A.M. Butlerov Chemistry Institute, Kazan Federal University, Kremlevskaya St., 18, Kazan, Russian Federation, 420008.
Sarov Physical Technical Institute, National Research Nuclear University "MEPhI" (Moscow Engineering Physics Institute), Dukhov St., 6, Sarov, Russian Federation, 607184.
Orig Life Evol Biosph. 2019 Jun;49(1-2):1-18. doi: 10.1007/s11084-019-09575-8. Epub 2019 Apr 19.
Syntheses under shock in nitrogen bubbled samples of the water - formamide - bicarbonate - sodium hydroxide system at pH 8.63, 9.46 and 10.44 were performed in the stainless steel preservation capsules. The maximum temperature and pressure in the capsules reached 545 K and 12.5 GPa respectively. Using the LC-MS-MS analysis, the 21 synthesis products have been identified, including amines and polyamines, carboxamide, acetamide and urea derivatives, compounds containing aniline, pyrrolidine, pyrrole, imidazole, as well as alcohol groups. It was found that the Fischer-Tropsch-type syntheses with catalysis on the surface of the stainless steel of the conservation capsule associated with the adsorbed hydrogen cyanide reactions and transamidation processes play the main role in the shock syntheses. Formation reactions of all the above-mentioned compounds have been suggested. It was proposed that hydrogen cyanide, ammonia, isocyanic acid, aminonitrile, aminoacetonitrile, as well as adsorbed species H, CH, CH, CHOH, NH and HCNH are especially important for the formation of the products. A reduction reaction of adsorbed bicarbonate with hydrogen to formaldehyde has been first postulated. In the studied system also classical reactions take place - Wöhler's synthesis of urea and Butlerov's synthesis of methenamine. It was suggest that material of meteorites may be an effective catalyst in the Fischer-Tropsch-type syntheses at falling of the iron-nickel meteorites in the water - formamide regions on the early Earth. It was concluded that life could have originated due to the impact of meteorites on alkaline water-formamide lakes located near volcanoes on the early Earth.
在 pH 值为 8.63、9.46 和 10.44 的氮气鼓泡水-甲酰胺-碳酸氢盐-氢氧化钠体系的不锈钢保存胶囊中进行了冲击波下的合成。胶囊内的最高温度和压力分别达到 545 K 和 12.5 GPa。使用 LC-MS-MS 分析,鉴定了 21 种合成产物,包括胺和多胺、甲酰胺、乙酰胺和尿素衍生物、含苯胺、吡咯烷、吡咯、咪唑的化合物以及醇类。研究发现,与吸附的氰化氢反应和转酰胺化过程相关的不锈钢表面上的费歇尔-托普希型催化作用在冲击波合成中起着主要作用。提出了所有上述化合物的形成反应。提出氰化氢、氨、异氰酸、氨基腈、氨基乙腈以及吸附的 H、CH、CH、CHOH、NH 和 HCNH 对产物的形成特别重要。首次提出了吸附的碳酸氢盐与氢还原生成甲醛的反应。在研究的体系中还发生了经典的反应——尿素的沃勒合成和甲缩醛的巴特勒洛夫合成。提出铁镍陨石在早期地球上落入水-甲酰胺区域时,陨石可能是费歇尔-托普希型合成的有效催化剂。研究结论表明,生命可能起源于早期地球上靠近火山的碱性水-甲酰胺湖中陨石的撞击。