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1.
We have elaborated an evolutionary turbulent model of the subnebula of Saturn derived from that of Dubrulle (1993, Icarus106, 59-76) for the solar nebula, which is valid for a geometrically thin disk. We demonstrate that if carbon and nitrogen were in the form of CO and N2, respectively, in the early subnebula, these molecules were not subsequently converted into CH4 and NH3 during the evolution of the disk, contrary to the current scenario initially proposed by Prinn and Fegley (1981, Astrophys. J., 249, 308-317). However, if the early subnebula contained some CH4 and NH3, these gases were not subsequently converted into CO and N2. We argue that Titan must have been formed from planetesimals migrating from the outer part of the subnebula to the present orbit of the satellite. These planetesimals were relics of those embedded in the feeding zone of Saturn prior to the completion of the planet and contained hydrates of NH3 and clathrate hydrates of CH4. It is shown that, for plausible abundances of CH4 and NH3 in the solar nebula at 10 AU, the masses of methane and nitrogen trapped in Titan were higher than the estimate of masses of these components in the primitive atmosphere of the satellite. If our scenario is valid and if our turbulent model properly describes the structure and the evolution of the actual subnebula of Saturn, the Xe/C ratio should be six times higher in Titan's atmosphere today than in the Sun, while the current scenario would probably result in a quasi solar Xe/C ratio. The mass spectrometer and gas chromatograph instrument aboard the Huygens Titan probe of the Cassini mission has the capability of measuring this ratio in 2004, thus permitting us to discriminate between the current scenario and the one proposed in this report. 相似文献
2.
We propose a new interpretation of the D/H ratio in CH4 observed in the atmosphere of Titan. Using a turbulent evolutionary model of the subnebula of Saturn (O. Mousis et al. 2002, Icarus156, 162-175), we show that in contrast to the current scenario, the deuterium enrichment with respect to the solar value observed in Titan cannot have occurred in the subnebula. Instead, we argue that values of the D/H ratio measured in Titan were obtained in the cooling solar nebula by isotopic thermal exchange of hydrogen with CH3D originating from interstellar methane D-enriched ices that vaporized in the nebula. The rate of the isotopic exchange decreased with temperature and became fully inhibited around 200 K. Methane was subsequently trapped in crystalline ices around 10 AU in the form of clathrate hydrates formed at 60 K, and incorporated into planetesimals that formed the core of Titan. The nitrogen-methane atmosphere was subsequently outgassed from the decomposition of the hydrates (Mousis et al. 2002). By use of a turbulent evolutionary model of the solar nebula (O. Mousis et al. 2000, Icarus148, 513-525), we have reconstructed the entire story of D/H in CH4, from its high value in the early solar nebula (acquired in the presolar cloud) down to the value measured in Titan's atmosphere today. Considering the two last determinations of the D/H ratio in Titan—D/H=(7.75±2.25)×10−5 obtained from ground-based observations (Orton 1992, In: Symposium on Titan, ESA SP-338, pp. 81-85), and D/H=(8.75+3.25−2.25)×10−5, obtained from ISO observations (Coustenis et al. 2002, submitted for publication)—we inferred an upper limit of the D/H ratio in methane in the early outer solar nebula of about 3×10−4. Our approach is consistent with the scenario advocated by several authors in which the atmospheric methane of Titan is continuously replenished from a reservoir of clathrate hydrates of CH4 at high pressures, located in the interior of Titan. If this scenario is correct, observations of the satellite to be performed by the radar, the imaging system, and other remote sensing instruments aboard the spacecraft of the Cassini-Huygens mission from 2004 to 2008 should reveal local disruptions of the surface and other signatures of the predicted outgassing. 相似文献
3.
It has been suggested that the present release rate of methane to the Martian atmosphere could be the result of serpentinization in the deep subsurface, followed by the conversion of H2 to CH4 in a CO2-rich fluid. Making this assumption, we show that the cryosphere could act as a buffer storing, under the form of micron-size methane clathrate particles, the methane delivered from below by hydrothermal fluids and progressively releasing it to the atmosphere at the top. From an extrapolation of the present CH4 release rate back to the past, we calculate that up to several hundred millibars (～200–2000 mbar) of CO2, resulting from the oxidation of the released CH4, in addition to the volcanic supply (～400 mbar), should have accumulated in the atmosphere in the absence of a CO2 sink. We reassess the capability of escape to have removed CO2 from the atmosphere by C non-thermal escape and show that it is not significant. We suggest that atmospheric carbon is recycled to the crust through an active subsurface hydrological system, and precipitates as carbonates within the crust. During episodic periods of magmatic activity, these carbonates are decomposed to CO2 dissolved in running water, and CO2 can react with H2 formed by serpentinization to build CH4. CH4 is then buffered in the subsurface cryosphere, above the water table, and finally released to the atmosphere, before being recycled to the subsurface hydrological system, and converted back to carbonates. We propose a typical evolution curve of the CO2 pressure since the late Noachian based on our hypothesis. Contrary to the steady state carbon cycle at work on Earth, a progressive damping of the carbon cycle occurs on Mars due to the absence of plate tectonics and the progressive cooling of the planet. 相似文献
4.
We model the subnebulae of Jupiter and Saturn wherein satellite accretion took place. We expect each giant planet subnebula to be composed of an optically thick (given gaseous opacity) inner region inside of the planet’s centrifugal radius (where the specific angular momentum of the collapsing giant planet gaseous envelope achieves centrifugal balance, located at rCJ ∼ 15RJ for Jupiter and rCS ∼ 22RS for Saturn) and an optically thin, extended outer disk out to a fraction of the planet’s Roche-lobe (RH), which we choose to be ∼RH/5 (located at ∼150 RJ near the inner irregular satellites for Jupiter, and ∼200RS near Phoebe for Saturn). This places Titan and Ganymede in the inner disk, Callisto and Iapetus in the outer disk, and Hyperion in the transition region. The inner disk is the leftover of the gas accreted by the protoplanet. The outer disk may result from the nebula gas flowing into the protoplanet during the time of giant planet gap-opening (or cessation of gas accretion). For the sake of specificity, we use a solar composition “minimum mass” model to constrain the gas densities of the inner and outer disks of Jupiter and Saturn (and also Uranus). Our model has Ganymede at a subnebula temperature of ∼250 K and Titan at ∼100 K. The outer disks of Jupiter and Saturn have constant temperatures of 130 and 90 K, respectively.Our model has Callisto forming in a time scale ∼106 years, Iapetus in 106-107 years, Ganymede in 103-104 years, and Titan in 104-105 years. Callisto takes much longer to form than Ganymede because it draws materials from the extended, low density portion of the disk; its accretion time scale is set by the inward drift times of satellitesimals with sizes 300-500 km from distances ∼100RJ. This accretion history may be consistent with a partially differentiated Callisto with a ∼300-km clean ice outer shell overlying a mixed ice and rock-metal interior as suggested by Anderson et al. (2001), which may explain the Ganymede-Callisto dichotomy without resorting to fine-tuning poorly known model parameters. It is also possible that particulate matter coupled to the high specific angular momentum gas flowing through the gap after giant planet gap-opening, capture of heliocentric planetesimals by the extended gas disk, or ablation of planetesimals passing through the disk contributes to the solid content of the disk and lengthens the time scale for Callisto’s formation. Furthermore, this model has Hyperion forming just outside Saturn’s centrifugal radius, captured into resonance by proto-Titan in the presence of a strong gas density gradient as proposed by Lee and Peale (2000). While Titan may have taken significantly longer to form than Ganymede, it still formed fast enough that we would expect it to be fully differentiated. In this sense, it is more like Ganymede than like Callisto (Saturn’s analog of Callisto, we expect, is Iapetus). An alternative starved disk model whose satellite accretion time scale for all the regular satellites is set by the feeding of planetesimals or gas from the planet’s Roche-lobe after gap-opening is likely to imply a long accretion time scale for Titan with small quantities of NH3 present, leading to a partially differentiated (Callisto-like) Titan. The Cassini mission may resolve this issue conclusively. We briefly discuss the retention of elements more volatile than H2O as well as other issues that may help to test our model. 相似文献
5.
We present new experimental results on impact shock chemistry into icy satellites of the outer planets. Icy mixtures of pure water ice with CO2, Na2CO3, CH3OH, and CH3OH/(NH4)2SO4 at 77 K were ablated with a powerful pulsed laser—a new technique used to simulate shock processes which can occur during impacts. New products were identified by GC-MS and FTIR analyses after laser ablation. Our results show that hydrogen peroxide is formed in irradiated H2O/CO2 ices with a final concentration of 0.23%. CO and CH3OH were also detected as main products. The laser ablation of frozen H2O/Na2CO3 generates only CO and CO2 as destruction products from the salt. Pulsed irradiation of water ice containing methanol leads also to the formation of CO and CO2, generates methane and more complex molecules containing carbonyl groups like acetaldehyde, acetone, methyl formate, and a diether, dimethyl formal. The last three compounds are also produced when adding ammonium sulfate to H2O/CH3OH ice, but acetone is more abundant. The formation of two hydrocarbons, CH4 and C2H6 is observed as well as the production of three nitrogen compounds, nitrous oxide, hydrogen cyanide, and acetonitrile. 相似文献
6.
We calculate the D/H ratio of CH4 from serpentinization on Titan to determine whether Titan’s atmospheric CH4 was originally produced inside the giant satellite. This is done by performing equilibrium isotopic fractionation calculations in the CH4-H2O-H2 system, with the assumption that the bulk D/H ratio of the system is equivalent to that of the H2O in the plume of Enceladus. These calculations show that the D/H ratio of hydrothermally produced CH4 would be markedly higher than that of atmospheric CH4 on Titan. The implication is that Titan’s CH4 is a primordial chemical species that was accreted by the moon during its formation. There are two evolutionary scenarios that are consistent with the apparent absence of endogenic CH4 in Titan’s atmosphere. The first is that hydrothermal systems capable of making CH4 never existed on Titan because Titan’s interior has always been too cold. The second is that hydrothermal systems on Titan were sufficiently oxidized so that C existed in them predominately in the form of CO2. The latter scenario naturally predicts the formation of endogenic N2, providing a new hypothesis for the origin of Titan’s atmospheric N2: the hydrothermal oxidation of 15N-enriched NH3. A primordial origin for CH4 and an endogenic origin for N2 are self-consistent, but both hypotheses need to be tested further by acquiring isotopic data, especially the D/H ratio of CH4 in comets, and the 15N/14N ratio of NH3 in comets and that of N2 in one of Enceladus’ plumes. 相似文献
7.
Caroline Thomas Olivier Mousis Sylvain Picaud Vincent Ballenegger 《Planetary and Space Science》2009,57(1):42-47
Recent observations have evidenced traces of methane (CH4) heterogeneously distributed in the martian atmosphere. However, because the lifetime of CH4 in the atmosphere of Mars is estimated to be around 300-600 years on the basis of photochemistry, its release from a subsurface reservoir or an active primary source of methane have been invoked in the recent literature. Among the existing scenarios, it has been proposed that clathrate hydrates located in the near subsurface of Mars could be at the origin of the small quantities of the detected CH4. Here, we accurately determine the composition of these clathrate hydrates, as a function of temperature and gas phase composition, by using a hybrid statistical thermodynamic model based on experimental data. Compared to the other recent works, our model allows us to calculate the composition of clathrate hydrates formed from a more plausible composition of the martian atmosphere by considering its main compounds, i.e. carbon dioxide, nitrogen and argon, together with methane. Besides, because there is no low temperature restriction in our model, we are able to determine the composition of clathrate hydrates formed at temperatures corresponding to the extreme ones measured in the polar caps. Our results show that methane enriched clathrate hydrates could be stable in the subsurface of Mars only if a primitive CH4-rich atmosphere has existed or if a subsurface source of CH4 has been (or is still) present. 相似文献
8.
Régis Courtin 《Icarus》1982,51(3):466-475
The pressure-induced absorptions of gaseous nitrogen (N2) and methane (CH4) are computed on the basis of the collisional lineshape theory of G. Birnhaum and E.R. Cohen [Canad. J. Phys.54, 593–602 (1976)]. Laboratory data at 300 and 124°K for N2 and at 296 and 195°K for CH4 are used to determine the collisional time constant and their temperature dependence. The spectrum of Titan from the microwave to the far-infrared region (0.1–600 cm?1) is then modeled using these opacities and a temperature profile of Titan's atmosphere derived from the Voyager 1 radio occultation experiment. The model atmosphere is composed of N2 and CH4, their relative proportions being determined by the vapor pressure law of CH4. A model with gaseous opacity alone is ruled out by the far-infrared observations. An additional opacity, thought to be associated with a methane cloud, is confirmed. The effective temperature of Titan is estimated at Te = 83.2 ± 1.4°K. 相似文献
9.
Complex organic materials may exist as haze layers in the atmosphere of Titan and as dark coloring agents on icy satellite surfaces. Laboratory measurements of optical constants of plausible complex organic materials are necessary for quantitative evaluation from remote sensing observations, and to document the existence of complex organic materials in the extraterrestrial environments. The recent Cassini VIMS and CIRS observations provide new constraints on Titan’s haze properties in the mid-infrared wavelength region. Here, we present the optical constants (2.5–25 μm) of Titan tholins generated with cold plasma irradiation of a N2/CH4 (90/10) gas mixture at pressures of 0.26 mbar, 1.6 mbar, and 23 mbar. Our new optical constants of three types of Titan tholins suggest that no single Titan tholin in this study fulfills all the observational constraints of the Titan haze material. The discrepancy remains a challenge for future modeling and laboratory efforts that aim toward a better understanding of Titan’s haze material. 相似文献
10.
Ever since their discovery the regular satellites of Jupiter and Saturn have held out the promise of providing an independent set of observations with which to test theories of planet formation. Yet elucidating their origins has proven elusive. Here we show that Iapetus can serve to discriminate between satellite formation models. Its accretion history can be understood in terms of a two-component gaseous subnebula, with a relatively dense inner region, and an extended tail out to the location of the irregular satellites, as in the SEMM model of Mosqueira and Estrada (2003a,b) (Mosqueira, I., Estrada, P.R. [2003a]. Icarus 163, 198-231; Mosqueira, I., Estrada, P.R. [2003b]. Icarus 163, 232-255). Following giant planet formation, planetesimals in the feeding zone of Jupiter and Saturn become dynamically excited, and undergo a collisional cascade. Ablation and capture of planetesimal fragments crossing the gaseous circumplanetary disks delivers enough collisional rubble to account for the mass budgets of the regular satellites of Jupiter and Saturn. This process can result in rock/ice fractionation as long as the make up of the population of disk crossers is non-homogeneous, thus offering a natural explanation for the marked compositional differences between outer solar nebula objects and those that accreted in the subnebulae of the giant planets. For a given size, icy objects are easier to capture and to ablate, likely resulting in an overall enrichment of ice in the subnebula. Furthermore, capture and ablation of rocky fragments become inefficient far from the planet for two reasons: the gas surface density of the subnebula is taken to drop outside the centrifugal radius, and the velocity of interlopers decreases with distance from the planet. Thus, rocky objects crossing the outer disks of Jupiter and Saturn never reach a temperature high enough to ablate either due to melting or vaporization, and capture is also greatly diminished there. In contrast, icy objects crossing the outer disks of each planet ablate due to the melting and vaporization of water-ice. Consequently, our model leads to an enhancement of the ice content of Iapetus, and to a lesser degree those of Titan, Callisto and Ganymede, and accounts for the (non-stochastic) compositions of these large, low-porosity outer regular satellites of Jupiter and Saturn. For this to work, the primordial population of planetesimals in the Jupiter-Saturn region must be partially differentiated, so that the ensuing collisional cascade produces an icy population of ?1 m size fragments to be ablated during subnebula crossing. We argue this is likely because the first generation of solar nebula ∼10 km planetesimals in the Jupiter-Saturn region incorporated significant quantities of 26Al. This is the first study successfully to provide a direct connection between nebula planetesimals and subnebulae mixtures with quantifiable and observable consequences for the bulk properties of the regular satellites of Jupiter and Saturn, and the only explanation presently available for Iapetus’ low density and ice-rich composition. 相似文献
11.
Infrared spectra and radiation chemical behavior of N2-dominated ices relevant to the surfaces of Triton and Pluto are presented. This is the first systematic IR study of proton-irradiated N2-rich ices containing CH4 and CO. Experiments at 12 K show that HCN, HNC, and diazomethane (CH2N2) form in the solid phase, along with several radicals. NH3 is also identified in irradiated N2 + CH4 and N2 + CH4 + CO. We show that HCN and HNC are made in irradiated binary ice mixtures having initial N2/CH4 ratios from 100 to 4, and in three-component mixtures have an initial N2/(CH4 + CO) ratio of 50. HCN and HNC are not detected in N2-dominated ices when CH4 is replaced with C2H6, C2H2, or CH3OH.The intrinsic band strengths of HCN and HNC are measured and used to calculate G(HCN) and G(HNC) in irradiated N2 + CH4 and N2 + CH4 + CO ices. In addition, the HNC/HCN ratio is calculated to be ∼1 in both icy mixtures. These radiolysis results reveal, for the first time, solid-phase synthesis of both HCN and HNC in N2-rich ices containing CH4.We examine the evolution of spectral features due to acid-base reactions (acids such as HCN, HNC, and HNCO and a base, NH3) triggered by warming irradiated ices from 12 K to 30-35 K. We identify anions (OCN−, CN−, and N3−) in ices warmed to 35 K. These ions are expected to form and survive on the surfaces of Triton and Pluto. Our results have astrobiological implications since many of these products (HCN, HNC, HNCO, NH3, NH4OCN, and NH4CN) are involved in the syntheses of biomolecules such as amino acids and polypeptides. 相似文献
12.
We have quantitatively studied, by infrared absorption spectroscopy, the CO/CO2 molecular number ratio after ion irradiation of ices and mixtures containing astrophysically relevant species such as CO,
CO2, H2O, CH4, CH3OH, NH3, O2, and N2 at 12–15 K. The ratios have also been measured after warm up to temperatures between 12 and 200 K. As a general result we
find that the CO/CO2 ratio decreases with the irradiation dose (amount of energy deposited on the sample). In all of the studied mixtures, as
expected, it decreases with increasing temperature because of CO sublimation. However the temperature where CO sublimes strongly
depends on the initial mixture, remaining at a temperature over 100 K in some cases. Our results might be relevant to interpret
the observed CO/CO2 ratio in several astrophysical scenarios such as planetary icy surfaces and ice mantles on grains in the interstellar medium.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
13.
To explain the observed abundances of CO2 in Titan's atmosphere, a relatively high water deposition into the atmosphere needs to be invoked due to the importance of H2O photolysis in CO2 production. A likely source of H2O is icy dust particles from space. This paper considers the direct dust input to Titan's atmosphere from the interplanetary environment, and also ejecta particles from micrometeoroid impacts with the icy satellites Hyperion, Iapetus and Phoebe. It is found that the likely mass influx to Titan is 10–16 to 10–15 kg m–2 s–1. This mass influx is an order of magnitude too low to explain the observed levels of CO2 in Titan's atmosphere in the context of a recent photochemical model. This leads one to speculate as to the likelihood of one large impact to Titan in the recent past;i.e., that the atmosphere is not in equilibrium but is cnrrently losing CO2. 相似文献
14.
The thermal histories of two geologically active satellites of Saturn—Titan and Enceladus—are discussed. During the Cassini mission, it was found that there are both nitrogen-containing compounds—NH3 and N2-and CO2 and CH4 in the water plumes of Enceladus; at that, ammonia is the prevailing form. This may testify that during evolution, the material
of the satellite was warmed up to T ∼ 500–600 K, when NH3 (the form of nitrogen capable of being accreted) could only be partly converted into N2. Contrary to Enceladus, the temperature inside Titan probably reached values higher than 800 K or even higher than 1000 K,
since the process of the chemical dissociation of ammonia was completely finished on this satellite and its atmosphere contains
only molecular nitrogen. While the internal heating of Titan up to high temperatures can be explained by its large mass, the
heating source for Enceladus’ interior is far from evident. Such traditional heating sources as the energy of gravitational
differentiation and the radiogenic heating due to shortliving 26Al and 60Fe could not be effective. The first one is because of the small size of Enceladus (RE ≈ 250 km), and the inefficiency of the second one is caused by the fact that the satellite was formed not earlier than 8–10
Myr after the formation of calcium and aluminum-enriched inclusions in carbonaceous chondrites (CAI), i.e., after 26Al had completely decayed. In the present paper, we propose other heating mechanisms-the heat of long-living radioactive elements
and tidal heat, which could provide the observed chemical composition of the water plumes of Enceladus rather than only the
differentiation of its protomatter into the ironstone core and the ice mantle. 相似文献
15.
Yasuhito Sekine Hiroshi Imanaka Takafumi Matsui Emma L.O. Bakes Christopher P. McKay 《Icarus》2008,194(1):186-200
In Titan's atmosphere consisting of N2 and CH4, large amounts of atomic hydrogen are produced by photochemical reactions during the formation of complex organics. This atomic hydrogen may undergo heterogeneous reactions with organic aerosol in the stratosphere and mesosphere of Titan. In order to investigate both the mechanisms and kinetics of the heterogeneous reactions, atomic deuterium is irradiated onto Titan tholin formed from N2 and CH4 gas mixtures at various surface-temperatures of the tholin ranging from 160 to 310 K. The combined analyses of the gas species and the exposed tholin indicate that the interaction mechanisms of atomic deuterium with the tholin are composed of three reactions; (a) abstraction of hydrogen from tholin resulting in gaseous HD formation (HD recombination), (b) addition of D atom into tholin (hydrogenation), and (c) removal of carbon and/or nitrogen (chemical erosion). The reaction probabilities of HD recombination and hydrogenation are obtained as ηabst=1.9(±0.6)×10−3×exp(−300/T) and ηhydro=2.08(±0.64)×exp(−1000/T), respectively. The chemical erosion process is very inefficient under the conditions of temperature range of Titan's stratosphere and mesosphere. Under Titan conditions, the rates of hydrogenation > HD recombination ? chemical erosion. Our measured HD recombination rate is about 10 times (with an uncertainty of a factor of 3-5) the prediction of previous theoretical model. These results imply that organic aerosol can remove atomic hydrogen efficiently from Titan's atmosphere through the heterogeneous reactions and that the presence of aerosol may affect the subsequent organic chemistry. 相似文献
16.
A.D. Fortes 《Planetary and Space Science》2012,60(1):10-17
Titan’s moment of inertia (MoI), estimated from the quadrupole gravity field measured by the Cassini spacecraft, is 0.342, which has been interpreted as evidence of a partially differentiated internal mass distribution. It is shown here that the observed MoI is equally consistent with a fully differentiated internal structure comprising a shell of water ice overlying a low-density silicate core; depending on the chemistry of Titan’s subsurface ocean, the core radius is between 1980 and 2120 km, and its uncompressed density is 2570–2460 kg m?3, suggestive of a hydrated CI carbonaceous chondrite mineralogy. Both the partially differentiated and fully differentiated hydrated core models constrain the deep interior to be several hundred degrees cooler than previously thought. I propose that Titan has a warm wet core below, or buffered at, the high-pressure dehydration temperature of its hydrous constituents, and that many of the gases evolved by thermochemical and radiogenic processes in the core (such as CH4 and 40Ar, respectively) diffuse into the icy mantle to form clathrate hydrates, which in turn may provide a comparatively impermeable barrier to further diffusion. Hence we should not necessarily expect to see a strong isotopic signature of serpentinization in Titan’s atmosphere. 相似文献
17.
We present near-IR (2.2-2.4 μm) reflectance and transmittance spectra of frozen (16 and 77 K) methanol (CH3OH) and water-methanol (1:1) mixtures before and after irradiation with 30 keV He+ and 200 keV H+ ions. Spectra of other simple hydrocarbons (CH4, C2H2, C2H4, C2H6) and CO have also been obtained both to help in the identification of the new molecules formed after ion irradiation of methanol-rich ices, and to get insight into the question of the presence of simple frozen hydrocarbons on the surface of some objects in the outer Solar System. The results confirm what obtained by studies performed in different spectral ranges, namely the ion-induced formation of CO and CH4, and, for the first time, evidence a strong decrease of the intensity of the methanol band at about 2.34 μm in comparison with that at 2.27 μm. The results are discussed in view of their relevance for icy objects in the Solar System (namely comets, Centaurs, and Kuiper belt objects) where CH3OH has been observed or suggested to be present. 相似文献
18.
Motivated by detections of nitriles in Titan's atmosphere, cometary comae, and the interstellar medium, we report laboratory investigations of the low-temperature chemistry of acetonitrile, propionitrile, acrylonitrile, cyanoacetylene, and cyanogen (CH3CN, CH3CH2CN, CH2CHCN, HCCCN, and NCCN, respectively). A few experiments were also done on isobutyronitrile and trimethylacetonitrile ((CH3)2CHCN and (CH3)3CCN, respectively). Trends were sought, and found, in the photo- and radiation chemical products of these molecules at 12-25 K. In the absence of water, all of these molecules isomerized to isonitriles, and CH3CN, CH3CH2CN, and (CH3)2CHCN also formed ketenimines. In the presence of H2O, no isonitriles were detected but rather the cyanate ion (OCN−) was seen in all cases. Although isonitriles, ketenimines, and OCN− were the main focus of our work, we also describe cases of hydrogen loss, to make smaller nitriles, and hydrogen addition (reduction), to make larger nitriles. HCN formation also was seen in most experiments. The results are presented in terms of nitrile ice chemistry on Titan, in cometary ice, and in the interstellar medium. Possible connections to prebiotic chemistry are briefly discussed. 相似文献
19.
C.Y. Robert WuD.L. Judge Bing-Ming ChengWen-Hao Shih Tai-Sone YihW.H. Ip 《Icarus》2002,156(2):456-473
Experimental results on the spectral identification of new infrared absorption features and the changes of their absorbances produced through vacuum ultraviolet-extreme ultraviolet (VUV-EUV) photon-induced chemical reactions in the C2H2-H2O mixed ices at 10 K are obtained. To the best of our knowledge, this is the first time that EUV photons have been employed in the study of the photolysis of ice analogues. Two different compositions, i.e., C2H2:H2O=1:4 and 1:1, were investigated in this work. A tunable intense synchrotron radiation light source available at the Synchrotron Radiation Research Center, Hsinchu, Taiwan, was employed to provide the required VUV-EUV photons. In this study, the photon wavelengths selected to irradiate the icy samples corresponded to the prominent solar hydrogen, helium, and helium ion lines at 121.6 nm, 58.4 nm, and 30.4 nm, respectively. The photon dosages used were typically in the range of 1×1015 to 2×1017 photons. Molecular species produced and identified in the ice samples at 10 K resulting from VUV-EUV photon irradiation are mainly CO, CO2, CH4, C2H6, CH3OH, and H2CO. In addition to several unidentified features, we have tentatively assigned several absorption features to HCO, C3H8, and C2H5OH. While new molecular species were formed, the original reactants, i.e., H2O and C2H2, were detectably depleted due to their conversion to other species. The new chemical species produced by irradiation of photons at 30.4 nm and 58.4 nm can be different from those produced by the 121.6-nm photolysis. In general, the product column density of CO reaches saturation at a lower photon dosage than that of CO2. Furthermore, the production yield of CO is higher than that of CO2 in the photon irradiation. In the present study, we also observe that the photon-induced chemical reaction yields are high using photons at 30.4 and 58.4 nm. The results presented in this work are essential to our understanding of chemical synthesis in ice analogues, e.g., the cometary-type ices and icy satellites of planetary systems. 相似文献
20.
Olga Prieto-Ballesteros Jeffrey S. Kargel Franck Selsis Eduardo Sebastián Martínez 《Icarus》2005,177(2):491-505
Several substances besides water ice have been detected on the surface of Europa by spectroscopic sensors, including CO2, SO2, and H2S. These substances might occur as pure crystalline ices, as vitreous mixtures, or as clathrate hydrate phases, depending on the system conditions and the history of the material. Clathrate hydrates are crystalline compounds in which an expanded water ice lattice forms cages that contain gas molecules. The molecular gases that may constitute Europan clathrate hydrates may have two possible ultimate origins: they might be primordial condensates from the interstellar medium, solar nebula, or jovian subnebula, or they might be secondary products generated as a consequence of the geological evolution and complex chemical processing of the satellite. Primordial ices and volatile-bearing compounds would be difficult to preserve in pristine form in Europa without further processing because of its active geological history. But dissociated volatiles derived from differentiation of a chondritic rock or cometary precursor may have produced secondary clathrates that may be present now. We have evaluated the current stability of several types of clathrate hydrates in the crust and the ocean of Europa. The depth at which the clathrates of SO2, CO2, H2S, and CH4 are stable have been obtained using both the temperatures observed in the surface [Spencer, J.R., Tamppari, L.K., Martin, T.Z., Travis, L.D., 1999. Temperatures on Europa from Galileo photopolarimeter-radiometer: Nighttime thermal anomalies. Science 284, 1514-1516] and thermal models for the crust. In addition, their densities have been calculated in order to determine their buoyancy in the ocean, obtaining different results depending upon the salinity of the ocean and type of clathrate. For instance, assuming a eutectic composition of the system MgSO4H2O for the ocean, CO2, H2S, and CH4 clathrates would float but SO2 clathrate would sink to the seafloor; an ocean of much lower salinity would allow all these clathrates to sink, except that CH4 clathrate would still float. Many geological processes may be driven or affected by the formation, presence, and destruction of clathrates in Europa such as explosive cryomagmatic activity [Stevenson, D.J., 1982. Volcanism and igneous processes in small icy satellites. Nature 298, 142-144], partial differentiation of the crust driven by its clathration, or the local retention of heat within or beneath clathrate-rich layers because of the low thermal conductivity of clathrate hydrates [Ross, R.G., Kargel, J.S., 1998. Thermal conductivity of Solar System ices, with special reference to martian polar caps. In: Schmitt, B., De Berg, C., Festou, M. (Eds.), Solar System Ices. Kluwer Academic, Dordrecht, pp. 33-62]. On the surface, destabilization of these minerals and compounds, triggered by fracture decompression or heating could result in formation of chaotic terrain morphologies, a mechanism that also has been proposed for some martian chaotic terrains [Tanaka, K.L., Kargel, J.S., MacKinnon, D.J., Hare, T.M., Hoffman, N., 2002. Catastrophic erosion of Hellas basin rim on Mars induced by magmatic intrusion into volatile-rich rocks. Geophys. Res. Lett. 29 (8); Kargel, J.S., Prieto-Ballesteros, O., Tanaka K.L., 2003. Is clathrate hydrate dissociation responsible for chaotic terrains on Earth, Mars, Europa, and Triton? Geophys. Res. 5. Abstract 14252]. Models of the evolution of the ice shell of Europa might take into account the presence of clathrate hydrates because if gases are vented from the silicate interior to the water ocean, they first would dissolve in the ocean and then, if the gas concentrations are sufficient, may crystallize. If any methane releases occur in Europa by hydrothermal or biological activity, they also might form clathrates. Then, from both geological and astrobiological perspectives, future missions to Europa should carry instrumentation capable of clathrate hydrate detection. 相似文献