Life | Special Issue : Origin of Life in Chemically Complex Messy Environments: 2nd Edition

Research

17 pages, 8483 KiB

Open AccessArticle

Groundwater-Driven Evolution of Prebiotic Alkaline Lake Environments

by Benjamin M. Tutolo, Robert Perrin, Rachel Lauer, Shane Bossaer, Nicholas J. Tosca, Alec Hutchings, Serhat Sevgen, Michael Nightingale, Daniel Ilg, Eric B. Mott and Thomas Wilson

Life 2024, 14(12), 1624; https://doi.org/10.3390/life14121624 - 7 Dec 2024

Viewed by 1011

Abstract

Alkaline lakes are thought to have facilitated prebiotic synthesis reactions on the early Earth because their modern analogs accumulate vital chemical feedstocks such as phosphate through the evaporation of dilute groundwaters. Yet, the conditions required for some building block synthesis reactions are distinct [...] Read more.

Alkaline lakes are thought to have facilitated prebiotic synthesis reactions on the early Earth because their modern analogs accumulate vital chemical feedstocks such as phosphate through the evaporation of dilute groundwaters. Yet, the conditions required for some building block synthesis reactions are distinct from others, and these conditions are generally incompatible with those permissible for nascent cellular function. However, because current scenarios for prebiotic synthesis have not taken account of the physical processes that drive the chemical evolution of alkaline lakes, the potential for the co-occurrence of both prebiotic synthesis and the origins and early evolution of life in prebiotic alkaline lake environments remains poorly constrained. Here, we investigate the dynamics of active, prebiotically relevant alkaline lakes using near-surface geophysics, aqueous geochemistry, and hydrogeologic modeling. Due to their small size, representative range of chemistry, and contrasting evaporation behavior, the investigated, neighboring Last Chance and Goodenough Lakes in British Columbia, Canada offer a uniquely tractable environment for investigating the dynamics of alkaline lake behavior. The results show that the required, extreme phosphate enrichments in alkaline lake waters demand geomorphologically-driven vulnerability to evaporation, while the resultant contrast between evaporated brines and inflowing groundwaters yields Rayleigh–Taylor instabilities and vigorous surface–subsurface cycling and mixing of lake and groundwaters. These results provide a quantitative basis to reconcile conflicting prebiotic requirements of UV light, salinity, metal concentration, and pH in alkaline lake environments. The complex physical and chemical processing inherent to prebiotic alkaline lake environments thus may have not only facilitated prebiotic reaction networks, but also provided habitable environments for the earliest evolution of life. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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15 pages, 3940 KiB

Open AccessArticle

Light-Assisted Formation of Nucleosides and Nucleotides from Formamide in the Presence of Cerium Phosphate

by Shoval Gilboa, Larisa Panz, Nitai Arbell and Yaron Paz

Life 2024, 14(7), 846; https://doi.org/10.3390/life14070846 - 5 Jul 2024

Viewed by 982

Abstract

The abiotic formation of nucleotides from small, simple molecules is of large interest in the context of elucidating the origin of life scenario. In what follows, it is shown that nucleosides and nucleotides can be formed from formamide in a one-pot reaction utilizing [...] Read more.

The abiotic formation of nucleotides from small, simple molecules is of large interest in the context of elucidating the origin of life scenario. In what follows, it is shown that nucleosides and nucleotides can be formed from formamide in a one-pot reaction utilizing the mineral cerium phosphate (CePO₄) as a photocatalyst, a catalyst and a reactant that supplies the necessary phosphate groups. While the most abundant RNA/DNA building blocks were thymidine and thymidine monophosphate, considerable yields of other building blocks such as cytidine, cytidine monophosphate, and adenosine cyclic monophosphate were found. Comparing the yield of nucleosides and nucleotides under light conditions to that in the dark suggests that in the presence of cerium phosphate, light promotes the formation of nucleobases, whereas the formation of nucleotides from nucleosides take place even in the absence of light. The scenario described herein is considerably simpler than other scenarios involving several steps and several reactants. Therefore, by virtue of the principle of Occam’s razor, it should be of large interest for the community. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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14 pages, 4788 KiB

Open AccessArticle

From Zero to Hero: The Cyanide-Free Formation of Amino Acids and Amides from Acetylene, Ammonia and Carbon Monoxide in Aqueous Environments in a Simulated Hadean Scenario

by Christian Seitz, Thomas Geisberger, Alexander Richard West, Jessica Fertl, Wolfgang Eisenreich and Claudia Huber

Life 2024, 14(6), 719; https://doi.org/10.3390/life14060719 - 1 Jun 2024

Viewed by 1102

Abstract

Amino acids are one of the most important building blocks of life. During the biochemical process of translation, cells sequentially connect amino acids via amide bonds to synthesize proteins, using the genetic information in messenger RNA (mRNA) as a template. From a prebiotic [...] Read more.

Amino acids are one of the most important building blocks of life. During the biochemical process of translation, cells sequentially connect amino acids via amide bonds to synthesize proteins, using the genetic information in messenger RNA (mRNA) as a template. From a prebiotic perspective (i.e., without enzymatic catalysis), joining amino acids to peptides via amide bonds is difficult due to the highly endergonic nature of the condensation reaction. We show here that amides can be formed in reactions catalyzed by the transition metal sulfides from acetylene, carbon monoxide and ammonia under aqueous conditions. Some α- and β-amino acids were also formed under the same conditions, demonstrating an alternative cyanide-free path for the formation of amino acids in prebiotic environments. Experiments performed with stable isotope labeled precursors, like ¹⁵NH₄Cl and ¹³C-acetylene, enabled the accurate mass spectroscopic identification of the products formed from the starting materials and their composition. Reactions catalyzed using the transition metal sulfides seem to offer a promising alternative pathway for the formation of amides and amino acids in prebiotic environments, bypassing the challenges posed by the highly endergonic condensation reaction. These findings shed light on the potential mechanisms by which the building blocks of life could have originated on early Earth. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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19 pages, 1439 KiB

Open AccessArticle

A Surface Hydrothermal Source of Nitriles and Isonitriles

by Paul B. Rimmer and Oliver Shorttle

Life 2024, 14(4), 498; https://doi.org/10.3390/life14040498 - 11 Apr 2024

Cited by 3 | Viewed by 5233

Abstract

Giant impacts can generate transient hydrogen-rich atmospheres, reducing atmospheric carbon. The reduced carbon will form hazes that rain out onto the surface and can become incorporated into the crust. Once heated, a large fraction of the carbon is converted into graphite. The result [...] Read more.

Giant impacts can generate transient hydrogen-rich atmospheres, reducing atmospheric carbon. The reduced carbon will form hazes that rain out onto the surface and can become incorporated into the crust. Once heated, a large fraction of the carbon is converted into graphite. The result is that local regions of the Hadean crust were plausibly saturated with graphite. We explore the consequences of such a crust for a prebiotic surface hydrothermal vent scenario. We model a surface vent fed by nitrogen-rich volcanic gas from high-temperature magmas passing through graphite-saturated crust. We consider this occurring at pressures of 1–

1000 bar

and temperatures of 1500–

1700^{\circ} C

. The equilibrium with graphite purifies the leftover gas, resulting in substantial quantities of nitriles (

0.1 %

HCN and

1 ppm

HC₃N) and isonitriles (

0.01 %

HNC) relevant for prebiotic chemistry. We use these results to predict gas-phase concentrations of methyl isocyanide of ∼1 ppm. Methyl isocyanide can participate in the non-enzymatic activation and ligation of the monomeric building blocks of life, and surface or shallow hydrothermal environments provide its only known equilibrium geochemical source. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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23 pages, 2745 KiB

Open AccessArticle

Prebiotic Syntheses of Organophosphorus Compounds from Reduced Source of Phosphorus in Non-Aqueous Solvents

by Maheen Gull, Tian Feng, Benjamin Smith, Laurent Calcul and Matthew A. Pasek

Life 2023, 13(11), 2134; https://doi.org/10.3390/life13112134 - 29 Oct 2023

Viewed by 1714

Abstract

Reduced-oxidation-state phosphorus (reduced P, hereafter) compounds were likely available on the early Earth via meteorites or through various geologic processes. Due to their reactivity and high solubility, these compounds could have played a significant role in the origin of various organophosphorus compounds of [...] Read more.

Reduced-oxidation-state phosphorus (reduced P, hereafter) compounds were likely available on the early Earth via meteorites or through various geologic processes. Due to their reactivity and high solubility, these compounds could have played a significant role in the origin of various organophosphorus compounds of biochemical significance. In the present work, we study the reactions between reduced P compounds and their oxidation products, with the three nucleosides (uridine, adenosine, and cytidine), with organic alcohols (glycerol and ethanolamine), and with the tertiary ammonium organic compound, choline chloride. These reactions were studied in the non-aqueous solvent formamide and in a semi-aqueous solvent comprised of urea: ammonium formate: water (UAFW, hereafter) at temperatures of 55–68 °C. The inorganic P compounds generated through Fenton chemistry readily dissolve in the non-aqueous and semi-aqueous solvents and react with organics to form organophosphites and organophosphates, including those which are identified as phosphate diesters. This dual approach (1) use of non-aqueous and semi-aqueous solvents and (2) use of a reactive inorganic P source to promote phosphorylation and phosphonylation reactions of organics readily promoted anhydrous chemistry and condensation reactions, without requiring any additive, catalyst, or other promoting agent under mild heating conditions. We also present a comparative study of the release of P from various prebiotically relevant phosphate minerals and phosphite salts (e.g., vivianite, apatite, and phosphites of iron and calcium) into formamide and UAFW. These results have direct implications for the origin of biological P compounds from non-aqueous solvents of prebiotic provenance. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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17 pages, 6790 KiB

Open AccessArticle

RETRACTED: Metal Catalysis Acting on Nitriles in Early Earth Hydrothermal Systems

by Miranda Sturtz and Christopher House

Life 2023, 13(7), 1524; https://doi.org/10.3390/life13071524 - 7 Jul 2023

Cited by 1 | Viewed by 1924 | Retraction

Abstract

Hydrothermal systems are areas in which heated fluids and organic molecules rush through basaltic material rich in metals and minerals. By studying malononitrile and acetonitrile, we examine the effects of metal and mineral nanoparticles on nitrile compounds in anoxic, hydrothermal conditions representing a [...] Read more.

Hydrothermal systems are areas in which heated fluids and organic molecules rush through basaltic material rich in metals and minerals. By studying malononitrile and acetonitrile, we examine the effects of metal and mineral nanoparticles on nitrile compounds in anoxic, hydrothermal conditions representing a prebiotic environment of early Earth. Polymerization, reduction, cyclization, and a phenomenon colloquially known as ‘chemical gardening’ (structure building via reprecipitation of metal compounds or complexing with organics) are all potential outcomes with the addition of metals and minerals. Reduction occurs with the addition of rhodium (Rh) or iron (II) sulfide (FeS), with positive identification of ethanol and ethylamine forming from acetonitrile reduction. We find that polymerization and insoluble product formation were associated with oxide minerals, metallic nickel (Ni), and metallic cobalt (Co) acting as catalysts. Oxide minerals strongly promoted polymerization into insoluble, tar-like products of nitriles. FeS, iron-nickel alloy (FeNi), and rhodium are unique cases that appear to act as reagents by actively participating in chemical gardening without returning to their initial state. Further, FeS tentatively had a phase change into the mineral parabutlerite. This research aims to identify metals and metal minerals that could best serve nitrile catalysis and reactions on early Earth. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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13 pages, 4968 KiB

Open AccessArticle

Serpentinization-Associated Mineral Catalysis of the Protometabolic Formose System

by Arthur Omran, Asbell Gonzalez, Cesar Menor-Salvan, Michael Gaylor, Jing Wang, Jerzy Leszczynski and Tian Feng

Life 2023, 13(6), 1297; https://doi.org/10.3390/life13061297 - 31 May 2023

Cited by 3 | Viewed by 2833

Abstract

The formose reaction is a plausible prebiotic chemistry, famed for its production of sugars. In this work, we demonstrate that the Cannizzaro process is the dominant process in the formose reaction under many different conditions, thus necessitating a catalyst for the formose reaction [...] Read more.

The formose reaction is a plausible prebiotic chemistry, famed for its production of sugars. In this work, we demonstrate that the Cannizzaro process is the dominant process in the formose reaction under many different conditions, thus necessitating a catalyst for the formose reaction under various environmental circumstances. The investigated formose reactions produce primarily organic acids associated with metabolism, a protometabolic system, and yield very little sugar left over. This is due to many of the acids forming from the degradation and Cannizaro reactions of many of the sugars produced during the formose reaction. We also show the heterogeneous Lewis-acid-based catalysis of the formose reaction by mineral systems associated with serpentinization. The minerals that showed catalytic activity include olivine, serpentinite, and calcium, and magnesium minerals including dolomite, calcite, and our Ca/Mg-chemical gardens. In addition, computational studies were performed for the first step of the formose reaction to investigate the reaction of formaldehyde, to either form methanol and formic acid under a Cannizzaro reaction or to react to form glycolaldehyde. Here, we postulate that serpentinization is therefore the startup process necessary to kick off a simple proto metabolic system—the formose protometabolic system. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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16 pages, 8397 KiB

Open AccessArticle

Straightforward Creation of Possibly Prebiotic Complex Mixtures of Thiol-Rich Peptides

by Ibrahim Shalayel, Naoual Leqraa, Véronique Blandin and Yannick Vallée

Life 2023, 13(4), 983; https://doi.org/10.3390/life13040983 - 10 Apr 2023

Cited by 2 | Viewed by 1874

Abstract

At the origin of life, extremely diverse mixtures of oligomers and polymers could be obtained from relatively simple molecular bricks. Here, we present an example of the polymerization of two amidonitriles derived from cysteine, Cys-Ala-CN and Cys-Met-CN. The thiol function in a molecule [...] Read more.

At the origin of life, extremely diverse mixtures of oligomers and polymers could be obtained from relatively simple molecular bricks. Here, we present an example of the polymerization of two amidonitriles derived from cysteine, Cys-Ala-CN and Cys-Met-CN. The thiol function in a molecule adds onto the nitrile group of another one, allowing efficient condensation reactions and making available an extensive range of polymers containing amide bonds and/or five-membered heterocycles, namely thiazolines. Macrocycles were also identified, the biggest one containing sixteen residues (cyclo(Cys-Met)₈). MALDI-TOF mass spectrometry was used to identify all the present species. What these examples show is that complex mixtures are likely to have formed on the primitive Earth and that, ultimately, the selection that must have followed may have been an even more crucial step towards life than the synthesis of the pre-biological species themselves. Full article

(This article belongs to the Special Issue Origin of Life in Chemically Complex Messy Environments: 2nd Edition)

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