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Nitric Acid–Amine Chemistry in the Gas Phase and at the Air–Water Interface
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    Nitric Acid–Amine Chemistry in the Gas Phase and at the Air–Water Interface
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 20, 6456–6466
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    https://doi.org/10.1021/jacs.8b03300
    Published April 24, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    Gas-phase simulations of nitric acid–amine chemistry suggest that the fundamental acid–base interaction between HNO3 and NH3 results in a variety of HNO3–NH3-based complexes, such as (HNO3)3·(NH3)2, (HNO3)3·(NH3)3, and (HNO3)4·(NH3)3, that can be formed. The formation of these complexes in the gas phase follow different growth mechanisms under different relative humidity conditions. On the other hand, at the air–water interface, Born–Oppenheimer molecular dynamics simulations suggest that the formation of the fundamental NO3··(R1)(R2)NH2+ [for NH3, R1 = R2 = H; CH3NH2, R1 = H, R2 = CH3; and (CH3)2NH, R1 = R2 = CH3] ion pairs require the formation of the HNO3··(R1)(R2)NH complexes in the gas-phase prior to their adsorption on the water surface. Ion-pair formation at the water surface involves proton transfer from HNO3 to (R1)(R2)NH and occurs within a few femtoseconds of the simulation. The NO3··(R1)(R2)NH2+ ion pairs preferentially remain at the interface over the picosecond time scale, where they are stabilized via hydrogen bonding with surface water molecules. This offers a novel chemical framework for understanding gas-to-particle partitioning in the atmosphere. These results not only improve our understanding of the formation of nitrate particulates in polluted urban environments, but also provide useful guidelines for understanding particle formation in forested or coastal environments, in which organic acids and organosulfates are present in significant quantities and their exact role in particle formation remains elusive.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b03300.

    • Tables S1–S4, listing optimized geometries of key species involved in the particle formation in the gas phase and giving flux information regarding the nitric acid–ammonia-based particle formation in the gas phase (PDF)

    • Movie S1, trajectories of the BOMD simulation for the HNO3–NH3 reaction at air–water interface (MPG)

    • Movie S2, trajectories of the BOMD simulation for the HNO3–CH3NH2 reaction at air–water interface (MPG)

    • Movie S3, trajectories of the BOMD simulation for the HNO3–(CH3)2NH reaction at air–water interface (MPG)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 20, 6456–6466
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.8b03300
    Published April 24, 2018
    Copyright © 2018 American Chemical Society

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