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Abstract Prebiotically‐plausible compartmentalization mechanisms include membrane vesicles formed by amphiphile self‐assembly and coacervate droplets formed by liquid–liquid phase separation. Both types of structures form spontaneously and can be related to cellular compartmentalization motifs in today's living cells. As prebiotic compartments, they have complementary capabilities, with coacervates offering excellent solute accumulation and membranes providing superior boundaries. Herein, protocell models constructed by spontaneous encapsulation of coacervate droplets by mixed fatty acid/phospholipid and by purely fatty acid membranes are described. Coacervate‐supported membranes form over a range of coacervate and lipid compositions, with membrane properties impacted by charge–charge interactions between coacervates and membranes. Vesicles formed by coacervate‐templated membrane assembly exhibit profoundly different permeability than traditional fatty acid or blended fatty acid/phospholipid membranes without a coacervate interior, particularly in the presence of magnesium ions (Mg2+). While fatty acid and blended membrane vesicles are disrupted by the addition of Mg2+, the corresponding coacervate‐supported membranes remain intact and impermeable to externally‐added solutes. With the more robust membrane, fluorescein diacetate (FDA) hydrolysis, which is commonly used for cell viability assays, can be performed inside the protocell model due to the simple diffusion of FDA and then following with the coacervate‐mediated abiotic hydrolysis to fluorescein.
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This content will become publicly available on November 21, 2025
Thermophilic Behavior of Heat-Dissociative Coacervate Droplets
In exploring the genesis of life, liquid–liquid phase-separated coacervate droplets have been proposed as primitive protocells. Within the hydrothermal hypothesis, these droplets would emerge from molecule-rich hot fluids and thus be subjected to temperature gradients. Investigating their thermophoretic behavior can provide insights into protocell footprints in thermal landscapes, advancing our understanding of life’s origins. Here, we report the thermophilic behavior of heat-dissociative droplets, contrary to the intuition that heat-associative condensates would prefer hotter areas. This aspect implies the preferential presence of heat-dissociative primordial condensates near hydrothermal environments, facilitating molecular incorporation and biochemical syntheses. Additionally, our investigations reveal similarities between thermophoretic and electrophoretic motions, dictated by molecular redistribution within droplets due to their fluid nature, which necessitates revising current electrophoresis frameworks for surface charge characterization. Our study elucidates how coacervate droplets navigate thermal and electric fields, reveals their thermal-landscape-dependent molecular characteristics, and bridges foundational theories of early life: the hydrothermal and condensate-as-protocell hypotheses.
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- Award ID(s):
- 2001650
- PAR ID:
- 10563143
- Publisher / Repository:
- American Chemical Society
- Date Published:
- Journal Name:
- Nano Letters
- Volume:
- 24
- Issue:
- 50
- ISSN:
- 1530-6984
- Page Range / eLocation ID:
- 15964 to 15972
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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