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亚铁碧玉介导的硝酸盐和乙醛酸合成甘氨酸:前生物胺合成的综合途径。

Glycine synthesis from nitrate and glyoxylate mediated by ferroan brucite: An integrated pathway for prebiotic amine synthesis.

机构信息

Department of Geological Sciences, University of Colorado, Boulder, CO 80309.

Department of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125.

出版信息

Proc Natl Acad Sci U S A. 2024 Nov 5;121(45):e2408248121. doi: 10.1073/pnas.2408248121. Epub 2024 Oct 28.

Abstract

Amino acids are present in all known life, so identifying the environmental conditions under which they can be synthesized constrains where life on Earth might have formed and where life might be found on other planetary bodies. All known abiotic amino acid syntheses require ammonia, which is only produced in reducing and neutral atmospheres. Here, we demonstrate that the Fe-bearing hydroxide mineral ferroan brucite [Fe,Mg(OH)] can mediate the reaction of nitrate and glyoxylate to form glycine, the simplest amino acid used in life. Up to 97% of this glycine was detected only after acid digestion of the mineral, demonstrating that it had been strongly partitioned to the mineral. The dicarboxylic amino acid 3-hydroxy aspartate was also detected, which suggests that reactants underwent a mechanism that simultaneously produced mono- and dicarboxylic amino acids. Nitrate can be produced in both neutral and oxidizing atmospheres, so reductive amination of nitrate and glyoxylate on a ferroan brucite surface expands origins of life scenarios. First, it expands the environmental conditions in which life's precursors could form to include oxidizing atmospheres. Second, it demonstrates the ability of ferroan brucite, an abundant, secondary mineral in serpentinizing systems where olivine is partly hydrated, to mediate reductive amination. Finally, the results demonstrate the need to consider mineral-bound products when analyzing samples for abiotic amino acid synthesis.

摘要

氨基酸存在于所有已知的生命中,因此确定它们可以在哪些环境条件下合成,就限制了地球上生命形成的地点,以及在其他行星体上可能发现生命的地点。所有已知的非生物氨基酸合成都需要氨,而氨只能在还原和中性大气中产生。在这里,我们证明含铁的氢氧化物矿物铁镁水羟镁矿 [Fe,Mg(OH)] 可以介导硝酸盐和乙醛酸的反应,形成生命中使用的最简单的氨基酸甘氨酸。只有在矿物经过酸消解后,才能检测到高达 97%的这种甘氨酸,这表明它已强烈分配到矿物中。还检测到二羧酸氨基酸 3-羟基天冬氨酸,这表明反应物经历了一种同时产生单羧酸和二羧酸氨基酸的机制。硝酸盐可以在中性和氧化气氛中产生,因此,在铁镁水羟镁矿表面上进行硝酸盐和乙醛酸的还原氨化扩展了生命起源的情景。首先,它扩大了生命前体形成的环境条件,包括氧化气氛。其次,它证明了富铁水羟镁矿的能力,富铁水羟镁矿是蛇纹石化系统中橄榄石部分水合时的一种丰富的次生矿物,可以介导还原氨化。最后,这些结果表明,在分析非生物氨基酸合成的样本时,需要考虑矿物结合产物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/de25/11551427/d02773aaa7f7/pnas.2408248121sch01.jpg

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