title: Self-reproducing catalyst drives repeated phospholipid synthesis and membrane growth.
abstract: Cell membranes are dynamic structures found in all living organisms. There have been numerous constructs that model phospholipid membranes. However, unlike natural membranes, these biomimetic systems cannot sustain growth owing to an inability to replenish phospholipid-synthesizing catalysts. Here we report on the design and synthesis of artificial membranes embedded with synthetic, self-reproducing catalysts capable of perpetuating phospholipid bilayer formation. Replacing the complex biochemical pathways used in nature with an autocatalyst that also drives lipid synthesis leads to the continual formation of triazole phospholipids and membrane-bound oligotriazole catalysts from simpler starting materials. In addition to continual phospholipid synthesis and vesicle growth, the synthetic membranes are capable of remodeling their physical composition in response to changes in the environment by preferentially incorporating specific precursors. These results demonstrate that complex membranes capable of indefinite self-synthesis can emerge when supplied with simpler chemical building blocks.
authors.affiliation: Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093;
authors.forename: Michael D
authors.initials: MD
authors.lastname: Hardy
authors.affiliation: Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093;
authors.forename: Jun
authors.initials: J
authors.lastname: Yang
authors.affiliation: The BioCircuits Institute, University of California, San Diego, La Jolla, CA 92093.
authors.forename: Jangir
authors.initials: J
authors.lastname: Selimkhanov
authors.affiliation: Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093;
authors.forename: Christian M
authors.initials: CM
authors.lastname: Cole
authors.affiliation: The BioCircuits Institute, University of California, San Diego, La Jolla, CA 92093.
authors.forename: Lev S
authors.initials: LS
authors.lastname: Tsimring
authors.affiliation: Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093; ndevaraj@ucsd.edu.
authors.forename: Neal K
authors.initials: NK
authors.lastname: Devaraj
mesh_terms: D002384:Catalysis; D002462:Cell Membrane / Q000737:chemistry* / Q000378:metabolism; D003300:Copper / Q000737:chemistry / Q000378:metabolism; D061565:Cycloaddition Reaction; D008051:Lipid Bilayers / Q000737:chemistry* / Q000378:metabolism; D009682:Magnetic Resonance Spectroscopy; D008563:Membrane Lipids / Q000138:chemical synthesis / Q000737:chemistry* / Q000378:metabolism; D008567:Membranes, Artificial; D018613:Microscopy, Confocal; D046529:Microscopy, Electron, Transmission; D008956:Models, Chemical; D015394:Molecular Structure; D010713:Phosphatidylcholines / Q000138:chemical synthesis / Q000737:chemistry / Q000378:metabolism; D010743:Phospholipids / Q000096:biosynthesis / Q000138:chemical synthesis / Q000737:chemistry*; D059008:Time-Lapse Imaging; D014230:Triazoles / Q000138:chemical synthesis / Q000737:chemistry / Q000378:metabolism; D053835:Unilamellar Liposomes / Q000737:chemistry
chemical_list: D008051:Lipid Bilayers; D008563:Membrane Lipids; D008567:Membranes, Artificial; D010713:Phosphatidylcholines; D010743:Phospholipids; D014230:Triazoles; D053835:Unilamellar Liposomes; D003300:Copper; C028694:1-palmitoyl-2-oleoylphosphatidylcholine
keywords: autocatalysis; lipids; membranes; self-assembly