Temperature-dependent kinetics study of the reactions of O(1D2) with N2 and O2

Strekowski, Rafal; Nicovich, J. M.; Wine, P. H.

doi:10.1039/b400243a

Cited by 24 publications

(39 citation statements)

References 56 publications

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“…The results, listed in Table 1 and illustrated in Fig. 2 for N 2 O, are k 10 (298 K)=(0.33±0.06)×10 −10 cm 3 molecule −1 s −1 and k 11 (298 K)=(1.45±0.2)×10 −10 cm 3 molecule −1 s −1 , which agree (within combined uncertainties) with the evaluated literature (Sander et al, 2006;Atkinson et al, 2007) and other recent determinations (Blitz et al, 2004;Dunlea and Ravishankara, 2004b;Strekowski et al, 2004;Carl, 2005;Takahashi et al, 2005). The good agreement indicates that potential problems associated with formation of vibrationally excited OH radicals are insignificant and give confidence in the values of k 1 obtained in this work.…”

Section: Resultssupporting

confidence: 81%

The atmospheric chemistry of sulphuryl fluoride, SO2F2

2008

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Abstract.The atmospheric chemistry of sulphuryl fluoride, SO 2 F 2 , was investigated in a series of laboratory studies.A competitive rate method, using pulsed laser photolysis (PLP) to generate O( 1 D) coupled to detection of OH by laser induced fluorescence (LIF), was used to determine the overall rate coefficient for the reaction O( 1 D)+SO 2 F 2 →products (R1) of k 1 (220-300 K) = (1.3±0.2) × 10 −10 cm 3 molecule −1 s −1 . Monitoring the O( 3 P) product (R1a) enabled the contribution (α) of the physical quenching process (in which SO 2 F 2 is not consumed) to be determined as α (225-296 K)=(0.55±0.04). Separate, relative rate measurements at 298 K provided a rate coefficient for reactive loss of O( 1 D), k 1b , of (5.8 ± 0.8) × 10 −11 cm 3 molecule −1 s −1 in good agreement with the value calculated from (1−α)×k 1 =(5.9±1.0)×10 −11 cm 3 molecule −1 s −1 . Upper limits for the rate coefficients for reaction of SO 2 F 2 with OH (R2, using PLP-LIF), and with O 3 (R3, static reactor) were determined as k 2 (294 K)<1×10 −15 cm 3 molecule −1 s −1 and k 3 (294 K)<1×10 −23 cm 3 molecule −1 s −1 . In experiments using the wetted-wall flow tube technique, no loss of SO 2 F 2 onto aqueous surfaces was observed, allowing an upper limit for the uptake coefficient of γ (pH 2-12)<1×10 −7 to be determined. These results indicate that SO 2 F 2 has no significant loss processes in the troposphere, and a very long stratospheric lifetime. Integrated band intensities for SO 2 F 2 infrared absorption features between 6 and 19 µm were obtained, and indicate a significant global warming potential for this molecule. In the course of this work, ambient temperature rate coefficients for the reactions O( 1 D) with several important atmospheric species were deter-

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Section: Resultssupporting

confidence: 81%

The atmospheric chemistry of sulphuryl fluoride, SO2F2

2008

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“…As in several previous studies of Oð 1 DÞ reaction kinetics carried out in our laboratory (19,(22)(23)(24)(25)(26)(27)(28)(29), all experiments employed the LFP-RF technique with kinetic information obtained by monitoring the temporal behavior of ground state oxygen atoms, Oð 3 PÞ. An apparatus description (23) and an apparatus diagram (30) are published elsewhere.…”

Section: Methodsmentioning

confidence: 99%

“…An apparatus description (23) and an apparatus diagram (30) are published elsewhere. Only details that are specific to this study are discussed below.…”

Section: Methodsmentioning

confidence: 99%

Reactive and nonreactive quenching of O(¹D) by the potent greenhouse gases SO₂F₂, NF₃, and SF₅CF₃

Zhao

Laine

Nicovich

et al. 2010

Proc. Natl. Acad. Sci. U.S.A.

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A laser flash photolysis-resonance fluorescence technique has been employed to measure rate coefficients and physical vs. reactive quenching branching ratios for O( 1 D) deactivation by three potent greenhouse gases, SO 2 F 2 (k 1 ), NF 3 (k 2 ), and SF 5 CF 3 (k 3 ). In excellent agreement with one published study, we find that k 1 (T) ¼ 9.0 × 10 −11 exp ( þ 98∕T) cm 3 molecule −1 s −1 and that the reactive quenching rate coefficient is k 1b ¼ (5.8 AE 2.3) × 10 −11 cm 3 molecule −1 s −1 independent of temperature. We find that k 2 (T) ¼ 2.0 × 10 −11 exp ( þ 52∕T) cm 3 molecule −1 s −1 with reaction proceeding almost entirely (∼99%) by reactive quenching. Reactive quenching of O( 1 D) by NF 3 is more than a factor of two faster than reported in one published study, a result that will significantly lower the model-derived atmospheric lifetime and global warming potential of NF 3 . Deactivation of O( 1 D) by SF 5 CF 3 is slow enough (k 3 < 2.0 × 10 −13 cm 3 molecule −1 s −1 at 298 K) that reaction with O( 1 D) is unimportant as an atmospheric removal mechanism for SF 5 CF 3 . The kinetics of O( 1 D) reactions with SO 2 (k 4 ) and CS 2 (k 5 ) have also been investigated at 298 K. We find that k 4 ¼ (2.2 AE 0.3) × 10 −10 and k 5 ¼ (4.6 AE 0.6) × 10 −10 cm 3 molecule −1 s −1 ; branching ratios for reactive quenching are 0.76 AE 0.12 and 0.94 AE 0.06 for the SO 2 and CS 2 reactions, respectively. All uncertainties reported above are estimates of accuracy (2σ) and rate coefficients k i (T) (i ¼ 1; 2) calculated from the above Arrhenius expressions have estimated accuracies of AE15% (2σ).atmosphere | chemistry | climate | kinetics

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“…The rate constant recommendations are based on the absolute rate constants reported by Streit et al [1249], Davidson et al [353] and Davidson et al [352] 3 , and CO 2 ; by Amimoto et al [21], Amimoto et al [20], and Force and Wiesenfeld [467,468] [791,792] for H 2 O and O 2 ; by Gericke and Comes [491] for H 2 O; and by Shi and Barker [1180] for N 2 and CO 2, by Talukdar and Ravishankara [1289] for H 2 , by Dunlea and Ravishankara [419] or N 2 , O 2 , O 3 , CO 2 , N 2 O, and H 2 O; by Strekowski et al [1253] for N 2 and O 2 , and by Blitz et al for N 2 , O 2 , N 2 O, CH 4 , H 2 , and CO 2 [153]. Measurements for other reactions are specifically cited in the notes for those reactions.…”

Section: Notes Tomentioning

confidence: 99%

Environmental effects of large igneous province magmatism: a Siberian perspective

Black

Lamarque

Shields

et al. 2015

Volcanism and Global Environmental Change

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Temperature-dependent kinetics study of the reactions of O(1D2) with N2 and O2

Cited by 24 publications

References 56 publications

The atmospheric chemistry of sulphuryl fluoride, SO<sub>2</sub>F<sub>2</sub>

The atmospheric chemistry of sulphuryl fluoride, SO<sub>2</sub>F<sub>2</sub>

Reactive and nonreactive quenching of O(¹D) by the potent greenhouse gases SO₂F₂, NF₃, and SF₅CF₃

Environmental effects of large igneous province magmatism: a Siberian perspective

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Temperature-dependent kinetics study of the reactions of O(1D2) with N2 and O2

Cited by 24 publications

References 56 publications

The atmospheric chemistry of sulphuryl fluoride, SO&lt;sub&gt;2&lt;/sub&gt;F&lt;sub&gt;2&lt;/sub&gt;

The atmospheric chemistry of sulphuryl fluoride, SO&lt;sub&gt;2&lt;/sub&gt;F&lt;sub&gt;2&lt;/sub&gt;

Reactive and nonreactive quenching of O(1D) by the potent greenhouse gases SO2F2, NF3, and SF5CF3

Environmental effects of large igneous province magmatism: a Siberian perspective

Contact Info

Product

Resources

About

The atmospheric chemistry of sulphuryl fluoride, SO<sub>2</sub>F<sub>2</sub>

The atmospheric chemistry of sulphuryl fluoride, SO<sub>2</sub>F<sub>2</sub>

Reactive and nonreactive quenching of O(¹D) by the potent greenhouse gases SO₂F₂, NF₃, and SF₅CF₃