Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics

Knopf, Daniel A.; Ammann, Markus; Berkemeier, Thomas; Pöschl, Ulrich; Shiraiwa, Manabu

doi:10.5194/acp-24-3445-2024

Title: Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics

Journal Article · 20 March 2024 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-24-3445-2024 · OSTI ID:2326090

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Stony Brook Univ., NY (United States)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Max Planck Institute for Chemistry, Mainz (Germany)
Univ. of California, Irvine, CA (United States)

Adsorption and desorption of gases on liquid or solid substrates are involved in multiphase processes and heterogeneous chemical reactions. The desorption energy ($$E_{des}^{0}$$), which depends on the intermolecular forces between adsorbate and substrate, determines the residence time of chemical species at interfaces. We show how $$E_{des}^{0}$$ and temperature influence the net uptake or release of gas species, the rates of surface–bulk exchange and surface or bulk reactions, and the equilibration timescales of gas–particle partitioning. Using literature data, we derive a parameterization to estimate $$E_{des}^{0}$$ for a wide range of chemical species based on the molecular mass, polarizability, and oxygen-to-carbon ratio of the desorbing species independent of substrate-specific properties, which is possible because of the dominant role of the desorbing species' properties. Correlations between $$E_{des}^{0}$$ and the enthalpies of vaporization and solvation are rooted in molecular interactions. The relation between $$E_{des}^{0}$$ and desorption kinetics reflects the key role of interfacial exchange in multiphase processes. For small molecules and semi-volatile organics (VOC, IVOC, SVOC), $$E_{des}^{0}$$ values around 10–100 kJ mol^-1 correspond to desorption lifetimes around nanoseconds to days at room temperature. Even higher values up to years are obtained at low temperatures and for low volatile organic compounds (LVOC, ELVOC/ULVOC) relevant for secondary organic aerosols (SOA). Implications are discussed for SOA formation, gas–particle partitioning, organic phase changes, and indoor surface chemistry. We expect these insights to advance the mechanistic and kinetic understanding of multiphase processes in atmospheric and environmental physical chemistry, aerosol science, materials science, and chemical engineering.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE

Contributing Organization:: Pacific Northwest National Laboratory (PNNL); Brookhaven National Laboratory (BNL); Argonne National Laboratory (ANL)

Grant/Contract Number:: SC0022139; AGS-1446286; AGS-2246502; AGS-1654104; 188662

OSTI ID:: 2326090

Alternate ID(s):: OSTI ID: 2336700

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 24, Issue 6; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: United States

Language:: English

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