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Article: Formation of polycyclic aromatic hydrocarbons from acetylene over nanosized olivine-type silicates

TitleFormation of polycyclic aromatic hydrocarbons from acetylene over nanosized olivine-type silicates
Authors
Issue Date2012
PublisherRoyal Society of Chemistry. The Journal's web site is located at http://www.rsc.org/pccp
Citation
Physical Chemistry Chemical Physics, 2012, v. 14 n. 18, p. 6603-6610 How to Cite?
AbstractThe formation mechanism of polycyclic aromatic hydrocarbon (PAH) molecules in interstellar and circumstellar environments is not well understood although the presence of these molecules is widely accepted. In this paper, addition and aromatization reactions of acetylene over astrophysically relevant nesosilicate particles are reported. Gas-phase PAHs produced from exposure of acetylene gas to crystalline silicates using pulsed supersonic jet expansion (SJE) conditions were detected by time-of-flight mass spectrometry (TOF-MS). The PAHs produced were further confirmed in a separate experiment using a continuous flow fixed-bed reactor in which acetylene was introduced at atmospheric pressure. The gas-phase effluent and solutions of the carbonaceous compounds deposited on the nesosilicate particles were analyzed using gas chromatography-mass spectrometry (GC-MS). A mechanism for PAH formation is proposed in which the Mg 2+ ions in the nesosilicate particles act as Lewis acid sites for the acetylene reactions. Our studies indicate that the formation of PAHs in mixed-chemistry astrophysical environments could arise from acetylene interacting with olivine nano-particles. These nesosilicate particles are capable of providing catalytic centres for adsorption and activation of acetylene molecules that are present in the circumstellar environments of mass-losing carbon stars. The structure and physical properties of the particles were characterized by means of X-ray diffraction (XRD), Fourier transform infrared (FT-IR) and high-resolution transmission electron microscopy (HRTEM) techniques. © the Owner Societies 2012.
Persistent Identifierhttp://hdl.handle.net/10722/146857
ISSN
2015 Impact Factor: 4.449
2015 SCImago Journal Rankings: 1.836
ISI Accession Number ID
Funding AgencyGrant Number
Research Grants Council of Hong Kong Special Administrative Region, China701309
University of Nottingham
EPSRC
Funding Information:

We thank Dr Michael Drake of the University of Arizona for kindly providing a geological olivine sample. This work was supported by a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. 701309). MH thanks the University of Nottingham for award of a Universitas 21 travel scholarship and EPSRC for a studentship.

References

 

DC FieldValueLanguage
dc.contributor.authorTian, Men_HK
dc.contributor.authorLiu, BSen_HK
dc.contributor.authorHammonds, Men_HK
dc.contributor.authorWang, Nen_HK
dc.contributor.authorSarre, PJen_HK
dc.contributor.authorCheung, ASCen_HK
dc.date.accessioned2012-05-23T05:42:46Z-
dc.date.available2012-05-23T05:42:46Z-
dc.date.issued2012en_HK
dc.identifier.citationPhysical Chemistry Chemical Physics, 2012, v. 14 n. 18, p. 6603-6610en_HK
dc.identifier.issn1463-9076en_HK
dc.identifier.urihttp://hdl.handle.net/10722/146857-
dc.description.abstractThe formation mechanism of polycyclic aromatic hydrocarbon (PAH) molecules in interstellar and circumstellar environments is not well understood although the presence of these molecules is widely accepted. In this paper, addition and aromatization reactions of acetylene over astrophysically relevant nesosilicate particles are reported. Gas-phase PAHs produced from exposure of acetylene gas to crystalline silicates using pulsed supersonic jet expansion (SJE) conditions were detected by time-of-flight mass spectrometry (TOF-MS). The PAHs produced were further confirmed in a separate experiment using a continuous flow fixed-bed reactor in which acetylene was introduced at atmospheric pressure. The gas-phase effluent and solutions of the carbonaceous compounds deposited on the nesosilicate particles were analyzed using gas chromatography-mass spectrometry (GC-MS). A mechanism for PAH formation is proposed in which the Mg 2+ ions in the nesosilicate particles act as Lewis acid sites for the acetylene reactions. Our studies indicate that the formation of PAHs in mixed-chemistry astrophysical environments could arise from acetylene interacting with olivine nano-particles. These nesosilicate particles are capable of providing catalytic centres for adsorption and activation of acetylene molecules that are present in the circumstellar environments of mass-losing carbon stars. The structure and physical properties of the particles were characterized by means of X-ray diffraction (XRD), Fourier transform infrared (FT-IR) and high-resolution transmission electron microscopy (HRTEM) techniques. © the Owner Societies 2012.en_HK
dc.languageengen_US
dc.publisherRoyal Society of Chemistry. The Journal's web site is located at http://www.rsc.org/pccpen_HK
dc.relation.ispartofPhysical Chemistry Chemical Physicsen_HK
dc.titleFormation of polycyclic aromatic hydrocarbons from acetylene over nanosized olivine-type silicatesen_HK
dc.typeArticleen_HK
dc.identifier.emailCheung, ASC:hrsccsc@hku.hken_HK
dc.identifier.authorityCheung, ASC=rp00676en_HK
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1039/c2cp23309fen_HK
dc.identifier.scopuseid_2-s2.0-84861853315en_HK
dc.identifier.hkuros199751en_US
dc.relation.referenceshttp://www.scopus.com/mlt/select.url?eid=2-s2.0-84861853315&selection=ref&src=s&origin=recordpageen_HK
dc.identifier.volume14en_HK
dc.identifier.issue18en_HK
dc.identifier.spage6603en_HK
dc.identifier.epage6610en_HK
dc.identifier.eissn1463-9084-
dc.identifier.isiWOS:000302951500056-
dc.publisher.placeUnited Kingdomen_HK
dc.identifier.scopusauthoridTian, M=55241414500en_HK
dc.identifier.scopusauthoridLiu, BS=24399628800en_HK
dc.identifier.scopusauthoridHammonds, M=6603227273en_HK
dc.identifier.scopusauthoridWang, N=55241136700en_HK
dc.identifier.scopusauthoridSarre, PJ=6603564950en_HK
dc.identifier.scopusauthoridCheung, ASC=7401806538en_HK

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