Heterogeneous reactivity of nitrous acid on submicron sulfuric acid aerosol

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发布日期
DOI 10.1039/A808702D
影响因子 3.676
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摘要

An aerosol flow reactor has been employed to study nitrous acid decomposition (2HONO→NO+NO2+H2O) on submicron sulfuric acid aerosol. The reactive uptake coefficient was obtained for 60 wt.% sulfuric acid at room temperature and pressure. It was found to be linearly dependent upon the nitrous acid partial pressure with γr≈pHONO(ppb)×10-8. The bulk-liquid phase reaction rate constant was measured in a separate experiment and a value of kII=(19.5±2.0) d mol-1 s-1 was obtained for 60 wt.% sulfuric acid at room temperature. This value is too small to explain the observed loss of HONO to the aerosol particles implying that the heterogeneous decay of nitrous acid occurs on the surface of the aerosol. A second-order surface rate constant of ksurf=(4.6±1.5)×10-17 cm3 m molecule-1 s-1 was determined that was a factor of a thousand greater than that previously reported for other surfaces. Despite this relatively large decay constant, it is still too small to have any significance upon nitrous acid concentrations in the night-time boundary layer. This work adds to the increasing number of heterogeneous reactions that are found to be significantly enhanced at the surface of a liquid.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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