2 research outputs found
Constraining the budget of NOx and volatile organic compounds at a remote tropical island using multi-platform observations and WRF-Chem model simulations
No full textVolatile organic compounds (VOCs) act as precursors to ozone and secondary organic aerosols, which have significant health and environmental impacts. They can also reduce the atmospheric oxidative capacity. However, their budget remains poorly quantified, especially over remote areas such as the tropical oceans. Here, we present high-resolution simulations of atmospheric composition over Réunion Island, located in the Indian Ocean, using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The coexistence and spatial heterogeneity of anthropogenic and biogenic emission sources in this region present a valuable but challenging test of the model performance. The WRF-Chem model is evaluated against several observational datasets, including proton transfer reaction mass spectrometry (PTR-MS) measurements of VOCs and oxygenated VOCs (OVOCs) at the Maïdo Observatory, Réunion Island (2160 m above sea level), in January and July 2019, representing austral summer and winter, respectively, and capturing the seasonal extremes for the region. While the primary goal of our study is to gain a better understanding of the (O)VOC budget at remote tropical latitudes, important model refinements have been made to improve the model performance, including the implementation of high-resolution anthropogenic and biogenic isoprene emissions, updates to the chemical mechanism, and adjustments to the boundary conditions. These refinements are supported by comparisons with PTR-MS data as well as with meteorological measurements at Maïdo; in situ NOx and O3 measurements from the air quality Atmo-Réunion network; Fourier transform infrared spectroscopy (FTIR) measurements of O3, CO, ethane, and several OVOCs, also at Maïdo; and satellite retrievals from the TROPOspheric Monitoring Instrument (TROPOMI). TROPOMI NO2 data suggest that anthropogenic emissions, particularly from power plants near Le Port, dominate NOx levels over the island. Both TROPOMI and in situ surface NO2 comparisons are used to adjust the power plant emissions at Le Port. Surface ozone concentrations are overestimated by ∼6 ppbv on average, likely due to the neglect of halogen chemistry in the model, though other factors may also contribute. While modelled NO2 over oceans is too low in summer when the lightning source is excluded, including this source results in model overestimations, as corroborated by comparisons with upper tropospheric NO2 mixing ratios derived from TROPOMI using the cloud-slicing technique (Marais et al., 2021). The model generally succeeds in reproducing the PTR-MS isoprene and its oxidation products (Iox), except for a moderate underestimation (∼30 %) of noontime isoprene concentrations, and modelled concentration peaks near dawn and dusk, which are not seen in the observations. The ratio of Iox to isoprene (0.8 at noon in January) is fairly well reproduced by the model. The methanol and monoterpenes observations both suggest overestimations of their biogenic emissions, by factors of about 2 and 5, respectively. Acetaldehyde anthropogenic emissions are likely strongly overestimated, due to the lumping of higher aldehydes into this compound. Without this lumping, the modelled acetaldehyde would be underestimated by almost one order of magnitude, suggesting the existence of a large missing source, likely photochemical. The comparisons suggest the existence of a biogenic source of methyl ethyl ketone (MEK), equivalent to about 3 % of isoprene emissions, likely associated with the dry deposition and conversion of key isoprene oxidation products to MEK. A strong model underestimation of the PTR-MS signal at mass 61 is also found, by a factor of 3–5 during daytime, consistent with previously reported missing sources of acetic and peracetic acid
Top-Down Evaluation of Volatile Chemical Product Emissions Using a Lagrangian Framework
No full textIn this study, we evaluate volatile chemical product (VCP; e.g., adhesives, personal care products) emissions in the McDonald et al. inventory using sector-specific tracers and the FLEXPART-WRF Lagrangian particle dispersion model. Observations of decamethylcyclopentasiloxane (D5-Siloxane) are used for optimizing emissions from personal care products, para-dichlorobenzene (PDCBZ) for insecticides, and parachlorobenzotrifluoride (PCBTF) for emissions from the construction (coatings + adhesives) subsector. Continuous ground-site measurements obtained in Las Vegas and Los Angeles (LA) during summer 2021 are used to optimize the temporal emission profiles of the area sources. Additionally, in situ aircraft-based observations (June 2021) over the LA region are used to evaluate emission factors for the basin. The configuration of the weather research and forecasting (WRF) model is optimized using vertical wind profile measurements obtained from the Pick-Up truck-based Mobile Atmospheric Sounder (PUMAS) deployed in the LA basin to minimize the uncertainty of the inversion due to meteorology. While the diurnal amplitude in emission rates from personal care products and insecticides is reduced after optimization, that of construction VCPs (coatings + adhesives) is enhanced. From the aircraft inversion, we find that the inventory underestimates the emissions originating from construction by a factor of 5.3 (95% confidence interval 4.3–6.3) in the LA basin. Emissions from consumer products (personal care + cleaning) and insecticides were reduced by a factor of 2.1 (1.7–2.5) and 5.2 (3.9–6.4), respectively, following optimization. AB - In this study, we evaluate volatile chemical product (VCP; e.g., adhesives, personal care products) emissions in the McDonald et al. inventory using sector-specific tracers and the FLEXPART-WRF Lagrangian particle dispersion model. Observations of decamethylcyclopentasiloxane (D5-Siloxane) are used for optimizing emissions from personal care products, para-dichlorobenzene (PDCBZ) for insecticides, and parachlorobenzotrifluoride (PCBTF) for emissions from the construction (coatings + adhesives) subsector. Continuous ground-site measurements obtained in Las Vegas and Los Angeles (LA) during summer 2021 are used to optimize the temporal emission profiles of the area sources. Additionally, in situ aircraft-based observations (June 2021) over the LA region are used to evaluate emission factors for the basin. The configuration of the weather research and forecasting (WRF) model is optimized using vertical wind profile measurements obtained from the Pick-Up truck-based Mobile Atmospheric Sounder (PUMAS) deployed in the LA basin to minimize the uncertainty of the inversion due to meteorology. While the diurnal amplitude in emission rates from personal care products and insecticides is reduced after optimization, that of construction VCPs (coatings + adhesives) is enhanced. From the aircraft inversion, we find that the inventory underestimates the emissions originating from construction by a factor of 5.3 (95% confidence interval 4.3–6.3) in the LA basin. Emissions from consumer products (personal care + cleaning) and insecticides were reduced by a factor of 2.1 (1.7–2.5) and 5.2 (3.9–6.4), respectively, following optimization
