Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Methanol Interactions with Nopinone Surfaces during Phase Evolution

Version 1 : Received: 1 February 2021 / Approved: 2 February 2021 / Online: 2 February 2021 (13:08:44 CET)

How to cite: Kong, X.; Lovric, J.; Johansson, S.; Prisle, N.; Pettersson, J. Methanol Interactions with Nopinone Surfaces during Phase Evolution. Preprints 2021, 2021020087 (doi: 10.20944/preprints202102.0087.v1). Kong, X.; Lovric, J.; Johansson, S.; Prisle, N.; Pettersson, J. Methanol Interactions with Nopinone Surfaces during Phase Evolution. Preprints 2021, 2021020087 (doi: 10.20944/preprints202102.0087.v1).

Abstract

Organic-organic interactions play important roles in the secondary organic aerosol formation, but the interactions are complex and poorly understood. Here we use environmental molecular beam experiments combined with molecular dynamics simulations to investigate the interactions between methanol and nopinone, as atmospheric organic proxies. In the experiments, methanol monomers and clusters are sent to collide with three types of surfaces, i.e., graphite, thin nopinone coating on graphite and multilayer surfaces, at temperatures between 140 K and 230 K. Methanol monomers are efficiently scattered from the graphite surface, whereas the scattering is substantially suppressed from nopinone surfaces. The desorption from the three surfaces is similar, suggesting that all the surfaces have weak or similar influences on the methanol desorption. The molecular dynamics results show that upon collisions the methanol clusters shatter, and the shattered fragments quickly diffuse and recombine to clusters. The desorption involves a series of processes, including detaching from clusters and desorbing as monomers. The experimental results also show that all trapped methanol molecules completely desorb within a short experimental time scale at temperatures of 180 K and above. At lower temperatures, the desorption rate decreases, and a long experimental time scale is used to resolve the desorption, where three desorption components are identified. The fast component is beyond the experimental detection limit. The intermediate component exhibits multi-step desorption character and has an activation energy of Ea = 0.18 ± 0.03 eV, in good agreement with simulation results. The slow desorption component is related to diffusion processes due to the weak temperature dependence.

Subject Areas

Environmental molecular beam; molecular dynamics; phase transition; secondary organic aerosol; sorption kinetics

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