Organocatalyzed bottom-up formation of protocells

Abstract

Abstract The organisation of living systems into cellular structures is a characteristic that enables differentiation from the environment. A pivotal step in the development of life is compartmentalisation, achieved through the formation of vesicle-like structures. Fatty acids - or phospholipids - have been used to simulate prebiotic vesicle and protocell formation. However, a process by which amphiphiles are formed from small prebiotically plausible molecules, which spontaneously self-assemble to protocells, is unknown. Here, we demonstrate that an organocatalytic reaction cascade starting from acetaldehyde with prebiotic imidazolidine-4-thione rapidly yields poly(hydroxy)alkenyl aldehydes that spontaneously self-assemble to protocells. In this process, lipid-like molecules (up to C20) develop a membrane, which additionally incorporates the organocatalyst at the liquid-lipid interface. These catalytically active protocells (11 nm – 7 μm) tolerate external influences such as pH value, temperature and salts. This finding unveils an organocatalytic pathway to selective lipid formation and spontaneous compartmentalisation without the necessity of preformed amphiphiles.