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New and Improved Infrared Absorption Cross Sections for Chlorodifluoromethane (HCFC-22)

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New and Improved Infrared Absorption Cross Sections for Chlorodifluoromethane (HCFC-22) Atmos. Meas. Tech., 9, 2593–2601, 2016 www.atmos-meas-tech.net/9/2593/2016/ doi:10.5194/amt-9-2593-2016 © Author(s) 2016. CC Attribution 3.0 License. New and improved infrared absorption cross sections for chlorodifluoromethane (HCFC-22) Jeremy J. Harrison1,2 1Department of Physics and Astronomy, University of Leicester, University Road, Leicester, LE1 7RH, UK 2National Centre for Earth Observation, University of Leicester, University Road, Leicester, LE1 7RH, UK Correspondence to: Jeremy J. Harrison ([email protected]) Received: 10 December 2015 – Published in Atmos. Meas. Tech. Discuss.: 18 January 2016 Revised: 3 May 2016 – Accepted: 6 May 2016 – Published: 17 June 2016 Abstract. The most widely used hydrochlorofluorocarbon 1 Introduction (HCFC) commercially since the 1930s has been chloro- difluoromethane, or HCFC-22, which has the undesirable The consumer appetite for safe household refrigeration led effect of depleting stratospheric ozone. As this molecule to the commercialisation in the 1930s of dichlorodifluo- is currently being phased out under the Montreal Pro- romethane, or CFC-12, a non-flammable and non-toxic re- tocol, monitoring its concentration profiles using infrared frigerant (Myers, 2007). Within the next few decades, other sounders crucially requires accurate laboratory spectroscopic chemically related refrigerants were additionally commer- data. This work describes new high-resolution infrared ab- cialised, including chlorodifluoromethane, or a hydrochlo- sorption cross sections of chlorodifluoromethane over the rofluorocarbon known as HCFC-22, which found use in a spectral range 730–1380 cm−1, determined from spectra wide array of applications such as air conditioners, chillers, recorded using a high-resolution Fourier transform spectrom- and refrigeration for food retail and industrial processes. Ad- eter (Bruker IFS 125HR) and a 26 cm pathlength cell. Spec- ditionally, HCFC-22 was a component of refrigerant R-502, tra of chlorodifluoromethane/dry synthetic air mixtures were an azeotropic blend of 48.8 % HCFC-22 and 51.2 % CFC- recorded at resolutions between 0.01 and 0.03 cm−1 (calcu- 115 by mass, introduced in the 1960s for commercial refrig- lated as 0.9/MOPD; MOPD denotes the maximum optical eration equipment (Watanabe, 2003). The use of chlorodi- path difference) over a range of temperatures and pressures fluoromethane has also grown as a feedstock, for example (7.5–762 Torr and 191–295 K) appropriate for atmospheric its pyrolysis yields tetrafluoroethylene (TFE), the monomer conditions. This new cross-section dataset improves upon for polytetrafluoroethylene (PTFE), which is trademarked as the one currently available in the HITRAN (HIgh-resolution Teflon (Myers, 2007). Furthermore, its manufacture results TRANsmission) and GEISA (Gestion et Etude des Informa- in the by-product trifluoromethane, or fluoroform (HFC-23), tions Spectroscopiques Atmosphériques) databases; in par- a very strong greenhouse gas which continues to increase in ticular it provides coverage over a wider range of pressures the atmosphere (Harrison et al., 2012). and temperatures, has more accurate wavenumber scales, The discovery that CFCs (chlorofluorocarbons) could more consistent integrated band intensities, improved signal- reach the stratosphere and photodissociate to release chlo- to-noise, is free of channel fringing, and additionally covers rine atoms, which would catalyse the destruction of strato- the ν2 and ν7 bands. spheric ozone (Solomon, 1999), led to international action and the ratification of the 1987 Montreal Protocol (and its later amendments), which aimed to phase out the worldwide production and use of CFCs and other ozone-depleting sub- stances. HCFCs (hydrochlorofluorocarbons), which were not regulated until the 1992 amendment and have a less delete- rious effect on the ozone layer than CFCs, were designated “transitional” replacements to aid in the rapid phase-out of Published by Copernicus Publications on behalf of the European Geosciences Union. 2594 J. J. Harrison: New and improved infrared absorption cross sections for HCFC-22 CFCs. With the worldwide CFC phase-out achieved, the fo- appropriate resolution (Doppler-limited at the lowest pres- cus has shifted to ending the use of HCFCs themselves, with sures). This work presents new spectroscopic data which im- a final phase-out currently scheduled for 2040 in the devel- prove upon those currently available in the HITRAN (HIgh- oping world and 2030 for developed countries. resolution TRANsmission) and GEISA (Gestion et Etude des HCFCs, in particular HCFC-22, continue to increase in the Informations Spectroscopiques Atmosphériques) databases. atmosphere. HCFC-22 is currently the most abundant HCFC In Sect. 2, a discussion of previous HCFC-22 IR absorp- in the Earth’s atmosphere; it has an ozone depletion potential tion cross-section datasets, derived from laboratory measure- of 0.034 (Harris et al., 2014), and an atmospheric lifetime of ments, is presented. Section 3 provides details on the new 11.9 years (Harris et al., 2014). It is also a very strong green- measurements taken as part of this work and the derivation house gas with a 100-year global warming potential of 1780 of cross sections, with Sect. 4 providing a discussion of the (Harris et al., 2014). It is unsurprising, therefore, that there is results and comparison with previous measurements. much work carried out in monitoring HCFC-22 atmospheric concentrations. For example, according to in situ, ground- 2 Previous quantitative spectroscopic measurements of based AGAGE (Advanced Global Atmospheric Gases Exper- chlorodifluoromethane iment) measurements, the tropospheric abundance of HCFC- 22 increased from 191.8 ppt in 2008 to 214.2 ppt in 2011 to There are two principal chlorodifluoromethane isotopo- 35 37 219.8 ppt in 2012 (Carpenter et al., 2014), with a 2011–2012 logues, CH ClF2 and CH ClF2, with abundances of ∼ 76 growth rate of 2.6 % yr−1. However, emissions of HCFC-22 and ∼ 24 %, respectively. Both isotopologues are asymmet- −1 have stabilised since 2008 at ∼ 370 Gg yr (Carpenter et al., ric tops belonging to the Cs point group, and each possess 2014). Saikawa et al. (2012) have estimated regional HCFC- a single plane of symmetry (CHCl) containing the a and c 22 emissions from globally distributed surface data, which principal axes. Chlorodifluoromethane has nine fundamental 0 indicate an increasing trend between 1995 and 2009, and a vibrational modes; six (ν1–ν6/ are symmetric (A ) with re- surge in HCFC-22 emissions between 2005 and 2009 from spect to the symmetry plane, appearing as a/c-type bands in 00 developing countries in Asia, including China and India, par- the IR, and three (ν7–ν9/ are antisymmetric (A ) with respect tially offsetting first efforts in developed countries to phase- to the symmetry plane, corresponding to b-type bands (Snels out production and consumption. Although there is believed and D’Amico, 2001). to be a large worldwide bank of HCFC-22 in refrigeration The 730–1380 cm−1 spectral range covered in the systems, it is expected that emissions will decline over the present work contains a number of strong band systems: −1 37 −1 coming decade as new refrigerants are adopted (Carpenter et the fundamental ν4 ∼ 804.5 cm (CH ClF2//809.3 cm 35 al., 2014). (CH ClF2/ (Ross et al., 1989) in Fermi resonance 37 Measurements of HCFC-22 in the atmosphere are also with the overtone 2ν6 ∼ 820.9 (CH ClF2//829.1 35 made using remote-sensing techniques. The literature re- (CH ClF2/ (Ross et al., 1989), and Coriolis-coupled −1 −1 ports a number of remote-sensing instruments capable of doublets ν3 ∼ 1108.7 cm and ν8 ∼ 1127.1 cm 37 −1 35 measuring HCFC-22 in the Earth’s atmosphere: the ATMOS (CH ClF2//1127.3 cm (CH ClF2/ (Snels and −1 37 (Atmospheric Trace MOlecule Spectroscopy) instrument de- D’Amico, 2001), and ν2 ∼ 1312.9 cm (CH ClF2//1313.1 35 −1 ployed on the space shuttle (Irion et al., 2002); the JPL (CH ClF2/ and ν7 ∼ 1351.7 cm (Thompson et al., 2002). balloon-borne MkIV interferometer (Velazco et al., 2011); Figure 1 provides a plot of the new absorption cross section the MIPAS (Michelson Interferometer for Passive Atmo- at 270.0 K and 7.51 Torr with these main band systems spheric Sounding) instrument on ENVISAT (ENVIronmen- labelled. Note that the ν4 and 2ν6 Q branches associated tal SATellite) (e.g. Moore and Remedios, 2008); and the with each isotopologue are easily identified in Fig. 1. Full ACE-FTS (Atmospheric Chemistry Experiment – Fourier details on the measurement conditions and derivation of this transform spectrometer) instrument on SCISAT (Brown et cross section are given in Sect. 3. al., 2011). The first published absolute intensities of chlorodiflu- Crucially these remote-sensing datasets all rely on the ac- oromethane IR bands were those of Varanasi and Chu- curacy of the underlying laboratory spectroscopy used in damani (1988); however it was several years later before the forward model. Since the chlorodifluoromethane infrared absorption cross sections appeared (McDaniel et al., 1991). (IR) spectrum consists of an abundance of densely packed Derived from measurements of pure chlorodifluoromethane lines, it is virtually an impossible task to derive spectroscopic at 0.03 cm−1 resolution and 203, 213, 233, 253, 273, and line parameters. The solution for remote-sensing purposes is 293 K (780–1335 cm−1/, these cross sections were subse- to derive absorption cross sections from air-broadened spec- quently incorporated into the HITRAN 1992 compilation tra recorded in the laboratory. In order to be most useful (Rothman et al., 1992; Massie and Goldman, 1992). N2- for remote sensing, these cross-section datasets require (1) broadened chlorodifluoromethane absorption cross sections accurate band intensities; (2) accurate wavenumber scales; for the bands between 700 and 1400 cm−1, derived from (3) a wide coverage of atmospherically relevant pressure– measurements over a range of temperatures down to 200 K temperature (PT) combinations; (4) spectra recorded at an at a spectral resolution of 0.03 cm−1, were subsequently pub- Atmos.
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