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Plausibility of the Formose Reaction in Alkaline Hydrothermal Vent Environments. 在碱性水热喷口环境中甲酸反应的合理性。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2023-06-01 Epub Date: 2020-09-15 DOI: 10.1007/s11084-020-09599-5
Arthur Omran

Prebiotic processes required a reliable source of free energy and complex chemical mixtures that may have included sugars. The formose reaction is a potential source of those sugars. At moderate to elevated temperature and pH ranges, these sugars rapidly decay. Here it is shown that CaCO3-based chemical gardens catalyze the formose reaction to produce glucose, ribose, and other monosaccharides. These thin inorganic membranes are explored as analogs of hydrothermal vent materials-a possible place for the origin of life-and similarly exposed to very steep pH gradients. Supported by simulations of a simple reaction-diffusion model, this study shows that such gradients allow for the dynamic accumulation of sugars in specific layers of the thin membrane, effectively protecting formose sugar yields. Therefore, the formose reaction may be a plausible prebiotic reaction in alkaline hydrothermal vent environments, possibly setting the stage for an RNA world.

益生元过程需要可靠的自由能来源和可能包括糖的复杂化学混合物。甲糖反应是这些糖的潜在来源。在中等到升高的温度和pH范围内,这些糖会迅速腐烂。研究表明,基于CaCO3的化学花园催化甲糖反应产生葡萄糖、核糖和其他单糖。这些薄无机膜被探索为水热喷口材料的类似物——一个可能的生命起源地,同样暴露在非常陡峭的pH梯度中。在简单反应-扩散模型模拟的支持下,这项研究表明,这种梯度允许糖在薄膜的特定层中动态积累,有效地保护了甲糖的产量。因此,在碱性水热喷口环境中,甲糖反应可能是一种看似合理的益生元反应,可能为RNA世界奠定了基础。
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引用次数: 7
The Possible Role of Anoxic Alkaline High Subcritical Water in the Formation of Ferric Minerals, Methane and Disordered Graphitic Carbon in a BARB3 Drilled Sample of the 3.4 Ga Buck Reef Chert. 缺氧碱性高亚临界水在3.4 Ga Buck Reef Chert BARB3钻孔样品中铁矿物、甲烷和无序石墨碳形成中的可能作用。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2023-06-01 Epub Date: 2023-08-16 DOI: 10.1007/s11084-023-09638-x
Marie-Paule Bassez

The present article reports Raman spectroscopic observations of siderite, hematite, disordered graphitic carbon and possibly greenalite inside the quartz matrix of a banded iron sample from the BARB3 core drilled inside the 3.4 Ga Buck Reef Chert of the Barberton Greenstone Belt in South Africa. The article also reports Raman spectroscopic observations of quartz cavities, concluding in the presence of water, methane and sodium hydroxide at high concentration leading to pH ~ 15 inside the inclusion, suggesting an Archean water which was strongly basic. FeIII-greenalite may also be present inside the inclusion. The possible role of anoxic alkaline high subcritical water in the formation of ferric minerals and the CO required for the synthesis of molecules of biological interest has been demonstrated theoretically since 2013 and summarized in the concept of Geobiotropy. The present article experimentally confirms the importance of considering water in its anoxic strongly alkaline high subcritical domain for the formation of quartz, hematite, FeIII-greenalite, methane and disordered graphitic carbon. Methane is proposed to form locally when the carbon dioxide that is dissolved in the Archean anoxic alkaline high subcritical water, interacts with the molecular hydrogen that is emitted during the anoxic alkaline oxidation of ferrous silicates. The carbon matter is proposed to form as deposition from the anoxic methane-rich fluid. A detailed study of carbon matter from diverse origins is presented in a supplementary file. The study shows that the BARB3_23B sample has been submitted to ~ 335 °C, a temperature of the high subcritical domain, and that the graphitic structure contains very low amounts of oxygen and no hydroxyl functional groups. The importance of considering the structure of water is applied to the constructions of the Neoproterozoic and Archean banded iron formations. It is proposed that their minerals are produced inside chemical reaction chambers containing ferrous silicates, and ejected from the Earth's oceanic crust or upper mantle, during processes involving subduction events or not.

本文报道了在南非Barberton Greenstone Belt的3.4 Ga Buck Reef Chert钻探的BARB3岩芯中,对带状铁样品的石英基质中的菱铁矿、赤铁矿、无序石墨碳以及可能的绿钠石进行的拉曼光谱观察。这篇文章还报道了石英腔的拉曼光谱观察结果,得出的结论是,存在高浓度的水、甲烷和氢氧化钠,导致pH值 ~ 包体内部有15个,表明为强烈碱性的太古宙水。FeIII绿钠石也可能存在于夹杂物内部。自2013年以来,缺氧碱性高亚临界水在合成具有生物学意义的分子所需的铁矿物和CO的形成中可能发挥的作用已在理论上得到证明,并在地生物性的概念中进行了总结。本文通过实验证实了在缺氧强碱性高亚临界区域考虑水对石英、赤铁矿、FeIII绿钠石、甲烷和无序石墨碳形成的重要性。当溶解在太古代缺氧碱性高亚临界水中的二氧化碳与硅酸亚铁缺氧碱性氧化过程中释放的分子氢相互作用时,甲烷被认为是局部形成的。碳物质被认为是由缺氧的富含甲烷的流体沉积而成。补充文件中介绍了对不同来源碳物质的详细研究。研究表明,BARB3_23B样品已提交 ~ 335°C,一个高亚临界域的温度,并且石墨结构包含非常少量的氧并且没有羟基官能团。考虑水结构的重要性适用于新元古代和太古代带状铁构造的建造。有人提出,它们的矿物是在含有硅酸亚铁的化学反应室内产生的,并在涉及俯冲事件或不涉及俯冲事件的过程中从地球的海洋地壳或上地幔喷出。
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引用次数: 0
Behaviour and the Origin of Organisms. 生物体的行为和起源。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2023-06-01 Epub Date: 2023-05-11 DOI: 10.1007/s11084-023-09635-0
Matthew Egbert, Martin M Hanczyc, Inman Harvey, Nathaniel Virgo, Emily C Parke, Tom Froese, Hiroki Sayama, Alexandra S Penn, Stuart Bartlett

It is common in origins of life research to view the first stages of life as the passive result of particular environmental conditions. This paper considers the alternative possibility: that the antecedents of life were already actively regulating their environment to maintain the conditions necessary for their own persistence. In support of this proposal, we describe 'viability-based behaviour': a way that simple entities can adaptively regulate their environment in response to their health, and in so doing, increase the likelihood of their survival. Drawing on empirical investigations of simple self-preserving abiological systems, we argue that these viability-based behaviours are simple enough to precede neo-Darwinian evolution. We also explain how their operation can reduce the demanding requirements that mainstream theories place upon the environment(s) in which life emerged.

在生命起源研究中,通常将生命的最初阶段视为特定环境条件的被动结果。本文考虑了另一种可能性:生命的前身已经在积极地调节他们的环境,以维持他们自己坚持下去所必需的条件。为了支持这一提议,我们描述了“基于生存能力的行为”:一种简单实体可以根据其健康状况自适应地调节其环境的方式,并以此增加其生存的可能性。根据对简单的自我保护非生物系统的实证研究,我们认为这些基于生存能力的行为足够简单,可以先于新达尔文主义进化。我们还解释了它们的运作如何降低主流理论对生命产生的环境的苛刻要求。
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引用次数: 1
Glycine to Oligoglycine via Sequential Trimetaphosphate Activation Steps in Drying Environments. 在干燥环境中通过三甲基磷酸酯顺序活化步骤合成甘氨酸到低甘氨酸。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-12-01 DOI: 10.1007/s11084-022-09634-7
Hayley Boigenzahn, John Yin

Polyphosphate-mediated peptide bond formation is central to protein synthesis in modern organisms, but a simpler form of activation likely preceded the emergence of proteins and RNA. One suggested scenario involves trimetaphosphate (TP), an inorganic phosphate that promotes peptide condensation. Peptide bond formation can also be promoted by high pH and drying, but the interaction of these factors with TP has yet to be characterized kinetically. We studied the formation of glycine oligomers formed under initially alkaline conditions in the presence of TP during the process of drying. Oligopeptide products sampled over 24 h were analyzed by functionalization and high-performance liquid chromatography with ultraviolet absorption (UV-HPLC). As they dried, two different pH-dependent mechanisms dominated during different stages of the process. The first mechanism occurs in alkaline solutions and activates monomer amino acids to form dimers while reducing the pH. Our results then become consistent with a second mechanism that proceeds at neutral pH and consumes dimers to form longer products. The possibility that a series of reactions might occur where the first reaction changes the environment to favor the second, and so on, may have broader implications for prebiotic polymerization. Studying how the environment changes during time-varying conditions, like drying, could help us understand how organic polymers formed during the origin of life.

在现代生物体中,多磷酸盐介导的肽键形成是蛋白质合成的核心,但在蛋白质和RNA出现之前,可能有一种更简单的激活形式。一种建议的方案涉及三甲基磷酸酯(TP),一种促进肽缩聚的无机磷酸盐。高pH和干燥也可以促进肽键的形成,但这些因素与TP的相互作用尚未得到动力学表征。我们研究了在干燥过程中TP存在的初始碱性条件下形成的甘氨酸低聚物的形成。采用功能化和紫外吸收高效液相色谱法(UV-HPLC)对24 h后的寡肽产物进行分析。当它们干燥时,两种不同的ph依赖机制在过程的不同阶段占主导地位。第一种机制发生在碱性溶液中,激活单体氨基酸形成二聚体,同时降低pH值。我们的结果与第二种机制一致,在中性pH下进行,消耗二聚体形成更长的产物。一系列反应可能发生,其中第一个反应改变环境以有利于第二个反应,以此类推,这可能对益生元聚合有更广泛的影响。研究环境在时间变化条件下的变化,比如干燥,可以帮助我们了解有机聚合物是如何在生命起源时形成的。
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引用次数: 4
Thymine Adsorption onto Cation Exchanged Montmorillonite Clay: Role of Biogenic Divalent Metal Cations in Prebiotic Processes of Chemical Evolution. 阳离子交换蒙脱土对胸腺嘧啶的吸附:生物源二价金属阳离子在益生元化学演化过程中的作用。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-12-01 DOI: 10.1007/s11084-022-09633-8
Satish Chandra Sati, Chandra Kala Pant, Preeti Bhatt, Yogesh Pandey

The adsorption of thymine, a key pyrimidine base of deoxyribonucleic acid (DNA) on montmorillonite clay (Mnt) exchanged with metal ions (Mnt-M2+, M2+  = Fe2+, Co2+, Cu2+, Ca2+, and Mg2+) over a range of concentration (7.0 × 10-5 M to 12.0 × 10-5 M) and pH (4.0 - 9.0) at ambient temperature has been investigated in aqueous environment spectrophotometrically (UV, FTIR, XRD, SEM-EDX). The effectiveness of various adsorbents was determined in terms of percent (%) binding and Langmuir constants (KL and Xm) using Langmuir adsorption isotherm at their respective pH of maximum adsorption. Transition metal ions incorporated Mnt, particularly Fe2+ have shown better adsorption ability than alkaline earth metal ions. The present study reveals the significant role of divalent metal cation exchanged Mnt clay in the chemical evolution of biomolecules of genetic continuity and self-replication which might have occurred through the adsorption of thymine on and between their silicate layers to protect and achieve biocompatibility.

采用紫外、FTIR、XRD、SEM-EDX等分光光度法研究了脱氧核酸(DNA)的关键嘧啶基胸腺嘧啶在常温下与金属离子(Mnt-M2+、M2+ = Fe2+、Co2+、Cu2+、Ca2+、Mg2+)交换蒙脱土(Mnt)在7.0 × 10-5 M ~ 12.0 × 10-5 M、pH(4.0 ~ 9.0)范围内的吸附行为。利用Langmuir吸附等温线,在各自的最大吸附pH值下,用结合率(%)和Langmuir常数(KL和Xm)来确定不同吸附剂的有效性。与碱土金属离子相比,掺入Mnt的过渡金属离子表现出更好的吸附能力,尤其是Fe2+。本研究揭示了二价金属阳离子交换Mnt粘土在生物分子遗传连续性和自我复制的化学演化过程中的重要作用,这些生物分子可能是通过胸腺嘧啶在其硅酸盐层上和层间的吸附来保护和实现生物相容性的。
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引用次数: 0
Mathematical Models of Chiral Symmetry-breaking - A Review of General Theories, and Adiabatic Approximations of the APED System. 手性对称性破缺的数学模型——对ped系统的一般理论和绝热近似的回顾。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-12-01 DOI: 10.1007/s11084-022-09631-w
Priscila C Diniz, Jonathan A D Wattis, Fernando P da Costa

We review the literature surrounding chiral symmetry-breaking in chemical systems, with a focus on understanding the mathematical models underlying these chemical processes. We comment in particular on the toy model of Sandars, Viedma's crystal grinding systems and the APED model. We include a few new results based on asymptotic analysis of the APED system.

我们回顾了有关化学系统中手性对称性破缺的文献,重点是理解这些化学过程背后的数学模型。我们特别评论了Sandars的玩具模型,Viedma的晶体研磨系统和ape模型。我们包括了一些新的基于渐近分析的结果。
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引用次数: 0
Evolutionary Approach to Biological Homochirality. 生物同手性的进化方法。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-12-01 DOI: 10.1007/s11084-022-09632-9
Konstantin K Konstantinov, Alisa F Konstantinova

We study a very simple linear evolutionary model based on distribution of protocells by total enantiomeric excess and without any mutual inhibition and show that such model can produce two species with values of total enantiomeric excess in each of the species approaching [Formula: see text] when there is a global [Formula: see text] symmetry. We then consider a scenario when there is a small external global asymmetry factor, like weak interaction, and show that only one of the species remains in such a case, and that is the one, which is more efficient in replication. We perform an estimate of the time necessary to reach homochirality in such a model and show that reasonable assumptions lead to an estimate of around 300 thousand years plus or minus a couple of orders of magnitude. Despite this seemingly large time to reach homochirality, the model is immune to racemization because amino acids in the model follow the lifespan of the protocells rather than the time needed to reach homochirality. We show that not needing mutual inhibition in such evolutionary model is due to the difference in the topology of the spaces in which considered model and many known models of biological homochirality operate. Bifurcation-based models operate in disconnected zero-dimensional space (the space is just two points with enantiomeric excess equal [Formula: see text] and [Formula: see text]), whereas considered evolutionary model (in its continuous representation) operates in one-dimensional connected space, that is the whole interval between [Formula: see text] and [Formula: see text] of total enantiomeric excess. We then proceed with the analysis of the replication process in non-homochiral environment and show that replication errors (the probability to attach an amino acid of wrong chirality) result in a smooth decrease of replication time when total enantiomeric excess of the replicated structure moves away from zero. We show that this decrease in replication time is sufficient for considered model to work.

我们研究了一个非常简单的线性进化模型,该模型基于原始细胞的总对映体过量分布,没有任何相互抑制,并表明当存在全局对称性时,这种模型可以产生两个物种,每个物种的总对映体过量值接近[公式:见文本]。然后,我们考虑一种情况,当存在一个小的外部全局不对称因素,如弱相互作用,并表明只有一个物种在这种情况下仍然存在,这是一个更有效的复制。我们对在这样一个模型中达到同手性所需的时间进行了估计,并表明合理的假设导致大约30万年正负两个数量级的估计。尽管达到同手性似乎需要很长的时间,但该模型不受外消旋作用的影响,因为模型中的氨基酸遵循原细胞的寿命,而不是达到同手性所需的时间。我们表明,在这种进化模型中不需要相互抑制是由于所考虑的模型和许多已知的生物同手性模型所处空间的拓扑结构不同。基于分岔的模型在不相连的零维空间中运行(空间只是两个点,对映体过量等于[公式:见文]和[公式:见文]),而考虑的进化模型(在其连续表示中)在一维连通空间中运行,即总对映体过量[公式:见文]和[公式:见文]之间的整个间隔。然后,我们继续分析非同手性环境下的复制过程,并表明当复制结构的总对映体过量远离零时,复制错误(附着错误手性氨基酸的概率)会导致复制时间的平稳减少。我们表明,复制时间的减少足以使所考虑的模型工作。
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引用次数: 0
Evaluating Mineral Lattices as Evolutionary Proxies for Metalloprotein Evolution. 评价矿物晶格作为金属蛋白进化的进化代理。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-12-01 DOI: 10.1007/s11084-022-09630-x
Kenneth N McGuinness, Gunnar W Klau, Shaunna M Morrison, Elisha K Moore, Jan Seipp, Paul G Falkowski, Vikas Nanda

Protein coordinated iron-sulfur clusters drive electron flow within metabolic pathways for organisms throughout the tree of life. It is not known how iron-sulfur clusters were first incorporated into proteins. Structural analogies to iron-sulfide minerals present on early Earth, suggest a connection in the evolution of both proteins and minerals. The availability of large protein and mineral crystallographic structure data sets, provides an opportunity to explore co-evolution of proteins and minerals on a large-scale using informatics approaches. However, quantitative comparisons are confounded by the infinite, repeating nature of the mineral lattice, in contrast to metal clusters in proteins, which are finite in size. We address this problem using the Niggli reduction to transform a mineral lattice to a finite, unique structure that when translated reproduces the crystal lattice. Protein and reduced mineral structures were represented as quotient graphs with the edges and nodes corresponding to bonds and atoms, respectively. We developed a graph theory-based method to calculate the maximum common connected edge subgraph (MCCES) between mineral and protein quotient graphs. MCCES can accommodate differences in structural volumes and easily allows additional chemical criteria to be considered when calculating similarity. To account for graph size differences, we use the Tversky similarity index. Using consistent criteria, we found little similarity between putative ancient iron-sulfur protein clusters and iron-sulfur mineral lattices, suggesting these metal sites are not as evolutionarily connected as once thought. We discuss possible evolutionary implications of these findings in addition to suggesting an alternative proxy, mineral surfaces, for better understanding the coevolution of the geosphere and biosphere.

蛋白质协调的铁硫簇驱动整个生命之树的生物体代谢途径中的电子流。目前尚不清楚铁硫团簇最初是如何结合到蛋白质中的。与早期地球上存在的硫化铁矿物的结构相似,表明蛋白质和矿物质的进化之间存在联系。大量蛋白质和矿物晶体结构数据集的可用性,为利用信息学方法大规模探索蛋白质和矿物的共同进化提供了机会。然而,与蛋白质中的金属团簇大小有限相比,矿物晶格的无限重复性质使定量比较变得混乱。我们使用Niggli还原来解决这个问题,将矿物晶格转换为有限的,独特的结构,当翻译时再现晶格。蛋白质和还原矿物结构用商图表示,边和节点分别对应键和原子。提出了一种基于图论的矿物商图与蛋白质商图之间最大共连通边子图(MCCES)的计算方法。MCCES可以适应结构体积的差异,并且在计算相似性时很容易考虑额外的化学标准。为了解释图形大小的差异,我们使用Tversky相似指数。使用一致的标准,我们发现在假定的古代铁硫蛋白簇和铁硫矿物晶格之间几乎没有相似性,这表明这些金属位点并不像以前认为的那样在进化上相互联系。为了更好地理解地圈和生物圈的共同进化,我们讨论了这些发现可能的进化意义,并提出了另一种替代方法——矿物表面。
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引用次数: 1
Biological Homochirality and the Search for Extraterrestrial Biosignatures. 生物同手性和寻找地外生物特征。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-09-01 Epub Date: 2022-08-15 DOI: 10.1007/s11084-022-09623-w
Marcelo Gleiser

Most amino acids and sugar molecules occur in mirror, or chiral, images of each other, knowns as enantiomers. However, life on Earth is mostly homochiral: proteins contain almost exclusively L-amino acids, while only D-sugars appear in RNA and DNA. The mechanism behind this fundamental asymmetry of life remains unknown, despite much progress in the theoretical and experimental understanding of homochirality in the past decades. We review three potential mechanisms for the emergence of biological homochirality on primal Earth and explore their implications for astrobiology: the first, that biological homochirality is a stochastic process driven by local environmental fluctuations; the second, that it is driven by circularly-polarized ultraviolet radiation in star-forming regions; and the third, that it is driven by parity violation at the elementary particle level. We argue that each of these mechanisms leads to different observational consequences for the existence of enantiomeric excesses in our solar system and in exoplanets, pointing to the possibility that the search for life elsewhere will help elucidate the origins of homochirality on Earth.

大多数氨基酸和糖分子互为镜像或手性映像,称为对映体。然而,地球上的生命大多是单手性的:蛋白质几乎只含有l -氨基酸,而RNA和DNA中只含有d -糖。尽管在过去的几十年里,对同手性的理论和实验理解取得了很大的进展,但这种基本的生命不对称性背后的机制仍然未知。我们回顾了原始地球上生物同手性出现的三种可能机制,并探讨了它们对天体生物学的影响:第一,生物同手性是一个由局部环境波动驱动的随机过程;第二,它是由恒星形成区域的圆偏振紫外线辐射驱动的;第三,它是由基本粒子层面的宇称破坏驱动的。我们认为,这些机制中的每一种都导致了太阳系和系外行星中对映体过量存在的不同观测结果,指出了在其他地方寻找生命将有助于阐明地球上同手性起源的可能性。
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引用次数: 1
Symmetry Breaking by Consecutive Amplification: Efficient Paths to Homochirality. 连续放大的对称性破缺:实现同手性的有效途径。
IF 2 4区 物理与天体物理 Q2 Agricultural and Biological Sciences Pub Date : 2022-09-01 DOI: 10.1007/s11084-022-09627-6
Laura Huber, Oliver Trapp

To understand chiral symmetry breaking on the molecular level, we developed a method to efficiently investigate reaction kinetics of single molecules. The model systems include autocatalysis as well as a reaction cascade to gain further insight into the prebiotic origin of homochirality. The simulated reactions start with a substrate and only a single catalyst molecule, and the occurrence of symmetry breaking was examined for its degree of dependence on randomness. The results demonstrate that interlocking processes, which e.g., form catalysts, autocatalytic systems, or reaction cascades that build on each other and lead to a kinetic acceleration, can very well amplify a statistically occurring symmetry breaking. These results suggest a promising direction for the experimental implementation and identification of such processes, which could have led to a shift out of thermodynamic equilibrium in the emergence of life.

为了在分子水平上理解手性对称性破缺,我们开发了一种有效研究单分子反应动力学的方法。模型系统包括自催化以及反应级联,以进一步了解同手性的益生元起源。模拟的反应从一个底物和一个催化剂分子开始,并检查了对称破缺的发生对随机性的依赖程度。结果表明,联锁过程,例如形成催化剂、自催化系统或相互建立并导致动力学加速的反应级联,可以很好地放大统计上发生的对称破缺。这些结果为实验实施和识别这些过程提供了一个有希望的方向,这些过程可能导致生命出现时热力学平衡的转变。
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引用次数: 3
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