离效率以及使生物分子（例如酶和底物）富集到区室内的催化反应或生物活性的能力来进一步研究。结果展示了物理化学线索驱动的类生命隔间向功能化的可编程转变，并为设计活体软材料迈出了新的一步。