Photochemical formation of organic compounds from mixtures of simple gases

Groth, W.; Weyssenhoff, Hanns von

doi:10.1016/0032-0633(60)90001-5

Cited by 52 publications

(28 citation statements)

References 18 publications

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“…The first, and arguably most important, of these demonstrations was the familiar Miller-Urey synthesis of numerous organic compounds from CH4, NH3, H2, and H20 with the energy coming from a spark discharge (Miller, 1953(Miller, , 1955Abelson, 1956Abelson, , 1957Miller and Urey, 1959;Ring et al, 1972;. Other investigators have shown that heat Fox, 1964, 1965;Fox and Windsor, 1970;Hayatsu et al, 1971;Wolman et al, 1971;Lawless and Boynton, 1973;Yanagawa et al, 1981), ultraviolet radiation (Groth and Van Weyssenhoff, 1960;Sagan and Khare, 1971;Bar-Nun and Hartman, 1978;Reiche and Bard, 1979), shock waves (Bar-Nun et al, 1970, 1971, and other forms of energy (Palm and Calvin, 1962;Gilvary and Hochstim, 1963;Scattergood et al 1989) can be used to overcome the kinetic barriers to the formation of metastable states from reduced starting mixtures. Perhaps owing to the success of these experiments, it is commonly thought that reduced starting materials are required for abiotic synthesis on the early Earth.…”

Section: Introductionmentioning

confidence: 91%

Geochemical constraints on the origin of organic compounds in hydrothermal systems

Shock

1990

Origins Life Evol Biosphere

275

183

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Abstract. It is proposed that abiotic synthesis of organic compounds occurs in metastable states. These states are permitted by kinetic barriers which inhibit the approach to stable equilibrium in the C-H-O-N system. Evidence for metastable equilibrium among organic compounds in sedimentary basins is reviewed, and further evidence is elucidated from hydrous pyrolysis experiments reported in the literature. This analysis shows that at hydrothermal conditions, organic compounds are formed or destroyed primarily through oxidation/reduction reactions, and that the role of temperature is to lower the kinetic barriers to these reactions. These lines of evidence allow the development of a scenario in which abiotic synthesis can occur at hydrothermal conditions through the reduction of CO2 and N2. This scenario can be tested quantitatively with distribution of species calculations as functions of temperature, pressure, hydrogen fugacity (JH~) and initial composition. One example of such a test is given for an early, sudden outgassing of the Earth, in which CO2, H20, and N2 are transported from the mantle to the atmosphere by hydrothermal solutions. Activities of metastabte aqueous organic species which form as a consequence of this process are evaluated at conditions appropriate for seafloor hydrothermat systems, and are found to maximize at about 200 °C and between the oxidation states set by two mineral assemblages common in the oceanic crust.

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Section: Introductionmentioning

confidence: 91%

Geochemical constraints on the origin of organic compounds in hydrothermal systems

Shock

1990

Origins Life Evol Biosphere

275

183

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“…Most of the photochemical reactions would occur in the upper atmosphere, and the products formed would, for the most part absorb at longer wavelengths, and so be decomposed before they reached the protection of the oceans. The yield of amino acids from the photolysis of CH4, NH3 and H20 at wavelengths of 1470 and 1294 A is quite low (Groth andWeyssenhoff, 1957, 1960), probably due to the low yields of hydrogen cyanide. The synthesis of amino acids by the photolysis of CH4, C2H6, NH3, H20 and H2S mixtures by UV light of wavelengths greater than 2000/~ (Sagan and Khare, 1971;Khare and Sagan, 1971) is also a low yield synthesis, but the amount of energy is much greater in this region of the sun's spectrum.…”

Section: Energy Sourcesmentioning

confidence: 98%

Origin of organic compounds on the primitive earth and in meteorites

1976

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The role and relative contributions of different forms of energy to the synthesis of amino acids and other organic compounds on the primitive earth, in the parent bodies or carbonaceous chondrites, and in the solar nebula are examined. A single source of energy or a single process would not account for all the organic compounds synthesized in the solar system. Electric discharges appear to produce amino acids more efficiently than other sources of energy and the composition of the synthesized amino acids is qualitatively similar to those found in the Murchison meteorite. Ultraviolet light is also likely to have played a major role in prebiotic synthesis. Although the energy in the sun's spectrum that can be absorbed by the major constituents of the primitive atmosphere is not large, reactive trace components such as H2S and formaldehyde absorb at longer wavelengths where greater amounts of energy are available and produce amino acids by reactions involving hot hydrogen atoms. The thermal reaction of CO + H2 + NH3 on Fischer-Tropsch catalysts generates intermediates that lead to amino acids and other organic compounds that have been found in meteorites. However, this synthesis appears to be less efficient than electric discharges and to require a special set of reaction conditions. It should be emphasized that after the reactive organic intermediates are generated by the above processes, the subsequent reactions which produce the more complete biochemical compounds are low temperature homogenous reactions occurring in an aqueous environment.

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“…We have established that (1) adenine is indeed a product of electron irradiation of a mixture of methane, ammonia, and water, (2) there is an inverse relationship between the amount of adenine synthesis and the amount of hydrogen gas present, and (3) of the five nucleic acid bases, adenine is the one most readily synthesized under prebiotic conditions. Materials and Methods.-Mixtures of methane-C'4, ammonium hydroxide (4 N), and, in some experiments, hydrogen were irradiated with electrons in the glass apparatus (volume approx.…”

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confidence: 97%

Formation of Adenine by Electron Irradiation of Methane, Ammonia, and Water

Ponnamperuma

Lemmon²,

Mariner³

et al. 1963

Proc. Natl. Acad. Sci. U.S.A.

103

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Several reports have described the effect of different forms of energy on gaseous mixtures of methane, ammonia, hydrogen, and water-the kind of mixture that probably comprised the atmosphere of the prebiotic earth.'-3 While the formation of amino acids in such experiments has been clearly demonstrated, there is little evidence for the formation of the heterocyclic bases which are major constituents of the nucleic acids. Apart from Or6's synthesis of adenine by the action of heat on a concentrated solution of ammonium cyanide4 and Fox's synthesis of uracil by a thermal reaction between malic acid and urea,5 there appears to be no report in the literature of the formation of a purine or pyrimidine under simulated prebiotic earth conditions. Palm and Calvin suggested that adenine was a probable product of the electron irradiation of a mixture of methane, ammonia, hydrogen, and water.' They had preliminary but not conclusive evidence for the formation of adenine.The primary object of the present investigation was to examine the possibility of the synthesis of heterocyclic bases from mixtures of primitive gases. We have established that (1) adenine is indeed a product of electron irradiation of a mixture of methane, ammonia, and water, (2) there is an inverse relationship between the amount of adenine synthesis and the amount of hydrogen gas present, and (3) of the five nucleic acid bases, adenine is the one most readily synthesized under prebiotic conditions. Materials and Methods.-Mixtures of methane-C'4, ammonium hydroxide (4 N), and, in some experiments, hydrogen were irradiated with electrons in the glass apparatus (volume approx. 750 ml) shown in Figure 1. The source of ionizing radiation used in these experiments was, simply as a matter of convenience, a linear electron accelerator. Four separate experiments were performed. Twenty ml of 4 N NH40H and two or three boiling chips (SiC) were introduced into the irradiation tube. The flask B was cooled to -78°and the tube evacuated. One-quarter mM of C14H4 (containing 0.5 mc; sources: Tracerlab, Inc. and New England Nuclear Corp.) was introduced, followed by nonlabeled methane (12 mM) until the pressure in the tube was 300 mm. During the methane addition, care was exercised to exclude all air from inlet tubes. In two experiments, no H2 was used. In a third experiment, 50 mm of H2 was added; in a fourth experiment, 100 mm of H2 was introduced into the irradiation tube.During the irradiations the tube was kept in a horizontal position. The electrons entered the tube through the concave end window, which was larger in diameter than the cross section of the electron beam. The electrons had an energy of 4.5 Mev and were delivered in 60 pulses per sec, each pulse lasting 6 gsec. The integrated dose rate was 18 samps, and the time of irradiation was 45 min. The current delivered during this time was 0.0486 coulombs. Cobalt glass dosimetry at the center of a similar irradiation tube indicated that 1.5 X 104 rads were absorbed per microcoulomb. The total energy absorption wa...

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Photochemical formation of organic compounds from mixtures of simple gases

Cited by 52 publications

References 18 publications

Geochemical constraints on the origin of organic compounds in hydrothermal systems

Geochemical constraints on the origin of organic compounds in hydrothermal systems

Origin of organic compounds on the primitive earth and in meteorites

Formation of Adenine by Electron Irradiation of Methane, Ammonia, and Water

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