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Open accessJournal ArticleDOI: 10.1039/D0SC05650B

Spontaneous emergence of membrane-forming protoamphiphiles from a lipid–amino acid mixture under wet–dry cycles

04 Mar 2021-Chemical Science (Royal Society of Chemistry)-Vol. 12, Iss: 8, pp 2970-2978
Abstract: Dynamic interplay between peptide synthesis and membrane assembly would have been crucial for the emergence of protocells on the prebiotic Earth. However, the effect of membrane-forming amphiphiles on peptide synthesis, under prebiotically plausible conditions, remains relatively unexplored. Here we discern the effect of a phospholipid on peptide synthesis using a non-activated amino acid, under wet–dry cycles. We report two competing processes simultaneously forming peptides and N-acyl amino acids (NAAs) in a single-pot reaction from a common set of reactants. NAA synthesis occurs via an ester–amide exchange, which is the first demonstration of this phenomenon in a lipid–amino acid system. Furthermore, NAAs self-assemble into vesicles at acidic pH, signifying their ability to form protocellular membranes under acidic geothermal conditions. Our work highlights the importance of exploring the co-evolutionary interactions between membrane assembly and peptide synthesis, having implications for the emergence of hitherto uncharacterized compounds of unknown prebiotic relevance.

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Topics: Peptide synthesis (54%), Amino acid (53%)
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7 results found


Open accessJournal ArticleDOI: 10.1039/C6SC90026G
23 May 2016-Chemical Science
Abstract: Correction for ‘Fatty acids' double role in the prebiotic formation of a hydrophobic dipeptide’ by Sara Murillo-Sanchez et al., Chem. Sci., 2016, DOI: 10.1039/c5sc04796j.

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Topics: Dipeptide (54%)

29 Citations


Journal ArticleDOI: 10.1038/S41570-021-00329-7
Amit Kahana1, Doron Lancet1Institutions (1)
20 Oct 2021-
Abstract: Protocells at life’s origin are often conceived as bilayer-enclosed precursors of life, whose self-reproduction rests on the early advent of replicating catalytic biopolymers. This Perspective describes an alternative scenario, wherein reproducing nanoscopic lipid micelles with catalytic capabilities were forerunners of biopolymer-containing protocells. This postulate gains considerable support from experiments describing micellar catalysis and autocatalytic proliferation, and, more recently, from reports on cross-catalysis in mixed micelles that lead to life-like steady-state dynamics. Such results, along with evidence for micellar prebiotic compatibility, synergize with predictions of our chemically stringent computer-simulated model, illustrating how mutually catalytic lipid networks may enable micellar compositional reproduction that could underlie primal selection and evolution. Finally, we highlight studies on how endogenously catalysed lipid modifications could guide further protocellular complexification, including micelle to vesicle transition and monomer to biopolymer progression. These portrayals substantiate the possibility that protocellular evolution could have been seeded by pre-RNA lipid assemblies. We propose that life originated in spontaneously formed catalytic lipid micelles. Accumulating experimental evidence shows that such micelles undergo compositional autocatalytic reproduction. Lipid-first constitutes a parsimonious alternative to the RNA-first scenario.

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Topics: Protocell (55%)

2 Citations



Journal ArticleDOI: 10.1007/S11084-021-09613-4
Abstract: How life arose on the primitive Earth is one of the biggest questions in science. Biomolecular emergence scenarios have proliferated in the literature but accounting for the ubiquity of oxidized (+ 5) phosphate (PO43−) in extant biochemistries has been challenging due to the dearth of phosphate and molecular oxygen on the primordial Earth. A compelling body of work suggests that exogenous schreibersite ((Fe,Ni)3P) was delivered to Earth via meteorite impacts during the Heavy Bombardment (ca. 4.1–3.8 Gya) and there converted to reduced P oxyanions (e.g., phosphite (HPO32−) and hypophosphite (H2PO2−)) and phosphonates. Inspired by this idea, we review the relevant literature to deduce a plausible reduced phospholipid analog of modern phosphatidylcholines that could have emerged in a primordial hydrothermal setting. A shallow alkaline lacustrine basin underlain by active hydrothermal fissures and meteoritic schreibersite-, clay-, and metal-enriched sediments is envisioned. The water column is laden with known and putative primordial hydrothermal reagents. Small system dimensions and thermal- and UV-driven evaporation further concentrate chemical precursors. We hypothesize that a reduced phospholipid arises from Fischer–Tropsch-type (FTT) production of a C8 alkanoic acid, which condenses with an organophosphinate (derived from schreibersite corrosion to hypophosphite with subsequent methylation/oxidation), to yield a reduced protophospholipid. This then condenses with an α-amino nitrile (derived from Strecker-type reactions) to form the polar head. Preliminary modeling results indicate that reduced phospholipids do not aggregate rapidly; however, single layer micelles are stable up to aggregates with approximately 100 molecules.

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Topics: Schreibersite (53%)

1 Citations


Open accessJournal ArticleDOI: 10.3390/LIFE11060539
09 Jun 2021-Life
Abstract: Although the habitability of early Mars is now well established, its suitability for conditions favorable to an independent origin of life (OoL) has been less certain. With continued exploration, evidence has mounted for a widespread diversity of physical and chemical conditions on Mars that mimic those variously hypothesized as settings in which life first arose on Earth. Mars has also provided water, energy sources, CHNOPS elements, critical catalytic transition metal elements, as well as B, Mg, Ca, Na and K, all of which are elements associated with life as we know it. With its highly favorable sulfur abundance and land/ocean ratio, early wet Mars remains a prime candidate for its own OoL, in many respects superior to Earth. The relatively well-preserved ancient surface of planet Mars helps inform the range of possible analogous conditions during the now-obliterated history of early Earth. Continued exploration of Mars also contributes to the understanding of the opportunities for settings enabling an OoL on exoplanets. Favoring geochemical sediment samples for eventual return to Earth will enhance assessments of the likelihood of a Martian OoL.

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Topics: Mars Exploration Program (65%), Martian (55%)

1 Citations


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66 results found


Open accessJournal ArticleDOI: 10.1038/S41467-018-07882-8
Maksim Kunitski1, Nicolas Eicke2, Pia Huber1, Jonas Köhler1  +12 moreInstitutions (2)
Abstract: Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.

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Topics: Ionization (55%), Neon (54%)

4,138 Citations


Open accessJournal ArticleDOI: 10.1038/S41467-019-12176-8
Abstract: Policies aiming to preserve vegetated coastal ecosystems (VCE; tidal marshes, mangroves and seagrasses) to mitigate greenhouse gas emissions require national assessments of blue carbon resources. Here, we present organic carbon (C) storage in VCE across Australian climate regions and estimate potential annual CO2 emission benefits of VCE conservation and restoration. Australia contributes 5–11% of the C stored in VCE globally (70–185 Tg C in aboveground biomass, and 1,055–1,540 Tg C in the upper 1 m of soils). Potential CO2 emissions from current VCE losses are estimated at 2.1–3.1 Tg CO2-e yr-1, increasing annual CO2 emissions from land use change in Australia by 12–21%. This assessment, the most comprehensive for any nation to-date, demonstrates the potential of conservation and restoration of VCE to underpin national policy development for reducing greenhouse gas emissions. Policies aiming to preserve vegetated coastal ecosystems (VCE) to mitigate greenhouse gas emissions require national assessments of blue carbon resources. Here the authors assessed organic carbon storage in VCE across Australian and the potential annual CO2 emission benefits of VCE conservation and find that Australia contributes substantially the carbon stored in VCE globally.

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Topics: Greenhouse gas (55%), Climate change mitigation (55%), Blue carbon (53%) ... read more

1,404 Citations


Journal ArticleDOI: 10.1038/228923A0
05 Dec 1970-Nature
Abstract: Extraterrestrial abiotic amino acids and hydrocarbons in type II carbonaceous chondrite at Murchison, Australia

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Topics: Murchison meteorite (71%), Carbonaceous chondrite (63%), Isovaline (52%)

726 Citations


Journal ArticleDOI: 10.1007/BF01808177
John A. Baross1, Sarah E. Hoffman2Institutions (2)
Abstract: Submarine hydrothermal vents are the only comtemporary geological environment which may be called truly primeval; they continue to be a major source of gases and dissolved elements to the modern ocean as they were to the Archean ocean. Then, as now, they encompassed a multiplicity of physical and chemical gradients as a direct result of interactions between extensive hydrothermal activity in the Earth's crust and the overlying oceanic and atmospheric environments. We have proposed that these gradients provided the necessary multiple pathways for the abiotic synthesis of chemical compounds, origin and evolution of ‘precells’ and ‘precell’ communities and, ultimately, the evolution of free-living organisms. This hypothesis is consistent with the tectonic, paleontological, and degassing history of the earth and with the use of thermal energy sources in the laboratory to synthesize amino acids and complex organic compounds. In this paper, we expand upon the geophysical, chemical, and possible microbiological analogies between contemporary and Archean hydrothermal systems and suggest several hypotheses, related to our model for the origin and evolution of life at Archean vents, which can be tested in present-day hydrothermal systems.

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Topics: Hydrothermal vent (61%), Hydrothermal circulation (56%), Archean (51%)

448 Citations


Journal ArticleDOI: 10.1023/A:1006592502746
Abstract: Ever since their discovery in the late 1970's, mid-ocean-ridge hydrothermal systems have received a great deal of attention as a possible site for the origin of life on Earth (and environments analogous to mid-ocean-ridge hydrothermal systems are postulated to have been sites where life could have originated or Mars and elsewhere as well) Because no modern-day terrestrial hydrothermal systems are free from the influence of organic compounds derived from biologic processes, laboratory experiments provide the best opportunity for confirmation of the potential for organic synthesis in hydrothermal systems Here we report on the formation of lipid compounds during Fischer-Tropsch-type synthesis from aqueous solutions of formic acid or oxalic acid Optimum synthesis occurs in stainless steel vessels by heating at 175 degrees C for 2-3 days and produces lipid compounds ranging from C2 to > C35 which consist of n-alkanols, n-alkanoic acids, n-alkenes, n-alkanes and alkanones The precursor carbon sources used are either formic acid or oxalic acid, which disproportionate to H2, CO2 and probably CO Both carbon sources yield the same lipid classes with essentially the same ranges of compounds The synthesis reactions were confirmed by using 13C labeled precursor acids

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Topics: Hydrothermal circulation (54%), Formic acid (54%), Organic synthesis (53%) ... read more

353 Citations


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