Catalytic conversion of methanol to larger organic molecules over crystalline forsterite: Laboratory study and astrophysical implications

Li, Q.; Dai, Wenxin; Liu, B.S.; Sarre, P. J.; Xie, Miao; Cheung, Any

doi:10.1016/j.molap.2018.09.002

Cited by 6 publications

(5 citation statements)

References 52 publications

(60 reference statements)

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“…Therefore, complex organic molecules formed by gas-phase chemical reactions under warm conditions (in the earlier evolutional stage of a circumplanetary disk) might finally be frozen and incorporated into satellitesimals as the circumplanetary disk cools down. Furthermore, the catalytic conversion of methanol to larger organic molecules over heated crystalline silicates grains (up to ~700 K) demonstrated by Li et al (2018) might occur in a circumplanetary disk. Because the equatorial plane of a circumplanetary disk is nearly the same as the equatorial plane of a solar nebula, the icy satellitesimals thrown out from a circumplanetary disk may be a source of "chemically unique" Jupiter-family comets, such as 21P/G-Z.…”

Section: Discussionmentioning

confidence: 98%

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Ootsubo

Kawakita

Shinnaka

et al. 2020

Icarus

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Comet 21P/Giacobini-Zinner (hereafter, comet 21P/G-Z) is a Jupiter-family comet and a parent comet of the October Draconids meteor shower. If meteoroids originating from a Jupiter-family comet contain complex organic molecules, such as amino acids, they are essential pieces of the puzzle regarding the origin of life on Earth. We observed comet 21P/G-Z in the mid-infrared wavelength region using the Cooled Mid-infrared Camera and Spectrometer (COMICS) on the 8.2 m Subaru Telescope on UT 2005 July 5. Here, we report the unidentified infrared (UIR) emission features of comet 21P/G-Z, which are likely due to complex organic molecules (both aliphatic and aromatic hydrocarbons), and the thermal emission from amorphous/crystalline silicates and amorphous carbon grains in its mid-infrared low-resolution spectrum. The UIR features at ~8.2 µm, ~8.5 µm, and ~11.2 µm found in the spectrum of comet 21P/G-Z could be attributed to polycyclic aromatic hydrocarbons (or hydrogenated amorphous carbons) contaminated by N-or O-atoms, although part of the feature at ~11.2 µm comes from crystalline olivine. The other feature at ~9.2 µm might originate from aliphatic hydrocarbons. Comet 21P/G-Z is enriched in complex organic molecules. Considering that the derived mass fraction of crystalline silicates in comet 21P/G-Z is typical of comets, we propose that the comet originated from a circumplanetary disk of giant planets (similar to Jupiter and Saturn) where was warmer than the typical comet-forming region (5-30 au from the Sun) and was suitable for the formation of complex organic molecules. Comets from circumplanetary disks might be enriched in complex organic molecules, such as comet 21P/G-Z, and may have provided pre-biotic molecules to ancient Earth by direct impact or meteor showers.

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Section: Discussionmentioning

confidence: 98%

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Ootsubo

Kawakita

Shinnaka

et al. 2020

Icarus

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“…4, Table 1). Although further studies are required to establish a mechanism for synthesizing these molecules, Li et al (2018) have proposed adsorption processes as a first step in the catalysis reactions of organic compounds. The authors used forsterite and methanol in their experiments as starting materials to synthesize PAHs.…”

Section: The Role Of Minerals In Frozen Solutionsmentioning

confidence: 99%

“…The authors used forsterite and methanol in their experiments as starting materials to synthesize PAHs. They observed the oxygen atom of methanol binds to the silicon atom of forsterite, which leads to the elongation of the O-H bond of methanol and its subsequent rupture, resulting in the formation of radicals (Li et al, 2018).…”

Section: The Role Of Minerals In Frozen Solutionsmentioning

confidence: 99%

Radiation-induced reactions in comet analogues

López-Islas

Negrón‐Mendoza

2022

International Journal of Astrobiology

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Comets are a source of prebiotic molecules that likely enriched the early Earth during the Late Heavy Bombardment period. Laboratory experiments that replicate cometary conditions may facilitate understanding of the chemical reactions and supplement observational studies of these icy bodies. Prebiotic compounds, such as formic acid and formaldehyde, have been observed in comets. Furthermore, these compounds can easily be formed in experimental models using a variety of gas combinations and energy sources. We conducted experimental cometary simulations using radiation chemistry tools to obtain insight into the possible fate of formic acid and formaldehyde. The main results suggest a redundant system, signifying that the irradiation of formic acid forms formaldehyde molecules and vice versa. This phenomenon ensures the permanence of prebiotic molecules in high-radiation environments. Additionally, the potential role of forsterite and graphite was explored in cometary simulations. Our experimental results show the differential formation of aldehydes and other carbonyl-containing compounds dependent on the mineral phase present.

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“…Forsterite (Mg 2 SiO 4 ) is one of the most abundant olivinic minerals available on Earth and in space. , Experimental studies have reported the potential catalytic role of forsterite and Fe-doped forsterite for the conversion of methanol to olefine and PAHs. , However, theoretical and mechanistic studies on the catalytic activity of forsterite are currently lacking. Only a few studies have addressed the interaction of organic species with a forsterite surface using first-principle methods. − …”

Section: Introductionmentioning

confidence: 99%

Adsorption of Polycyclic Aromatic Hydrocarbons and C₆₀ onto Forsterite: C–H Bond Activation by the Schottky Vacancy

Campisi

Lamberts

Dzade

et al. 2022

ACS Earth Space Chem.

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Understanding how to catalytically break the C–H bond of aromatic molecules, such as polycyclic aromatic hydrocarbons (PAHs), is currently a big challenge and a subject of study in catalysis, astrochemistry, and planetary science. In the latter, the study of the breakdown reaction of PAHs on mineral surfaces is important to understand if PAHs are linked to prebiotic molecules in regions of star and planet formation. In this work, we employed a periodic density functional theory along with Grimme’s D4 (DFT-D4) approach for studying the adsorption of a sample of PAHs (naphthalene, anthracene, fluoranthene, pyrene, coronene, and benzocoronene) and fullerene on the [010] forsterite surface and its defective surfaces (Fe-doped and Ni-doped surfaces and a MgO-Schottky vacancy) for their implications in catalysis and astrochemistry. On the basis of structural and binding energy analysis, large PAHs and fullerene present stronger adsorption on the pristine, Fe-doped, and Ni-doped forsterite surfaces than small PAHs. On a MgO-Schottky vacancy, parallel adsorption of the PAH leads to the chemisorption process (C–Si and/or C–O bonds), whereas perpendicular orientation of the PAH leads to the catalytic breaking of the aromatic C–H bond via a barrierless reaction. Spin density and charge analysis show that C–H dissociation is promoted by electron donation from the vacancy to the PAH. As a result of the undercoordinated Si and O atoms, the vacancy acts as a Frustrated Lewis Pair (FLP) catalyst. Therefore, a MgO-Schottky vacancy [010] forsterite surface proved to have potential catalytic activity for the activation of C–H bond in aromatic molecules.

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Catalytic conversion of methanol to larger organic molecules over crystalline forsterite: Laboratory study and astrophysical implications

Cited by 6 publications

References 52 publications

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Radiation-induced reactions in comet analogues

Adsorption of Polycyclic Aromatic Hydrocarbons and C₆₀ onto Forsterite: C–H Bond Activation by the Schottky Vacancy

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Catalytic conversion of methanol to larger organic molecules over crystalline forsterite: Laboratory study and astrophysical implications

Cited by 6 publications

References 52 publications

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Unidentified infrared emission features in mid-infrared spectrum of comet 21P/Giacobini-Zinner

Radiation-induced reactions in comet analogues

Adsorption of Polycyclic Aromatic Hydrocarbons and C60 onto Forsterite: C–H Bond Activation by the Schottky Vacancy

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Adsorption of Polycyclic Aromatic Hydrocarbons and C₆₀ onto Forsterite: C–H Bond Activation by the Schottky Vacancy