Measurements of infrared absorption cross-sections for n-C3F8, c-C4F8, n-C4F10, and n-C5F12 from 298 to 350 K

IF 1.4 4区 物理与天体物理 Q4 PHYSICS, ATOMIC, MOLECULAR & CHEMICAL Journal of Molecular Spectroscopy Pub Date : 2024-03-01 DOI:10.1016/j.jms.2024.111900
Muhammad Osama Ishtiak , Orfeo Colebatch , Karine Le Bris , Paul J. Godin , Kimberly Strong
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Abstract

Perfluoro-n-propane, perfluorocyclobutane, perfluoro-n-butane, and perfluoro-n-pentane are non-ozone-depleting industrial alternatives to chlorofluorocarbons and hydrochlorofluorocarbons. However, these perfluoroalkanes have significant band strength in the atmospheric window from 800 to 1200 cm−1. Coupled with their millennial-scale atmospheric lifetimes, they can lead to significant long-term global warming. Infrared spectra are required to quantify the climate impacts. This work provides a set of high-temperature infrared absorption cross-sections in the range 298–350 K at 0.1 cm−1 resolution from 515 to 1500 cm−1 for each compound. Our cross-sections generally agree with literature measurements except for perfluoro-n-pentane. We use density functional theory to calculate the absorption cross-sections from 0 to 515 cm−1 using the B3LYP functional and several basis sets. The 6-31G(d,p) basis set provides the best results for linear perfluoroalkanes, while the def2-TZVP basis set provides the best results for cyclic perfluoroalkanes. Using experimental cross-sections, we calculate the radiative efficiency and global warming potential for each compound, utilizing the Pinnock curve from Shine and Myhre (2020) and atmospheric lifetimes from Hodnebrog et al. (2020). These quantities are found to be independent of temperature. The average 100-year global warming potential derived from all cross-sections is 9,610±1,260, 10,800±1,420, 10,100±1,330, and 9,380±1,230 for perfluoro-n-propane, perfluorocyclobutane, perfluoro-n-butane, and perfluoro-n-pentane, respectively. Combining the data in this work with our previous measurements reveals that the global warming potential for perfluoroalkanes with an increasing number of CF bonds depends on the ratio of radiative efficiency to molecular weight.

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正-C3F8、正-C4F8、正-C4F10 和正-C5F12 在 298 至 350 K 之间的红外吸收截面测量结果
全氟正丙烷、全氟环丁烷、全氟正丁烷和全氟正戊烷是氯氟化碳和氯氟烃的非臭氧消耗工业替代品。然而,这些全氟烷烃在 800 至 1200 厘米的大气窗口中具有显著的带强度。再加上它们在大气中的千年寿命,它们会导致全球长期显著变暖。需要红外光谱来量化对气候的影响。这项研究为每种化合物提供了一组 298-350 K 范围内的高温红外吸收截面,分辨率为 0.1 厘米(从 515 厘米到 1500 厘米)。除全氟正戊烷外,我们的横截面与文献测量结果基本吻合。我们利用密度泛函理论,使用 B3LYP 函数和多个基集计算了 0 至 515 厘米的吸收截面。6-31G(d,p) 基集为线性全氟烷烃提供了最佳结果,而 def2-TZVP 基集则为环状全氟烷烃提供了最佳结果。通过实验截面,我们利用 Shine 和 Myhre(2020 年)的平诺克曲线以及 Hodnebrog 等人(2020 年)的大气寿命计算出了每种化合物的辐射效率和全球变暖潜势。研究发现,这些数值与温度无关。从所有横截面得出的全氟正丙烷、全氟环丁烷、全氟正丁烷和全氟正戊烷的 100 年平均全球升温潜能值分别为 9,610 ± 1,260 、10,800 ± 1,420 、10,100 ± 1,330 和 9,380 ± 1,230 。将这项工作中的数据与我们之前的测量结果相结合,可以发现 CF 键数量不断增加的全氟烷烃的全球变暖潜势取决于辐射效率与分子量之比。
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来源期刊
CiteScore
2.70
自引率
21.40%
发文量
94
审稿时长
29 days
期刊介绍: The Journal of Molecular Spectroscopy presents experimental and theoretical articles on all subjects relevant to molecular spectroscopy and its modern applications. An international medium for the publication of some of the most significant research in the field, the Journal of Molecular Spectroscopy is an invaluable resource for astrophysicists, chemists, physicists, engineers, and others involved in molecular spectroscopy research and practice.
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