Influence of Composition of Nickel‐Iron Nanoparticles for Abiotic CO<sub>2</sub> Conversion to Early Prebiotic Organics

Beyazay, Tuğçe; Ochoa‐Hernández, Cristina; Song, Youngdong; Belthle, Kendra Solveig; Martin, William; Tüysüz, Harun

doi:10.1002/ange.202218189

Cited by 5 publications

(3 citation statements)

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“…A protometabolic hypothesis for the origins of life has gained traction in recent years. Prebiotic reactions analogous to core, autotrophic metabolic pathways have now been shown to take place under aqueous conditions, albeit with low efficiency [ 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 , 29 ]. Examples of such pathways include the acetyl-coA pathway, reactions of the Krebs cycle and parts of the pentose phosphate pathway.…”

Section: Introductionmentioning

confidence: 99%

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Harrison

Webb

Rammu

et al. 2023

Life

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A protometabolic approach to the origins of life assumes that the conserved biochemistry of metabolism has direct continuity with prebiotic chemistry. One of the most important amino acids in modern biology is aspartic acid, serving as a nodal metabolite for the synthesis of many other essential biomolecules. Aspartate’s prebiotic synthesis is complicated by the instability of its precursor, oxaloacetate. In this paper, we show that the use of the biologically relevant cofactor pyridoxamine, supported by metal ion catalysis, is sufficiently fast to offset oxaloacetate’s degradation. Cu2+-catalysed transamination of oxaloacetate by pyridoxamine achieves around a 5% yield within 1 h, and can operate across a broad range of pH, temperature, and pressure. In addition, the synthesis of the downstream product β-alanine may also take place in the same reaction system at very low yields, directly mimicking an archaeal synthesis route. Amino group transfer supported by pyridoxal is shown to take place from aspartate to alanine, but the reverse reaction (alanine to aspartate) shows a poor yield. Overall, our results show that the nodal metabolite aspartate and related amino acids can indeed be synthesised via protometabolic pathways that foreshadow modern metabolism in the presence of the simple cofactor pyridoxamine and metal ions.

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Section: Introductionmentioning

confidence: 99%

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Harrison

Webb

Rammu

et al. 2023

Life

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“…To have a further understanding, CO 2 -temperature programmed desorption (CO 2 -TPD) and H 2 -temperature programmed reduction (H 2 -TPR) analyses were performed for zeolite-NaY and SBA-15-supported catalysts, viz., Pd/PdO–Fe 2 O 3 -Y and Pd–Fe 2 O 3 -SBA-15 (Figure S8). From the CO 2 -TPD analysis, a change in the nature of basic sites in the catalysts Pd/PdO–Fe 2 O 3 -Y and Pd–Fe 2 O 3 -SBA-15 was distinguishable. ,– Zeolite-NaY usually shows desorption of CO 2 at temperatures below 300 °C for weak and medium basic sites . In case of Pd/PdO–Fe 2 O 3 -Y catalyst, CO 2 desorption occurred at 464, 491, and 567 °C, indicating moderate to strong interaction of the CO 2 with the basic sites (Figure S8a).…”

Section: Catalytic Studymentioning

confidence: 95%

Low-Palladium-Content Iron(III) Nanocatalyst Supported on Zeolite-NaY for C–Cl Bond Activation

Bora,

Hazarika,

Gour

et al. 2023

ACS Appl. Nano Mater.

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A heterogeneous nanocatalyst comprising palladium (Pd/PdO) and iron(III) oxide (Fe 2 O 3 ) in the dimension of 1−4 nm was synthesized using sodium-exchanged zeolite-Y or zeolite-NaY [a type of faujasite (FAU) zeolite having an aluminosilicate framework with a general formula of (Na 2 ) 3.5 [Al 7 Si 17 O 48 ]•32H 2 O] as a support matrix. The catalyst was investigated as a true heterogeneous catalyst for activation of the robust C−Cl bond of aryl chlorides in the Suzuki−Miyaura cross-coupling (SMCC) reaction. The catalyst with very low Pd loading (0.0037 mol %) exhibited high reactivity in the SMCC reaction with various derivatives of aryl chlorides (Ar−Cl). Biaryl products were obtained with up to a 92% yield, high selectivity, and a good turnover number with this Pd/PdO−Fe 2 O 3 -Y catalyst. The catalyst exhibited good thermal stability and was highly recyclable. The reaction was found to be reliant on various parameters such as solvent system, temperature, time, and catalyst amount. A small aliquot of water (H 2 O) mixed with methanol (CH 3 OH) dramatically brought a substantial improvement in the product yield of the desired biaryl product. The role of zeolite-NaY was also investigated by comparing the results with various other synthesized catalysts. Different experimental studies indicated that the surface hydroxyl (−OH) groups of zeolite-NaY, modification of basic sites, and the ability to influence the reduction temperature of iron (Fe) and palladium (Pd) influenced the catalytic performance of the synthesized catalyst. The impact of Fe on the electronic structure and reactivity of Pd was analyzed through a density functional theory calculation. This study provided strong evidence for creation of a negative (−ve) charge on Pd with an increasing amount of Fe content and thereby favored the in situ transformation of Pd(II) to Pd(0) as required in the activation of the C−Cl bond.

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“…Serpentinization provided the electron donor (H 2 ) and energy to fix CO 2 in the early vent systems [38]. Vent reactions were promoted by inorganic catalysts, likely including greigite (Fe 3 S 4 ), magnetite (Fe 3 O 4 ), and awaruite (Ni 3 Fe), as well as heteroatoms incorporating Co, Mg, Al, Ca, Ti, and Zr, in the vent flux and microchamber walls [98][99][100]. Fougèrite (Green Rust) may also have played a role as a microchamber catalytic site [101].…”

Section: Initial Rafsmentioning

confidence: 99%

Opinion: The Key Steps in the Origin of Life to the Formation of the Eukaryotic Cell

Brunk,

Marshall

2024

Life

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The path from life’s origin to the emergence of the eukaryotic cell was long and complex, and as such it is rarely treated in one publication. Here, we offer a sketch of this path, recognizing that there are points of disagreement and that many transitions are still shrouded in mystery. We assume life developed within microchambers of an alkaline hydrothermal vent system. Initial simple reactions were built into more sophisticated reflexively autocatalytic food-generated networks (RAFs), laying the foundation for life’s anastomosing metabolism, and eventually for the origin of RNA, which functioned as a genetic repository and as a catalyst (ribozymes). Eventually, protein synthesis developed, leading to life’s biology becoming dominated by enzymes and not ribozymes. Subsequent enzymatic innovation included ATP synthase, which generates ATP, fueled by the proton gradient between the alkaline vent flux and the acidic sea. This gradient was later internalized via the evolution of the electron transport chain, a preadaptation for the subsequent emergence of the vent creatures from their microchamber cradles. Differences between bacteria and archaea suggests cellularization evolved at least twice. Later, the bacterial development of oxidative phosphorylation and the archaeal development of proteins to stabilize its DNA laid the foundation for the merger that led to the formation of eukaryotic cells.

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Influence of Composition of Nickel‐Iron Nanoparticles for Abiotic CO₂ Conversion to Early Prebiotic Organics

Cited by 5 publications

References 74 publications

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Low-Palladium-Content Iron(III) Nanocatalyst Supported on Zeolite-NaY for C–Cl Bond Activation

Opinion: The Key Steps in the Origin of Life to the Formation of the Eukaryotic Cell

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Influence of Composition of Nickel‐Iron Nanoparticles for Abiotic CO2 Conversion to Early Prebiotic Organics

Cited by 5 publications

References 74 publications

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Prebiotic Synthesis of Aspartate Using Life’s Metabolism as a Guide

Low-Palladium-Content Iron(III) Nanocatalyst Supported on Zeolite-NaY for C–Cl Bond Activation

Opinion: The Key Steps in the Origin of Life to the Formation of the Eukaryotic Cell

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Influence of Composition of Nickel‐Iron Nanoparticles for Abiotic CO₂ Conversion to Early Prebiotic Organics