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Density Functional Study of Sulfur Hexafluoride (SF6) and Its Hydrogen Derivatives Jacek Piechota, Marta Kinga Bruska

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Density Functional Study of Sulfur Hexafluoride (SF6) and Its Hydrogen Derivatives Jacek Piechota, Marta Kinga Bruska Density Functional Study of Sulfur Hexafluoride (SF6) and its Hydrogen Derivatives Jacek Piechota, Marta Kinga Bruska To cite this version: Jacek Piechota, Marta Kinga Bruska. Density Functional Study of Sulfur Hexafluoride (SF6) and its Hydrogen Derivatives. Molecular Simulation, Taylor & Francis, 2008, 34 (10-15), pp.1041-1050. 10.1080/08927020802258708. hal-00515048 HAL Id: hal-00515048 https://hal.archives-ouvertes.fr/hal-00515048 Submitted on 4 Sep 2010 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. For Peer Review Only Density Functional Study of Sulfur Hexafluoride (SF6) and its Hydrogen Derivatives Journal: Molecular Simulation/Journal of Experimental Nanoscience Manuscript ID: GMOS-2008-0043.R1 Journal: Molecular Simulation Date Submitted by the 15-May-2008 Author: Complete List of Authors: Piechota, Jacek; University of Warsaw, ICMM Bruska, Marta; Jagiellonian University, Department of Chemistry Keywords: sulfur hexafluoride, greenhouse gases, density functional theory Note: The following files were submitted by the author for peer review, but cannot be converted to PDF. You must view these files (e.g. movies) online. SF6_Bruska_Piechota_figures.rar SF6_Bruska_Piechota_update_figures.tar http://mc.manuscriptcentral.com/tandf/jenmol Page 1 of 30 1 2 "Catchline" (i.e. wording at head of first page only) Journal Name in Full 3 Vol. X, No. X, Month 200X, 000–000 4 (PLEASE LEAVE THESE VOLUME/ 5 6 ISSUE DETAILS TO BE ASSIGNED BY 7 JOURNALS PRODUCTION AT 8 A LATER STAGE) 9 10 11 12 The Authors 13 14 (DO NOT INCLUDE THIS AT FIRST SUBMISSION FOR 15 BLIND REVIEW, BUT DO INCUDE IT WHEN PREPARING 16 For Peer THE FINALLYReview ACCEPTED Only MANUSCRIPT FOR SUBM.) 17 Molecular Simulation 18 19 RESEARCH NOTE 20 21 22 Density Functional Study of Sulfur Hexafluoride (SF 6) and its Hydrogen Derivatives. 23 24 25 26 Abstract 27 28 29 Density functional study has been performed for group of compounds derived from sulfur 30 hexafluoride (SF 6) by consecutively substituting fluorine with hydrogen. SF 6 is widely used as the 31 insulating gas in the electrical industry and is recognized as one of the greenhouse gases with 32 33 extraordinary global warming potential. The aim of the present study is to look for potential 34 industrial alternatives to SF 6 as well as to examine mechanisms that can contribute to its faster 35 atmospheric decay. The ground state geometries, binding energies, vibrational spectra, charge 36 distributions, dipole moments, as well as thermodynamic properties for the series of the SF 6-nHn 37 (n=0…6) molecules have been obtained and discussed. For comparison, computational results for 38 39 the SCl 6 molecule have also been included in the present study. 40 41 Keywords : sulfur hexafluoride; greenhouse gases; density functional theory; 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 - 1 - http://mc.manuscriptcentral.com/tandf/jenmol Page 2 of 30 1 2 "Catchline" (i.e. wording at head of first page only) Journal Name in Full 3 Vol. X, No. X, Month 200X, 000–000 4 5 6 7 8 9 10 11 12 13 M. K. Bruska, J. Piechota 14 15 16 For Peer Review Only 17 Molecular Simulation 18 19 20 RESEARCH NOTE 21 22 23 Density Functional Study of Sulfur Hexafluoride (SF 6) and its Hydrogen Derivatives. 24 25 26 27 28 a b* 29 MARTA KINGA BRUSKA AND JACEK PIECHOTA 30 a Department of Chemistry, Jagiellonian University, ul. R. Ingardena 3,30-060 Kraków, Poland 31 b Interdisciplinary Centre for Materials Modelling, University of Warsaw, ul. Pawinskiego 5a, 02-106 Warszawa, Poland 32 33 34 35 36 Abstract 37 38 39 Density functional study has been performed for group of compounds derived from sulfur 40 hexafluoride (SF ) by consecutively substituting fluorine with hydrogen. SF is widely used as the 41 6 6 42 insulating gas in the electrical industry and is recognized as one of the greenhouse gases with 43 extraordinary global warming potential. The aim of the present study is to look for potential 44 industrial alternatives to SF 6 as well as to examine mechanisms that can contribute to its faster 45 atmospheric decay. The ground state geometries, binding energies, vibrational spectra, charge 46 distributions, dipole moments, as well as thermodynamic properties for the series of the SF H 47 6-n n 48 (n=0…6) molecules have been obtained and discussed. For comparison, computational results for 49 the SCl 6 molecule have also been included in the present study. 50 51 Keywords : sulfur hexafluoride; greenhouse gases; density functional theory; 52 53 54 55 56 57 58 59 60 _____________________ * Email: [email protected] - 2 - http://mc.manuscriptcentral.com/tandf/jenmol Page 3 of 30 1 2 1. Introduction 3 4 Interest in the sulfur hexafluoride (SF ) system stems both from practical and theoretical 5 6 6 considerations. It is one of the most popular (next to air) insulating gases, with a breakdown 7 strength of about 3 times that of air. It has a number of technologically important properties: it is 8 not flammable and non-toxic; at normal temperatures, it is also non-corrosive, and is fairly inert. 9 That is why SF 6 is commonly used in industry as a gaseous dielectric and as a plasma etching gas in 10 applications such as: circuit breakers, gas-insulated busbar systems, and also for large scale 11 12 scientific applications such as tandem particle accelerators. Other areas of application of SF 6 13 include the magnesium industry to protect molten magnesium from oxidation and potentially 14 violent burning, and semiconductor manufacturing to create circuitry patterns on silicon wafers. 15 Also, SF 6 is a candidate refrigerant to replace the chlorofluorocarbons (CFC's) which are damaging 16 For Peer Review Only the ozone layer. For an extensive review of SF 6 technical applications see, for example, [1] and 17 publications therein. 18 19 On the theoretical side, SF 6 has become a classic molecule for the study of electron 20 attachment at ultralow electron energies. The attachment of low energy electrons to SF 6 results in 21 — — formation of a metastable negative ion by the process: SF 6 + e → SF 6 [2-5]. An understanding of 22 the thermal electron attachment properties and temperature behaviour of rate constant for SF is, in 23 6 24 turn, of importance in the design of gaseous insulators and diffuse discharge switchers. 25 Furthermore, SF 6 has a unique, octahedral symmetry structure, which provides good 26 example of shape resonance phenomena. The infrared active modes of octahedral molecules are of 27 F1u symmetry and ν3 as well as ν4 bands are allowed in absorption [6]. In particular, the region of 28 the ν fundamental near 950 cm -1 has very strong absorption. The bond dissociation energy of SF 29 3 6 30 (to SF 5 + F) is 3.82 eV, but photodissociation is not observed until the photon energy exceeds ~10 31 eV [4]. 32 However, at the same time SF 6 is the most potent greenhouse gas that has been evaluated by 33 the Intergovernmental Panel on Climate Change (IPCC), with a global warming potential (GWP) of 34 22,800 times that of CO 2 when compared over a 100 year period [7]. Two main factors contributing 35 to this extraordinary high value of GWP is strong radiative forcing (0.52 Wm -2ppb-1) and very long 36 37 atmospheric lifetime (3200 years) [8]. In the stratosphere, the highest energy solar photons have an 38 energy of ~6 eV, so it is very unlikely that SF 6 will be photodissociated there. Therefore, although 39 the concentration of SF 6 is still relatively low in the Earth's atmosphere (5.21 ppt) [8], it is one of 40 the greenhouse gases that the Kyoto Protocol seeks to control [9], as even small amounts of SF 6 41 emissions can constitute a significant carbon-equivalent emission tonnage. 42 Apart from destroying ozone layer greenhouse gases that can absorb infrared radiation in the 43 -1 44 so-called “atmospheric window” between the wavelengths of 800 - 1400 cm are of great concern 45 because they are able to trap radiation that would have otherwise been emitted into space — most of 46 the radiation emitted by the earth's surface at wavelengths within in the atmospheric window would 47 have passed through the Earth's atmosphere without heating it. 48 Recently, another compound with extremely strong radiative forcing (of 0.59 Wm -2ppb -1), 49 50 identified as trifluoromethyl sulfur pentafluoride (SF 5CF 3), has been detected in the atmosphere 51 [10,11]. It is supposed that SF 5CF 3 originates as a breakdown product of SF 6 formed by high- 52 voltage discharges in electric industry equipment [10]. Atmospheric lifetime of SF 5CF 3 (~800 53 years) is lower than that of SF 6, but its value of GWP (~17,700) is one of the highest of all other 54 greenhouse gases [7]. 55 56 It is worth noting, however, that the greenhouse gases with the greatest GWP values are the 57 fully fluorinated compounds (FFC’s): CF 4, C 2F6, C 3F8, c-C4F8, SF 6, NF 3 and CHF 3, that are widely 58 used by the semiconductor industry [12].
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