Kinetic Study of Ni and NiO Reactions Pertinent to the Earth’s Upper Atmosphere

Mangan, Thomas P.; McAdam, N. T.; Daly, Shane; Plane, J. M. C.

doi:10.1021/acs.jpca.8b11382

Cited by 15 publications

(26 citation statements)

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“…A satisfactory fit of the model to the experimental data is obtained with k 5 (294 K) = (3.0 ± 0.5) × 10 −11 cm 3 molecule −1 s −1 , illustrated in Figure 2. This value is in very good agreement with the only previous study of R5 by Mangan et al (2019) using the pulsed laser photolysis‐laser induced fluorescence (PLP‐LIF) technique in a slow flow reactor, which reported k 5 (190–377 K) = (3.2 ± 0.6) × 10 −11 ( T /200) −0.19 ± 0.05 cm 3 molecule −1 s −1 , that is, k 5 (294 K) = (3.0 ± 0.6) × 10 −11 cm 3 molecule −1 s −1 .…”

Section: Underpinning Laboratory and Theoretical Worksupporting

confidence: 93%

“…The experimental points are shown in Figure 2. The recycling of Ni was modeled by applying the rate coefficients and branching ratios for Ni and NiO reacting with O 2 and O 3 (i.e., , , , and ) determined previously (Mangan et al, 2019). A satisfactory fit of the model to the experimental data is obtained with k 5 (294 K) = (3.0 ± 0.5) × 10 −11 cm 3 molecule −1 s −1 , illustrated in Figure 2.…”

Section: Underpinning Laboratory and Theoretical Workmentioning

confidence: 99%

“…We have also recently carried out a series of kinetic studies of the relevant neutral (Mangan et al, 2019) and ion‐molecule (Bones et al, 2020) chemistry of the metal. Figure 1 illustrates the reactions connecting neutral Ni species (green boxes) and ionized species (blue boxes).…”

Section: Introductionmentioning

confidence: 99%

“…Figure 1 illustrates the reactions connecting neutral Ni species (green boxes) and ionized species (blue boxes). In the MLT, Ni is oxidized by O 3 and O 2 (Mangan et al, 2019):

Ni + O_{3} \to NiO + O_{2}

Ni + O_{2} ()(, + normalM) \to {NiO}_{2}, where normalM = N_{2} or O_{2}

NiO + O_{3} \to {NiO}_{2} + O_{2}

\to Ni + {2O}_{2}

By analogy with other meteoric metals (Plane et al, 2015), the resulting oxides are then likely to be reduced back to Ni by O and CO (red arrows in Figure 1):

NiO + normalO \to Ni + O_{2}

NiO + CO \to Ni + {CO}_{2}

{NiO}_{2} + normalO \to NiO + O_{2}

…”

Section: Introductionmentioning

confidence: 99%

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The Meteoric Ni Layer in the Upper Atmosphere

et al. 2020

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The first global atmospheric model of Ni (WACCM‐Ni) has been developed to understand recent observations of the mesospheric Ni layer by ground‐based resonance lidars. The three components of the model are: the Whole Atmospheric Community Climate Model (WACCM6); a meteoric input function derived by coupling an astronomical model of dust sources in the solar system with a chemical meteoric ablation model; and a comprehensive set of neutral, ion‐molecule, and photochemical reactions pertinent to the chemistry of Ni in the upper atmosphere. In order to achieve closure on the chemistry, the reaction kinetics of three important reactions were first studied using a fast flow tube with pulsed laser ablation of a Ni target, yielding k(NiO + O) = (4.6 ± 1.4) × 10−11, k(NiO + CO) = (3.0 ± 0.5) × 10−11, and k(NiO2 + O) = (2.5 ± 1.2) × 10−11 cm3 molecule−1 s−1 at 294 K. The photodissociation rate of NiOH was computed to be J(NiOH) = 0.02 s−1. WACCM‐Ni simulates satisfactorily the observed neutral Ni layer peak height and width, and Ni+ measurements from rocket‐borne mass spectrometry. The Ni layer is predicted to have a similar seasonal and latitudinal variation as the Fe layer, and its unusually broad bottom‐side compared with Fe is caused by the relatively fast NiO + CO reaction. The quantum yield for photon emission from the Ni + O3 reaction, observed in the nightglow, is estimated to be between 6% and 40%.

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Section: Underpinning Laboratory and Theoretical Worksupporting

confidence: 93%

Section: Underpinning Laboratory and Theoretical Workmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

“…Figure 1 illustrates the reactions connecting neutral Ni species (green boxes) and ionized species (blue boxes). In the MLT, Ni is oxidized by O 3 and O 2 (Mangan et al, 2019):

Ni + O_{3} \to NiO + O_{2}

Ni + O_{2} ()(, + normalM) \to {NiO}_{2}, where normalM = N_{2} or O_{2}

NiO + O_{3} \to {NiO}_{2} + O_{2}

\to Ni + {2O}_{2}

By analogy with other meteoric metals (Plane et al, 2015), the resulting oxides are then likely to be reduced back to Ni by O and CO (red arrows in Figure 1):

NiO + normalO \to Ni + O_{2}

NiO + CO \to Ni + {CO}_{2}

{NiO}_{2} + normalO \to NiO + O_{2}

…”

Section: Introductionmentioning

confidence: 99%

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The Meteoric Ni Layer in the Upper Atmosphere

et al. 2020

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“…However, taking a recently measured rate coefficient k(Ni + O 3 → NiO + O 2 ) = (6.5 ± 0.7)·10 −10 cm 3 per molecule per second (Mangan et al, 2018) and a typical O 3 concentration at 85 km of 5 · 10 8 cm −3 , the e-folding time for Ni conversion to NiO will be ∼3.1 s. During this time, the Ni atom will experience on the order of 10 5 collisions with air molecules and, given that the separation of the 3 D and 3 F states is only 204.8 cm −1 , it is very likely that these states will be fully equilibrated. This is the first example of a metal resonance lidar where this is the case.…”

Section: Discussionmentioning

confidence: 99%

Lidar Soundings of the Mesospheric Nickel Layer Using Ni(³F) and Ni(³D) Transitions

Gerding

Daly

Plane

2019

Geophysical Research Letters

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During six nights between January and March 2018 we observed the mesospheric Ni layer by lidar from Kühlungsborn, Germany (54°N, 12°E). For most of the soundings we utilized for the first time a transition from the low‐lying excited Ni(3D) state at 341 nm. For additional soundings we used the ground‐state Ni(3F) transition at 337 nm, giving similar results but a worse signal‐to‐noise ratio. We observed nightly mean Ni peak densities between ∼280 and 450 cm−3 and column abundances between 3.1·108 and 4.9·108 cm−2. Comparing with iron densities we get a Fe/Ni ratio of 38, which is a factor of 2 larger than the ratio in CI chondrites and factor of 32 larger than the Fe/Ni ratio observed by the only previous measurement of mesospheric Ni (Collins et al., 2015, https://doi.org/10.1002/2014GL062716). The underabundance of Ni compared to CI chondrites suggests that Ni is more efficiently sequestered as Ni+ or neutral reservoir species than Fe.

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Kinetic Study of Ni and NiO Reactions Pertinent to the Earth’s Upper Atmosphere

Abstract: This is a repository copy of Kinetic Study of Ni and NiO Reactions Pertinent to the Earth's Upper Atmosphere.

Cited by 15 publications

References 33 publications

The Meteoric Ni Layer in the Upper Atmosphere

The Meteoric Ni Layer in the Upper Atmosphere

Lidar Soundings of the Mesospheric Nickel Layer Using Ni(³F) and Ni(³D) Transitions

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Kinetic Study of Ni and NiO Reactions Pertinent to the Earth’s Upper Atmosphere

Abstract: This is a repository copy of Kinetic Study of Ni and NiO Reactions Pertinent to the Earth's Upper Atmosphere.

Cited by 15 publications

References 33 publications

The Meteoric Ni Layer in the Upper Atmosphere

The Meteoric Ni Layer in the Upper Atmosphere

Lidar Soundings of the Mesospheric Nickel Layer Using Ni(3F) and Ni(3D) Transitions

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Contact Info

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Lidar Soundings of the Mesospheric Nickel Layer Using Ni(³F) and Ni(³D) Transitions