Chemical origin of life articles within Nature Chemistry

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  • Article
    | Open Access

    Enzyme-initiated polymerization-induced self-assembly has been used to generate various biomimetic structures. Now, myoglobin’s activity is used for biocatalytic polymerization-induced self-assembly to generate vesicular artificial cells. As various cargoes can be encapsulated during polymerization, these artificial cells are capable of protein expression and can act as microreactors for distinct enzymatic reactions.

    • Andrea Belluati
    • , Sètuhn Jimaja
    •  & Nico Bruns

  • Article |

    The onset of eco-evolutionary dynamics marks a stepping stone in the transition from chemistry to biology. Now a minimal replicator system showing such dynamics has been developed. The replicators adapt to changes in their environment that they themselves induced through photoredox catalysis.

    • Kai Liu
    • , Alex Blokhuis
    •  & Sijbren Otto

  • Article |

    The coupling of autocatalysis to compartment growth and division is a key step in the origin of life. Now it has been shown that compartmentalizing the formose reaction in emulsion droplets leads to several crucial properties of living and evolving systems (growth, division, variation, competition, rudimentary heredity and selection).

    • Heng Lu
    • , Alex Blokhuis
    •  & Andrew D. Griffiths

  • Article
    | Open Access

    The streamlined synthesis of multiple (proto)biomolecules from common starting materials is a key goal of prebiotic chemistry. Now, a one-pot synthesis of ribo-aminooxazoline (a precursor for prebiotic nucleotide synthesis) from HCN has been achieved. Additionally, the two moieties used in extant terpenoid biosynthesis have been accessed, with all carbon atoms also originating from HCN.

    • Dougal J. Ritson
    •  & John D. Sutherland

  • Article |

    The apparent disconnect between prebiotic aldehyde-based Strecker synthesis of amino acids and the α-ketoacid-based metabolism of extant biochemistry necessitates an evolutionary switch between these disparate chemistries. Now it has been shown that Bucherer–Bergs reactions of α-ketoacids produce α-amino acids and dihydroorotate, paralleling the biochemical synthesis of orotate and suggesting a more congruent evolutionary pathway from cyanide-based chemistries.

    • Sunil Pulletikurti
    • , Mahipal Yadav
    •  & Ramanarayanan Krishnamurthy

  • News & Views |

    Amino-containing four-carbon threose nucleic acids (TNAs) have long been considered to be prebiotically irrelevant due to their difficult formation. Now, a prebiotically plausible route to 3′-amino-TNA nucleoside triphosphate has been developed, raising the possibility of 3′-amino-TNA as a non-canonical nucleic acid during the origin of life.

    • Yingyu Liu
    •  & Yajun Wang

  • Article |

    Nucleotides are essential to the origins of life, and their synthesis is a key challenge for prebiotic chemistry. Contrary to prior expectation, non-canonical 3′-amino-TNA nucleosides are shown to be synthesized diastereoselectively and regiospecifically under prebiotically plausible conditions. The enhanced reactivity of 3′-amino-TNAs also promotes their selective non-enzymatic triphosphorylation in water.

    • Daniel Whitaker
    •  & Matthew W. Powner

  • News & Views |

    Explaining the controlled emergence and growth of molecular complexity at life’s origins is one of prebiotic chemistry’s grand challenges. Now, it has been shown that we can observe how the self-organization of a complex carbohydrate network can be modulated by its environment.

    • Quentin Dherbassy
    •  & Kamila B. Muchowska

  • Article |

    The process by which life arose using information from the prebiotic environment and inherent molecular reactivity is unclear. Now, it has been shown that systems of chemical reactions exhibit well-defined self-organization in varying environments, providing a potential mechanism for chemical evolution processes that bridge the gap between prebiotic building blocks and life’s origin.

    • William E. Robinson
    • , Elena Daines
    •  & Wilhelm T. S. Huck

  • Article |

    Oscillations are widespread throughout the natural world and a number of fascinating inorganic oscillating reactions are known—but the formation and control of oscillating, self-replicating synthetic systems has remained challenging. Now, it has been shown that chemically fuelled oscillations within a network of organic replicators can drive supramolecular assembly and disassembly.

    • Michael G. Howlett
    • , Anthonius H. J. Engwerda
    •  & Stephen P. Fletcher

  • News & Views |

    The emergence of protometabolic reactions that evolved into today’s metabolic pathways is unclear. Now, evidence suggests that the chemical origin of biological carbon metabolism may have relied on the versatility of a single primitive C1 feedstock molecule — hydrogen cyanide.

    • Saidul Islam

  • Article |

    It’s unclear how protometabolic reactions emerged and evolved into extant metabolic pathways such as the tricarboxylic acid cycle. Now, it has been shown that cyanide acts as a mild and efficient reducing agent, mediating abiotic transformations of tricarboxylic acid intermediates and derivatives.

    • Mahipal Yadav
    • , Sunil Pulletikurti
    •  & Ramanarayanan Krishnamurthy

  • News & Views |

    Membraneless coacervate droplets have been widely investigated as potential candidates for early cells or protocells. Now, they are shown to grow, divide and differentiate into two populations in a rock pore model that mimics an early Earth environment.

    • Hadi M. Fares

  • Article |

    Threose nucleic acid (TNA) is a potential RNA evolutionary progenitor and a nuclease-resistant synthetic genetic polymer. Now, a TNA catalyst that cleaves RNA has been identified in vitro. The TNA catalyst shows strong sequence selectivity towards a mutant RNA substrate involved in drug resistance, resulting in selective gene silencing in eukaryotic cells.

    • Yueyao Wang
    • , Yao Wang
    •  & Hanyang Yu

  • Article
    | Open Access

    Complex coacervate microdroplets have been proposed as primordial cells, but their ability to evolve by fusion, growth and fission has not yet been demonstrated. Now, it has been shown that gas bubbles inside heated rock pores can drive the growth, fusion, division and selection of coacervate microdroplets.

    • Alan Ianeselli
    • , Damla Tetiker
    •  & T.-Y. Dora Tang

  • News & Views |

    Phase separation offers a fundamental mechanism for organization and compartmentalization. Now, peptide-based synthons have been shown to form catalytically active coacervates providing a stepping stone for creating synthetic primitive cells.

    • Samrat Mukhopadhyay

  • Article |

    Carbon dioxide is a substantial component of many planetary atmospheres, but reduction of carbon dioxide requires conditions and substrates that are rare on planetary surfaces. Now, the reduction of carbon dioxide to organic species with biological relevance has been photochemically coupled to the oxidation of sulfite, suggesting that prebiotic carbon fixation could take place on the surfaces of rocky planets.

    • Ziwei Liu
    • , Long-Fei Wu
    •  & John D. Sutherland

  • Article |

    Liquid–liquid phase separation plays an important role in creating cellular compartments and protocells, but designing small-molecule models remains difficult. A peptide-based synthon for liquid–liquid phase separation consisting of two stickers and a flexible, polar spacer has now been presented. Condensates formed by these synthons can concentrate biomolecules and catalyse anabolic reactions.

    • Manzar Abbas
    • , Wojciech P. Lipiński
    •  & Evan Spruijt

  • News & Views |

    The origin and evolution of translational machinery — which produces a specific peptide from an RNA sequence — is a major unsolved puzzle in prebiotic chemistry. Now, the coupling of amino acids directed by RNA templates in the absence of a ribosome provides clues on how this protein synthesis process might have started.

    • Ya Ying Zheng
    •  & Jia Sheng

  • Article |

    Elucidating the origin of translation—the process that produces a specific peptide from an RNA sequence—is one of the most difficult challenges in prebiotic chemistry and evolutionary biology. Now, it has been shown that aminoacylated nucleotides couple to amino-acid-bearing oligoribonucleotides, directed by an RNA template, forming specific di- and tripeptides in the absence of ribosomal machinery.

    • Biswarup Jash
    • , Peter Tremmel
    •  & Clemens Richert

  • Article |

    Droplet interface bilayer measurements have now shown that membranes formed from chiral phospholipid bilayers are enantioselectively permeable to chiral amino acids. The results show that membrane stereochemistry is necessary and sufficient to drive such enantioselective transport, presenting a new potential route to homochirality. These findings could also have implications for pharmacokinetics and drug design.

    • Juan Hu
    • , Wesley G. Cochrane
    •  & Brian M. Paegel

  • Article |

    Mirror-symmetry breaking in chiral systems by a chiral solvent has remained poorly understood for decades. Now, the supramolecular polymerization of triphenylene derivatives has shown that—through the additive effects of polymerization—the cumulative entropic effects of the interactions between chiral solvents and solutes create measurable differences in free enthalpy.

    • Marcin L. Ślęczkowski
    • , Mathijs F. J. Mabesoone
    •  & E. W. Meijer

  • Editorial |

    It is far from certain how simple chemical reactions became interconnected networks that gave rise to life on early Earth. Exploring the possible ways in which this could have occurred is an active area of research and a collection of articles in this issue consider what chemical steps may have been taken on the path towards life as we know it today.

  • News & Views |

    It’s generally assumed that primitive forms of cellular life arose from nucleic acids and peptides compartmentalized within vesicles — all underpinned by a non-enzymatic protometabolism. Three studies now provide new insights into the ancient chemistry that may have supported early biology.

    • Albert C. Fahrenbach
    •  & Quoc Phuong Tran

  • Article |

    Life requires a constant supply of energy, but the energy sources that drove the transition from prebiotic chemistry to biochemistry on the early Earth are unknown. Now, a potentially prebiotic chemical activating reagent has been shown to enable the synthesis, in aqueous conditions and catalysed by small molecules, of peptides, peptidyl–RNAs, RNA oligomers and primordial phospholipids.

    • Ziwei Liu
    • , Long-Fei Wu
    •  & John D. Sutherland

  • Article |

    It is unclear how phospholipid membranes formed on the early Earth, as modern cells synthesize the phospholipid constituents of their membranes enzymatically. Now, a combination of ion pairing and self-assembly has enabled transacylation of lysophospholipids with acyl donors in water, affording a variety of membrane-forming natural diacylphospholipids in high yields.

    • Luping Liu
    • , Yike Zou
    •  & Neal K. Devaraj

  • Article |

    Metal-catalysed prebiotic reactions have been proposed as forerunners of modern metabolism. Now, an abiotic pathway resembling the reverse tricarboxylic acid cycle has been shown to proceed without metal catalysis. The reaction of glyoxylate and pyruvate produces a series of α-ketoacid tricarboxylic acid analogues, and provides a route to generate α-amino acids by transamination.

    • R. Trent Stubbs
    • , Mahipal Yadav
    •  & Greg Springsteen

  • News & Views |

    It’s not known how life’s essential properties of replication, metabolism and compartmentalization were first integrated. Two recent articles now shed light on how metabolic characteristics may be incorporated into replicating systems, harnessing an external energy source to increase their rate of replication and acquiring catalytic activity.

    • Pablo Solís-Muñana
    •  & Jack L. Y. Chen

  • Article |

    Asymmetric autocatalysis—such as that observed experimentally in the Soai reaction—may have been responsible for the origin of biological homochirality. The magnitude of the energy imbalance required to induce directed symmetry breaking and asymmetric amplification in the Soai reaction has now been identified and compared to the parity violation energy difference.

    • Neil A. Hawbaker
    •  & Donna G. Blackmond

  • Article |

    The emergence of pristine RNA and DNA on the early Earth would have been hindered by a lack of specificity in their prebiotic syntheses. Now, it has been shown that chimeric sequences—with a mixture of RNA and DNA backbones—mediate the template-directed ligation of oligomers present in mixtures of nucleic acids, enabling the simultaneous appearance of RNA and DNA.

    • Subhendu Bhowmik
    •  & Ramanarayanan Krishnamurthy

  • News & Views |

    Proteins are biosynthesized from α-amino acids using hefty biological machinery, but the origin of this process on the early Earth is unclear. Now, a bottom-up approach for forming peptides, taking place under mild, prebiotically-plausible conditions, has been developed. This strategy uses α-aminonitrile precursors, bypassing α-amino acids entirely.

    • Robert Pascal
    •  & Irene A. Chen

  • Article |

    High concentrations of prebiotic molecules and dry–wet cycles are difficult to achieve in a submerged system. Now, it has been shown that temperature gradients across gas bubbles in submerged rock pores can provide these conditions. Molecules are continuously accumulated at the warm side of bubbles at the gas–water interface, which enables or enhances many prebiotically relevant processes.

    • Matthias Morasch
    • , Jonathan Liu
    •  & Dieter Braun

  • News & Views |

    The chemical functionality necessary for the origin of life may have emerged from simple reactions assembled into complex networks. Now, it has been shown that prebiotically relevant heterogeneous reaction networks can generate robust oscillations within complex mixtures comprised of precursors that do not oscillate on their own.

    • Nathaniel Wagner
    •  & Gonen Ashkenasy

  • Article |

    RNA is usually considered to be the first genetic polymer, with DNA a product of a biochemical pathway that arose after the origin of life. Now, studies into the prebiotic phosphorylation of an RNA nucleoside reveal pathways for the synthesis of DNA building blocks, providing experimental support for a prebiotic link between RNA and DNA.

    • Jianfeng Xu
    • , Nicholas J. Green
    •  & John D. Sutherland

  • Article |

    The simplest sugar—glycolaldehyde—has recently been detected in space and now a mechanistic rationale for its formation is presented, which includes its onward reaction to the next higher aldose, glyceraldehyde. The key species in the chemistry at play is the formaldehyde isomer hydroxymethylene, which reacts with the carbonyl component in an essentially barrierless carbonyl–ene-type reaction.

    • André K. Eckhardt
    • , Michael M. Linden
    •  & Peter R. Schreiner

  • Thesis |

    Bruce C. Gibb takes us on a journey through the physical and chemical evolution of planet Earth and suggests that the reverse Hofmeister effect, the phenomenon whereby poorly solvated ions associate in water, could be a powerful driving force towards the first hint of life on the rock we call home.

    • Bruce C. Gibb

  • Article |

    Phosphorylation of (pre)biological molecules in water has been a long-sought goal in prebiotic chemistry. Now, it has been demonstrated that diamidophosphate phosphorylates nucleosides, amino acids and glycerol/fatty acids in aqueous medium, while simultaneously leading to higher-order structures such as oligonucleotides, peptides and liposomes in the same reaction mixture.

    • Clémentine Gibard
    • , Subhendu Bhowmik
    •  & Ramanarayanan Krishnamurthy

  • Article |

    Current mineral-based theories do not fully address how enzymes emerged from prebiotic catalysts. Now, iron–sulfur clusters can be synthesized by UV-light-mediated photolysis of organic thiols and photooxidation of ferrous ions. Iron–sulfur peptides may have formed easily on early Earth, facilitating the emergence of iron–sulfur-cluster-dependent metabolism.

    • Claudia Bonfio
    • , Luca Valer
    •  & Sheref S. Mansy

  • Editorial |

    There are many unanswered questions regarding how the biomolecules and biomechanical processes that define life came to be. A collection of Articles in this issue show how intermediates in RNA synthesis might have formed and how the initiation and evolution of RNA replication might have occurred.

  • Article |

    Lysine-rich peptides from the ribosomal core and derived homolysine decapeptides of either L-, D- or mixed chirality have now been shown to enhance RNA polymerase ribozyme activity at low magnesium concentrations, accelerate ribozyme evolution and enable templated RNA synthesis within membranous protocells.

    • Shunsuke Tagami
    • , James Attwater
    •  & Philipp Holliger

  • Article |

    Di- and tripeptide building blocks in which the C-terminus has been converted into an aldehyde are shown to form dynamic chemical networks through imine condensation followed by the formation of cyclic N,N-acetals. The networks exhibit multi-phase growth of prion-like assemblies that template the formation of chain-length-specific peptide-like oligomers.

    • Chenrui Chen
    • , Junjun Tan
    •  & David G. Lynn

  • Article |

    Simple peptides are shown to assemble into well-defined amyloid phases with paracrystalline surfaces that can catalyse reactions in an enantioselective manner. Modifying individual amino acids in the building blocks enables the structure of the assembled aggregates, and the reactions that they can catalyse, to be controlled predictably.

    • Tolulope O. Omosun
    • , Ming-Chien Hsieh
    •  & David G. Lynn

  • Article |

    2-aminothiazole — a hybrid of prebiotic amino acid and nucleotide precursors — sequentially accumulates and purifies glycolaldehyde and glyceraldehyde from complex mixtures in the order required for ribonucleotide synthesis, dynamically resolves glyceraldehyde from its ketose-isomer dihydroxyacetone, and provides the first strategy to select natural amino acids from abiotic aldehydes and ketones.

    • Saidul Islam
    • , Dejan-Krešimir Bučar
    •  & Matthew W. Powner

  • Article |

    Although ribose aminooxazoline has been shown to be a potential intermediate in prebiotic pyrimidine ribonucleotide synthesis, a route by which this could occur has remained elusive. Now, a remarkably efficient photoanomerization reaction has been investigated by theory and experiment. The new route affords enantiomerically pure ribonucleotides when the starting material is enantioenriched.

    • Jianfeng Xu
    • , Maria Tsanakopoulou
    •  & John D. Sutherland

  • Article |

    Genetic circuits are important for synthetic biology, biochemistry and bioengineering. Now, the encapsulation of genetic circuits into liposomes has been shown to enable a more modular design, the selective isolation of reactions from the environment and from each other, and the hierarchical assembly of reaction products.

    • Katarzyna P. Adamala
    • , Daniel A. Martin-Alarcon
    •  & Edward S. Boyden

  • Article |

    Chemical reconstitution of the triose glycolysis pathway is controlled by α-phosphorylation and provides a generational link between prebiotic ribonucleotide synthesis, triose glycolysis and serine metabolism. Now, research suggests that unification of nucleotide synthesis and triose metabolism may have been a fundamentally important step towards the origins of life.

    • Adam J. Coggins
    •  & Matthew W. Powner

  • Article |

    An unanswered question in the RNA world scenario is how sequence information could be transferred during replication of duplex RNA. Without the aid of sophisticated enzymes, strand reannealing occurs more quickly than template-directed synthesis. Now, a plausible prebiotic solution to this problem is presented, in which a viscous solvent enables information transfer from a gene-length double-stranded template.

    • Christine He
    • , Isaac Gállego
    •  & Nicholas V. Hud

  • Article |

    Identifying a non-enzymatic method of replicating RNA for multiple cycles has been problematic because rapid strand reannealing outcompetes slow non-enzymatic template copying. Now, oligoarginine peptides have been shown to inhibit reannealing while still allowing short primers and activated monomers to bind to the template strand, facilitating the next round of template copying.

    • Tony Z. Jia
    • , Albert C. Fahrenbach
    •  & Jack W. Szostak

  • Article |

    During the early stages of life on Earth sophisticated RNA catalysts must have formed from simple precursors. Here it is shown that freeze–thaw cycles can drive the assembly of complex RNA polymerase ribozymes from networks of short RNA oligonucleotides through an unanticipated RNA chaperone effect.

    • Hannes Mutschler
    • , Aniela Wochner
    •  & Philipp Holliger

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