The self‐assembly behaviour of a pH‐responsive amphiphile, mono‐N‐dodecyl phosphate (DDP) is illustrated on the front cover. As shown, they readily form vesicles over a very wide pH range by themselves, thereby providing a robust alternative to fatty acid‐based protocellular systems. This feature also provides a respite from the constraints that limit the environments that would have been suitable for the emergence of protocells on the early Earth. Further, they result in robust vesicles when mixed with other single‐ and di‐acyl chain derivatives. In all, the unique pH‐responsive nature of DDP‐based membranes highlights the advantages that these systems would have had for emergence of early functional cells and for the engineering of tuneable membranes with potential translational implications. [Designed by Ms. Tejal Vyas with critical scientific inputs from Dr. Chaitanya Mungi (Affiliation: Science Activity Centre at IISER Pune).] More information can be found in the Research Article by S. Sarkar, S. Rajamani et al.

Prebiotically plausible single-chain amphiphiles are enticing as model protocellular compartments to study the emergence of cellular life, owing to their self-assembling properties. Here, we investigated the self-assembly behaviour of mono-N-dodecyl phosphate (DDP) and mixed systems of DDP with 1-dodecanol (DDOH) at varying pH conditions. Membranes composed of DDP showed pH-responsive vesicle formation in a wide range of pH with a low critical bilayer concentration (CBC). Further, the addition of DDOH to DDP membrane system enhanced vesicle formation and stability in alkaline pH regimes. We also compared the high-temperature behaviour of DDP and DDP: DDOH membranes with conventional fatty acid membranes. Both, DDP and DDP:DDOH mixed membranes possess packing that is similar to decanoic acid membrane. However, the micropolarity of these systems is similar to phospholipid membranes. Finally, the pH-dependent modulation of different phospholipid membranes doped with DDP was also demonstrated to engineer tuneable membranes with potential translational implications.

Prebiotically plausible single-chain amphiphiles are enticing as model protocellular compartments to study the emergence of cellular life owing to their self-assembling properties. Here, we investigated the self-assembly behaviour of mono-N-dodecyl phosphate (DDP) and mixed systems of DDP with dodecyl 1-dodecanol (DOH) at varying pH conditions. Membranes composed of DDP showed pH-responsive vesicle formation in a wide range of pH with a low critical bilayer concentration (CBC). Further, the addition of DOH to DDP membrane system enhanced vesicle formation and stability in alkaline pH regimes. We also compared the high-temperature behaviour of DDP and DDP-DOH membranes with conventional fatty acid membranes. Both, DDP and DDP:DOH mixed membranes possess packing that is similar to decanoic acid membrane. However, the micropolarity of these systems are similar to phospholipid membranes. Finally, the pH-dependent modulation of different phospholipid membranes doped with DDP was also demonstrated to engineer tuneable membranes with potential translational implications.