Abstract

The self-reproduction of supramolecular assemblies based on the synthesis and self-assembly of building blocks is a critical step towards the construction of chemical systems with autonomous, adaptive, and propagation properties. In this report, we demonstrate that giant vesicles can grow and produce daughter vesicles by synthesizing and incorporating phospholipids in situ from ad-hoc precursors. Our model involves acyl chain elongation via copper(I)-catalyzed azide-alkyne [3 + 2] cycloaddition reaction and the ensuing production of synthetic phospholipids to induce budding and division. In addition, the growth and budding of giant vesicles were compatible with the encapsulation and transfer of macromolecules as large as lambda phage DNA to the buds. This chemical system provides a useful model towards the implementation of cell-like compartments capable of propagation and transport of biological materials.

Highlights

  • Shape transformations and fission in GVs have been demonstrated using various methods, the capability to control these processes to couple budding and growth and afford spherical, single-walled daughter vesicles with diameters of approximately 5 μm through division remains limited

  • Immature mother GVs composed of ad-hoc precursors

  • The collective results strongly suggest that the growth, budding, and division of the mature mothers GVs can be directly attributed to the addition of the catalytic solution and membrane precursors. 1H nuclear magnetic resonance (NMR) and image analyses demonstrated that these dynamics are linked to phospholipid synthesis and the production of additional membrane surface

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Summary

Introduction

Shape transformations and fission in GVs have been demonstrated using various methods, the capability to control these processes to couple budding and growth and afford spherical, single-walled daughter vesicles with diameters of approximately 5 μm through division remains limited. Compartmentalization and transport of macromolecules and reagents within self-reproducing systems are critical requirements for the synthesis of dynamic microreactors and model protocells In vesicular systems, this step has been limited in part by the size and inner structure of the mother and daughter vesicles. Upon addition of a catalytic solution and ad-hoc precursors, this vesicular system readily forms a synthetic phosphatidylcholine containing a triazole ring at its hydrophobic chain (TPC). This additional membrane component becomes integrated into the GV membrane, determining its own growth, budding, and division. Owing to their size (approximately 5 μm in diameter) and nominal single-walled structure, macromolecules as large as lambda phage DNA (48 kb) were encapsulated within the immature mother GVs and later observed in the buds

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