Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness
Protocells capable of nonenzymatic metabolism and environmental adaptation are essential models for understanding the emergence of cellular life. However, existing protocell designs often lack the robustness or prebiotic relevance to explain how functional supramolecular assemblies could have formed...
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2025
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| _version_ | 1849927644323250176 |
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| author | Shuai Cao (775058) |
| author2 | Guangle Li (4458430) Peng Zhou (116747) Ehud Gazit (231491) Xuehai Yan (591222) Chengqian Yuan (4746615) |
| author2_role | author author author author author |
| author_facet | Shuai Cao (775058) Guangle Li (4458430) Peng Zhou (116747) Ehud Gazit (231491) Xuehai Yan (591222) Chengqian Yuan (4746615) |
| author_role | author |
| dc.creator.none.fl_str_mv | Shuai Cao (775058) Guangle Li (4458430) Peng Zhou (116747) Ehud Gazit (231491) Xuehai Yan (591222) Chengqian Yuan (4746615) |
| dc.date.none.fl_str_mv | 2025-11-24T15:06:27Z |
| dc.identifier.none.fl_str_mv | 10.1021/jacs.5c15328.s002 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/dataset/Entropy-Driven_Amino_Acid-Based_Coacervates_with_Enzyme-Free_Metabolism_and_Prebiotic_Robustness/30695512 |
| dc.rights.none.fl_str_mv | CC BY-NC 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Biophysics Biochemistry Cell Biology Genetics Evolutionary Biology Environmental Sciences not elsewhere classified Astronomical and Space Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Information Systems not elsewhere classified sustaining biochemical complexity structures autonomously generate stress tolerance within geochemically plausible pathway exhibit exceptional resilience driven amino acid compact spherical morphologies also adaptively remodel 6 – 2 sudden environmental changes early earth conditions prebiotic pigment synthesis including sulfur metabolism δph ≈ 0 form membraneless protocells sup >+</ sup prebiotic conditions environmental adaptation prebiotic relevance nonenzymatic metabolism free metabolism work highlights synergistic effect selective enrichment results establish proton gradient nonenzymatic catalysis mediated hydrogen living systems interfacial acceleration integrating compartmentalization high salinity functional protocells free reactions extraterrestrial bodies essential models energy transduction divalent cations coacervation process cellular life bridge nonliving bonding networks based systems based microcompartments based coacervates antiport activity |
| dc.title.none.fl_str_mv | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| dc.type.none.fl_str_mv | Dataset info:eu-repo/semantics/publishedVersion dataset |
| description | Protocells capable of nonenzymatic metabolism and environmental adaptation are essential models for understanding the emergence of cellular life. However, existing protocell designs often lack the robustness or prebiotic relevance to explain how functional supramolecular assemblies could have formed under early Earth conditions. In this study, we demonstrate that simple amino acid derivatives, observed on extraterrestrial bodies and under simulated prebiotic Earth conditions, undergo entropy-driven liquid–liquid phase separation to form membraneless protocells through a self-coacervation process. The synergistic effect of selective enrichment of metabolites and interfacial acceleration in these coacervate microdroplets enhances enzyme-free reactions, including sulfur metabolism and prebiotic pigment synthesis. The protocells are stabilized by water-mediated hydrogen-bonding networks and exhibit exceptional resilience to prebiotically plausible stressorssuch as high salinity (up to 4.0 M NaCl), high concentrations of divalent cations (4.0 M Mg<sup>2+</sup>/Ca<sup>2+</sup>), UV radiation, and extreme temperature fluctuationswhich typically disrupt existing vesicle-based systems. Remarkably, these structures autonomously generate and maintain a proton gradient (ΔpH ≈ 0.6–2.1) across their interfaces, enabling primitive chemiosmotic coupling via Na<sup>+</sup>–H<sup>+</sup> antiport activity. They also adaptively remodel into compact spherical morphologies in response to sudden environmental changes, thereby preserving structural integrity. By integrating compartmentalization, nonenzymatic catalysis, energy transduction, and stress tolerance within a minimalist amino acid framework, our results establish a geochemically plausible pathway for the formation and persistence of functional protocells. This work highlights the potential of coacervate-based microcompartments to bridge nonliving and living systems by sustaining biochemical complexity under prebiotic conditions. |
| eu_rights_str_mv | openAccess |
| id | Manara_c57be69c2a7053e24ae00606ef38669e |
| identifier_str_mv | 10.1021/jacs.5c15328.s002 |
| network_acronym_str | Manara |
| network_name_str | ManaraRepo |
| oai_identifier_str | oai:figshare.com:article/30695512 |
| publishDate | 2025 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY-NC 4.0 |
| spelling | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic RobustnessShuai Cao (775058)Guangle Li (4458430)Peng Zhou (116747)Ehud Gazit (231491)Xuehai Yan (591222)Chengqian Yuan (4746615)BiophysicsBiochemistryCell BiologyGeneticsEvolutionary BiologyEnvironmental Sciences not elsewhere classifiedAstronomical and Space Sciences not elsewhere classifiedBiological Sciences not elsewhere classifiedChemical Sciences not elsewhere classifiedInformation Systems not elsewhere classifiedsustaining biochemical complexitystructures autonomously generatestress tolerance withingeochemically plausible pathwayexhibit exceptional resiliencedriven amino acidcompact spherical morphologiesalso adaptively remodel6 – 2sudden environmental changesearly earth conditionsprebiotic pigment synthesisincluding sulfur metabolismδph ≈ 0form membraneless protocellssup >+</ supprebiotic conditionsenvironmental adaptationprebiotic relevancenonenzymatic metabolismfree metabolismwork highlightssynergistic effectselective enrichmentresults establishproton gradientnonenzymatic catalysismediated hydrogenliving systemsinterfacial accelerationintegrating compartmentalizationhigh salinityfunctional protocellsfree reactionsextraterrestrial bodiesessential modelsenergy transductiondivalent cationscoacervation processcellular lifebridge nonlivingbonding networksbased systemsbased microcompartmentsbased coacervatesantiport activityProtocells capable of nonenzymatic metabolism and environmental adaptation are essential models for understanding the emergence of cellular life. However, existing protocell designs often lack the robustness or prebiotic relevance to explain how functional supramolecular assemblies could have formed under early Earth conditions. In this study, we demonstrate that simple amino acid derivatives, observed on extraterrestrial bodies and under simulated prebiotic Earth conditions, undergo entropy-driven liquid–liquid phase separation to form membraneless protocells through a self-coacervation process. The synergistic effect of selective enrichment of metabolites and interfacial acceleration in these coacervate microdroplets enhances enzyme-free reactions, including sulfur metabolism and prebiotic pigment synthesis. The protocells are stabilized by water-mediated hydrogen-bonding networks and exhibit exceptional resilience to prebiotically plausible stressorssuch as high salinity (up to 4.0 M NaCl), high concentrations of divalent cations (4.0 M Mg<sup>2+</sup>/Ca<sup>2+</sup>), UV radiation, and extreme temperature fluctuationswhich typically disrupt existing vesicle-based systems. Remarkably, these structures autonomously generate and maintain a proton gradient (ΔpH ≈ 0.6–2.1) across their interfaces, enabling primitive chemiosmotic coupling via Na<sup>+</sup>–H<sup>+</sup> antiport activity. They also adaptively remodel into compact spherical morphologies in response to sudden environmental changes, thereby preserving structural integrity. By integrating compartmentalization, nonenzymatic catalysis, energy transduction, and stress tolerance within a minimalist amino acid framework, our results establish a geochemically plausible pathway for the formation and persistence of functional protocells. This work highlights the potential of coacervate-based microcompartments to bridge nonliving and living systems by sustaining biochemical complexity under prebiotic conditions.2025-11-24T15:06:27ZDatasetinfo:eu-repo/semantics/publishedVersiondataset10.1021/jacs.5c15328.s002https://figshare.com/articles/dataset/Entropy-Driven_Amino_Acid-Based_Coacervates_with_Enzyme-Free_Metabolism_and_Prebiotic_Robustness/30695512CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/306955122025-11-24T15:06:27Z |
| spellingShingle | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness Shuai Cao (775058) Biophysics Biochemistry Cell Biology Genetics Evolutionary Biology Environmental Sciences not elsewhere classified Astronomical and Space Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Information Systems not elsewhere classified sustaining biochemical complexity structures autonomously generate stress tolerance within geochemically plausible pathway exhibit exceptional resilience driven amino acid compact spherical morphologies also adaptively remodel 6 – 2 sudden environmental changes early earth conditions prebiotic pigment synthesis including sulfur metabolism δph ≈ 0 form membraneless protocells sup >+</ sup prebiotic conditions environmental adaptation prebiotic relevance nonenzymatic metabolism free metabolism work highlights synergistic effect selective enrichment results establish proton gradient nonenzymatic catalysis mediated hydrogen living systems interfacial acceleration integrating compartmentalization high salinity functional protocells free reactions extraterrestrial bodies essential models energy transduction divalent cations coacervation process cellular life bridge nonliving bonding networks based systems based microcompartments based coacervates antiport activity |
| status_str | publishedVersion |
| title | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| title_full | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| title_fullStr | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| title_full_unstemmed | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| title_short | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| title_sort | Entropy-Driven Amino Acid-Based Coacervates with Enzyme-Free Metabolism and Prebiotic Robustness |
| topic | Biophysics Biochemistry Cell Biology Genetics Evolutionary Biology Environmental Sciences not elsewhere classified Astronomical and Space Sciences not elsewhere classified Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Information Systems not elsewhere classified sustaining biochemical complexity structures autonomously generate stress tolerance within geochemically plausible pathway exhibit exceptional resilience driven amino acid compact spherical morphologies also adaptively remodel 6 – 2 sudden environmental changes early earth conditions prebiotic pigment synthesis including sulfur metabolism δph ≈ 0 form membraneless protocells sup >+</ sup prebiotic conditions environmental adaptation prebiotic relevance nonenzymatic metabolism free metabolism work highlights synergistic effect selective enrichment results establish proton gradient nonenzymatic catalysis mediated hydrogen living systems interfacial acceleration integrating compartmentalization high salinity functional protocells free reactions extraterrestrial bodies essential models energy transduction divalent cations coacervation process cellular life bridge nonliving bonding networks based systems based microcompartments based coacervates antiport activity |