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Chemoadaptive Polymeric Assemblies by Integrated Chemical Feedback in Self-Assembled Synthetic Protocells.

ABSTRACT: The design and chemical synthesis of artificial material objects which can mimic the functions of living cells is an important ongoing scientific endeavor. A key challenge necessary for fulfilling the criteria for a system to be living currently regards evolution, which is derived from adaptivity. Integrated chemical loops capable of feedback control are required to achieve chemical systems which exhibit adaptivity. To explore this, we present an integrated, two-component orthogonal chemical process involving reversible addition-fragmentation chain transfer (RAFT) based polymerization-induced self-assembly (PISA) and a copper-catalyzed azide-alkyne click (CuAAC) coupling reaction. The chemical processes are linked through electron transfer from the activated chain-transfer agent (CTA) to the dormant Cu(II) precatalyst. We show that combining these complementary chemistries in a single reaction pot resulted in two primary outcomes: (i) simplification of the PISA process to synthesize the macro-CTA in situ from available nonamphiphilic components and (ii) routes to complexity and adaptation involving population dynamics, morphologies, and dissipative phenomena observed during in situ microscopy analysis.

SUBMITTER: Pearce S

PROVIDER: S-EPMC8461774 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:BackgroundProtocell refers to the basic unit of life and synthetic molecular assembly with cell structure and function. The protocells have great applications in the field of biomedical technology. Simulating the morphology and function of cells is the key to the preparation of protocells. However, some organic solvents used in the preparation process of protocells would damage the function of the bioactive substance. Perfluorocarbon, which has no toxic effect on bioactive substances, is an ideal solvent for protocell preparation. However, perfluorocarbon cannot be emulsified with water because of its inertia.MethodsSpheroids can be formed in nature even without emulsification, since liquid can reshape the morphology of the solid phase through the scouring action, even if there is no stable interface between the two phases. Inspired by the formation of natural spheroids such as pebbles, we developed non-interfacial self-assembly (NISA) of microdroplets as a step toward synthetic protocells, in which the inert perfluorocarbon was utilized to reshape the hydrogel through the scouring action.ResultsThe synthetic protocells were successfully obtained by using NISA-based protocell techniques, with the morphology very similar to native cells. Then we simulated the cell transcription process in the synthetic protocell and used the protocell as an mRNA carrier to transfect 293T cells. The results showed that protocells delivered mRNAs, and successfully expressed proteins in 293T cells. Further, we used the NISA method to fabricate an artificial cell by extracting and reassembling the membrane, proteins, and genomes of ovarian cancer cells. The results showed that the recombination of tumor cells was successfully achieved with similar morphology as tumor cells. In addition, the synthetic protocell prepared by the NISA method was used to reverse cancer chemoresistance by restoring cellular calcium homeostasis, which verified the application value of the synthetic protocell as a drug carrier.ConclusionThis synthetic protocell fabricated by the NISA method simulates the occurrence and development process of primitive life, which has great potential application value in mRNA vaccine, cancer immunotherapy, and drug delivery.

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Chemoadaptive Polymeric Assemblies by Integrated Chemical Feedback in Self-Assembled Synthetic Protocells.

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