globalchange  > 过去全球变化的重建
DOI: 10.1021/acs.jpca.9b03095
WOS记录号: WOS:000472800600006
论文题名:
Rate Coefficients for the Gas-Phase Reaction of (E)- and (Z)-CF3CF=CFCF3 with the OH Radical and Cl-Atom
作者: Baasandorj, Munkhbayar1,2,3; Papadimitriou, Vassileios C.1,2,4; Burkholder, James B.1
通讯作者: Burkholder, James B.
刊名: JOURNAL OF PHYSICAL CHEMISTRY A
ISSN: 1089-5639
EISSN: 1520-5215
出版年: 2019
卷: 123, 期:24, 页码:5051-5060
语种: 英语
WOS关键词: ATMOSPHERIC CHEMISTRY ; RATE CONSTANTS ; KINETICS ; POTENTIALS ; MECHANISMS ; PRODUCTS ; SPECTRA
WOS学科分类: Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS研究方向: Chemistry ; Physics
英文摘要:

The rate coefficients, k, for the gas-phase reaction of the OH radical and Cl-atom with (E)- and (Z)-CF3CF=CFCF3 were measured using a relative rate technique over a range of temperature (240-375 K) and bath gas pressure (50-630 Torr, He). The obtained rate coefficients were found to be independent of pressure under these conditions. The obtained rate coefficients for the reaction of Cl-atom with (E)- and (Z)-CF3CF=CFCF3 at 296 K were k(1)(296 K) = (7.23 +/- 0.3) x 10(-12) cm(3) molecule(-1) s(-1) and k(2)(296 K) = (6.70 +/- 0.3) x 10(-12) cm(3) molecule(-1) s(-1), respectively, with the temperature dependence described by the Arrhenius expressions: k(1)(T) = (3.47 +/- 0.35) x 10(-12) exp[(210 +/- 25)/T] cm(3) molecule(-1) s(-1) and k(2)(T) = (3.37 +/- 0.35) x 10(-12) exp[(199 +/- 25)/T] cm(3) molecule(-1) s(-1). The rate coefficients for the OH radical reaction with (E)- and (Z)-CF3CF=CFCF3 were found to be k(3)(296-375 K) = (4.34 +/- 0.45) x 10(-13) cm(3) molecule(-1) s(-1) and k(4)(296-375 K) = (3.30 +/- 0.35) x 10(-13) cm(3) molecule(-1) s(-1), respectively. The quoted rate coefficient uncertainties are 2 sigma (95% confidence level) and include estimated systematic errors. The rate coefficients for the reaction of OH with a mixture of the two stereoisomers were determined using a pulsed laser photolysis-laser-induced fluorescence (PLP-LIF) technique for comparison with previous kinetic measurements using stereoisomer mixtures. The effective rate coefficient for the 0.7/0.3 (E)/(Z) stereoisomer sample was found to be nearly independent of temperature over the range 222-375 K with a value of (4.47 +/- 0.36) x 10(-13) cm(3) molecule(-1) s(-1). The atmospheric lifetimes for (E)- and (Z)-CF3CF=CFCF3 due to OH-reactive loss are estimated to be 25 and 35 days, respectively. The lifetime-corrected radiative efficiencies (W m(-2) ppb(-1)) and 100 year time horizon global warming potentials derived in this work are 0.05 and 1.2 for (E)-CF3CF=CFCF3 and 0.13 and 4.1 for (Z)-CF3CF=CFCF3. The photochemical ozone creation potentials for (E)- and (Z)-CF3CF=CFCF3 are estimated to be 2.5 and 2.1, respectively.


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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/140505
Appears in Collections:过去全球变化的重建

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作者单位: 1.NOAA, Earth Syst Res Lab, Chem Sci Div, 325 Broadway, Boulder, CO 80305 USA
2.Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
3.Utah Div Air Qual, Salt Lake City, UT 84114 USA
4.Univ Crete, Dept Chem, Lab Photochem & Chem Kinet, Iraklion, Crete, Greece

Recommended Citation:
Baasandorj, Munkhbayar,Papadimitriou, Vassileios C.,Burkholder, James B.. Rate Coefficients for the Gas-Phase Reaction of (E)- and (Z)-CF3CF=CFCF3 with the OH Radical and Cl-Atom[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2019-01-01,123(24):5051-5060
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