Reply to the ‘Comment on “Enhancement in the production of nucleating clusters due to dimethylamine and large uncertainties in the thermochemistry of amine-enhanced nucleation”’ by Kupiainen-Maatta et al.

Nadykto, Alexey B.; Herb, Jason; Yu, Fangqun; Nazarenko, Ekaterina S.; Xu, Yisheng

doi:10.1016/j.cplett.2015.01.028

Cited by 13 publications

(17 citation statements)

References 23 publications

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“…28 Only recently, simulations involving hydrated clusters using their Gibbs free energies in the system of sulfuric acid and dimethylamine were carried out to provide predicted particle formation rates for comparison to observed ones. 74,77,78 Calculation of free energies for all relevant hydrated clusters up to a reasonable size for incorporation into a ''birth-death equations'' model is not feasible for the MSA-TMA-H 2 O system at the …”

Section: Proposed Kinetics Schemementioning

confidence: 99%

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Chen

Ezell

Arquero

et al. 2015

Phys. Chem. Chem. Phys.

110

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New particle formation from gas-to-particle conversion represents a dominant source of atmospheric particles and affects radiative forcing, climate and human health. The species involved in new particle formation and the underlying mechanisms remain uncertain. Although sulfuric acid is commonly recognized as driving new particle formation, increasing evidence suggests the involvement of other species. Here we study particle formation and growth from methanesulfonic acid, trimethylamine and water at reaction times from 2.3 to 32 s where particles are 2-10 nm in diameter using a newly designed and tested flow system. The flow system has multiple inlets to facilitate changing the mixing sequence of gaseous precursors. The relative humidity and precursor concentrations, as well as the mixing sequence, are varied to explore their effects on particle formation and growth in order to provide insight into the important mechanistic steps. We show that water is involved in the formation of initial clusters, greatly enhancing their formation as well as growth into detectable size ranges. A kinetics box model is developed that quantitatively reproduces the experimental data under various conditions. Although the proposed scheme is not definitive, it suggests that incorporating such mechanisms into atmospheric models may be feasible in the near future.

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Section: Proposed Kinetics Schemementioning

confidence: 99%

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Chen

Ezell

Arquero

et al. 2015

Phys. Chem. Chem. Phys.

110

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“…14,15,17,18,20,21 The abundance of the bimolecular complexes is directly proportional to K, and the calculated range (∼2−9 kJ/mol) would lead to a 16-fold variation in K, which may result in qualitatively different conclusions with respect to the composition and growth of atmospheric clusters. 11,12 In humid conditions (100% relative humidity) at a temperature of 296 K, our determined equilibrium constants suggest that ∼0.5% of DMA and TMA molecules in the atmosphere are bound to H 2 O.…”

Section: ■ Results and Discussionmentioning

confidence: 87%

“…10 The role and importance of H 2 O in nucleation are discussed largely based on theoretical approaches. 11,12 The growth process of aerosols is dictated by the Gibbs energy of the process and the atmospheric abundance of the respective molecules.…”

Section: ■ Introductionmentioning

confidence: 99%

Room Temperature Gas-Phase Detection and Gibbs Energies of Water Amine Bimolecular Complex Formation

et al. 2020

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We have detected the H2O·DMA and H2O·TMA (DMA, dimethylamine; TMA, trimethylamine) bimolecular complexes at room temperature in the gas phase using Fourier transform infrared spectroscopy. For both complexes, five vibrational bands associated with the H2O molecule are observed and assigned. Within a reduced dimensional local mode framework, we set up a six-dimensional model, including the three H2O vibrational modes and three of the six intermolecular modes, all described with internal curvilinear coordinates. The single points on the potential energy surface and Eckart corrected dipole moment surface are calculated with the CCSD(T)-F12a/cc-pVDZ-F12 method. Combining the measured and calculated transition intensities, we determine the Gibbs energy of complex formation of both complexes from each of the observed bands. The multiple determinations give similar Gibbs energies, for each complex, and increase the confidence in the combined experimental and theoretical approach, and improve the accuracy of the determined Gibbs energies. The average Gibbs energies of complex formation are found to be 5.0 ± 0.2 and 3.8 ± 0.2 kJ/mol for H2O·DMA and H2O·TMA, respectively. In addition to the experimental uncertainty, there is a potential error on the calculated intensities corresponding to 0.4 kJ/mol. However, the small spread among the four determinations suggests that this error is even less. The Gibbs energies of these complexes serve as accurate benchmarks for theoretical approaches that are prevalent in hydrogen bonding and nucleation studies.

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“…18 The amino group of amide can strongly bond with SA that enhances the formation of SA-containing pre-nucleation clusters, and, thus promotes NPF. 19,20 Zhao et al conducted a quantum chemistry study on the molecular interactions between some amides and methanol clusters 21 and showed that the formation free energies of the clusters were strongly negative.…”

Section: Introductionmentioning

confidence: 99%

Propionamide participating in H₂SO₄-based new particle formation: a theory study

Zhao

Zuo

et al. 2021

RSC Adv.

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Reply to the ‘Comment on “Enhancement in the production of nucleating clusters due to dimethylamine and large uncertainties in the thermochemistry of amine-enhanced nucleation”’ by Kupiainen-Maatta et al.

Cited by 13 publications

References 23 publications

New particle formation and growth from methanesulfonic acid, trimethylamine and water

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Room Temperature Gas-Phase Detection and Gibbs Energies of Water Amine Bimolecular Complex Formation

Propionamide participating in H₂SO₄-based new particle formation: a theory study

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Reply to the ‘Comment on “Enhancement in the production of nucleating clusters due to dimethylamine and large uncertainties in the thermochemistry of amine-enhanced nucleation”’ by Kupiainen-Maatta et al.

Cited by 13 publications

References 23 publications

New particle formation and growth from methanesulfonic acid, trimethylamine and water

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Room Temperature Gas-Phase Detection and Gibbs Energies of Water Amine Bimolecular Complex Formation

Propionamide participating in H2SO4-based new particle formation: a theory study

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Propionamide participating in H₂SO₄-based new particle formation: a theory study