Implementation and refinement of a surface model for heterogeneous HONO formation in a 3-D chemical transport model

Karamchandani, Prakash; Emery, Chris; Yarwood, Greg; Lefer, B. L.; Stutz, J.; Couzo, Evan; Vizuete, William

doi:10.1016/j.atmosenv.2015.01.046

Cited by 14 publications

(17 citation statements)

References 79 publications

(106 reference statements)

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“…The maximum ratio of 1.73% in this study is comparable to the value of 1.7 % in Houston, Texas, observed by Rappenglück et al (2013). The derived emission ratios were within the range of other published results (0.19 %-2.1 %) (Kirchstetter et al, 1996;Kurtenbach et al, 2001;Su et al, 2008a;Rappengluck et al, 2013;Yang et al, 2014;Xu et al, 2015;Trinh et al, 2017;Liang et al, 2017;Zhang et al, 2018;. Comparisons of the derived HONO/NO x ratios with the results obtained previously are summarized in Table S2.…”

Section: Direct Emissionssupporting

confidence: 89%

“…S9), indicating the potential effect of direct emissions on the observed HONO at night. The emission ratio of HONO/NO x has been determined from tunnel measurements in California (Kirchstetter et al, 1996), Germany (Kurtenbach et al, 2001, and Hong Kong (Liang et al, 2017). However, considering the differences in the type of vehicles, fuel compositions, and other factors, the reported emission factor of HONO/NO x might not be representative for the Beijing region.…”

Section: Direct Emissionsmentioning

confidence: 99%

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High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

et al. 2020

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Abstract. Nitrous acid (HONO), an important precursor of the hydroxyl radical (OH), plays a key role in atmospheric chemistry, but its sources are still debated. The production of HONO on aerosol surfaces or on ground surfaces in nocturnal atmospheres remains controversial. The vertical profile provides vertical information on HONO and NO2 to understand the nocturnal HONO production and loss. In this study, we report the first high-resolution (<2.5 m) nocturnal vertical profiles of HONO and NO2 measured from in situ instruments on a movable container that was lifted on the side wiring of a 325 m meteorological tower in Beijing, China. High-resolution vertical profiles revealed the negative gradients of HONO and NO2 in nocturnal boundary layers, and a shallow inversion layer affected the vertical distribution of HONO. The vertical distribution of HONO was consistent with stratification and layering in the nocturnal urban atmosphere below 250 m. The increase in the HONO ∕ NO2 ratio was observed throughout the column from the clean episode to the haze episode, and relatively constant HONO∕NO2 ratios in the residual layer were observed during the haze episode. Direct HONO emissions from traffic contributed 29.3 % ± 12.4 % to the ambient HONO concentrations at night. The ground surface dominates HONO production by heterogeneous uptake of NO2 during clean episodes. In contrast, the HONO production on aerosol surfaces (30–300 ppt) explained the observed HONO increases (15–368 ppt) in the residual layer, suggesting that the aerosol surface dominates HONO production aloft during haze episodes, while the surface production of HONO and direct emissions into the overlying air are minor contributors. Average dry deposition rates of 0.74±0.31 and 1.55±0.32 ppb h−1 were estimated during the clean and haze episodes, respectively, implying that significant quantities of HONO could be deposited to the ground surface at night. Our results highlight the ever-changing contributions of aerosol and ground surfaces in nocturnal HONO production at different pollution levels and encourage more vertical gradient observations to evaluate the contributions from varied HONO sources.

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Section: Direct Emissionssupporting

confidence: 89%

Section: Direct Emissionsmentioning

confidence: 99%

High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

et al. 2020

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“…Investigators have proposed hydrolysis of NO2 on the humid aerosol surfaces, heterogeneous conversion of NO2 on ground surfaces, photolysis of NO3 -, catalytical formation on soot particles and acid displacement process in the atmosphere during the past several years (Stemmler et al, 2006;Karamchandani et al, 2015;VandenBoer et al, 2015;Tong et al, 2016;Ye et al, 2016;Ye et al, 2017;Lu et al, 2018;Xu et al, 2018b;Gen et al, 2019;Zhang et al, 2019d). Xue et al (2020) and Liu et al (2019) recently measured summertime atmospheric HONO concentrations in a rural area in China and performed simulations using a box model with updated chemical reactions for HONO production published in the literature.…”

Section: Heterogeneous Hono Chemistrymentioning

confidence: 99%

Improving the representation of HONO chemistry in CMAQ and examining its impact on haze over China

Zhang

Sarwar

Xing

et al. 2021

Preprint

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Abstract. We compare Community Multiscale Air Quality (CMAQ) model predictions with measured nitrous acid (HONO) concentrations in Beijing, China for December 2015. The model with the existing HONO chemistry in CMAQ severely under-estimates the observed HONO concentrations with a normalized mean bias of −97 %. We revise the HONO chemistry in the model by implementing six additional heterogeneous reactions in the model: reaction of nitrogen dioxide (NO2) on ground surfaces, reaction of NO2 on aerosol surfaces, reaction of NO2 on soot surfaces, photolysis of aerosol nitrate, nitric acid displacement reaction, and hydrochloric acid displacement reaction. The model with the revised chemistry substantially increases HONO predictions and improves the comparison with observed data with a normalized mean bias of −5 %. The photolysis of HONO enhances day-time hydroxyl radical by almost a factor of two. The enhanced hydroxyl radical concentrations compare favorably with observed data and produce additional sulfate via the reaction with sulfur dioxide, aerosol nitrate via the reaction with nitrogen dioxide, and secondary organic aerosols via the reactions with volatile organic compounds. The additional sulfate stemming from revised HONO chemistry improves the comparison with observed concentration; however, it does not close the gap between model prediction and the observation during polluted days.

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“…The unexplained daytime HONO is usually attributed to the light-enhanced NO2 heterogeneous reactions (R6 and R7) (George et al, 2016;Karamchandani et al, 2015;Sörgel et al, 2011). In addition, the daytime HONO can also be produced via the photolysis of particulate nitrates or absorbed nitric acid on surfaces of ground or leaves (R8) (Kasibhatla et al, 2018;Laufs and Kleffmann, 2016;Oswald et al, 2015;Sörgel et al, 2015;Zhou et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

Nitrous acid in marine boundary layer over eastern Bohai Sea, China: Characteristics, sources, and implications

Wen

Chen

Zheng

et al. 2019

Science of The Total Environment

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Nitrous acid (HONO) serves as a key source of hydroxyl radicals and plays important roles in atmospheric photochemistry. In this study, gaseous HONO and related species and parameters were measured in autumn of 2016 at a marine background site on Tuoji Island in eastern Bohai Sea, China. The HONO concentration in marine boundary layer (MBL) was on average 0.20±0.20 ppbv (average ± standard deviation) with a maximum hourly value of 1.38 ppbv. It exhibited distinct diurnal variations featuring with elevated concentrations in the late night and frequent concentration peaks in the early afternoon. During nighttime, the HONO was produced at a fast rate with the NO2-HONO 2 conversion rate ranging from 0.006 to 0.036 h-1. The fast HONO production and the strong dependence of temperature implied the enhancement of nocturnal HONO formation caused by air-sea interactions at high temperature. At daytime, HONO concentration peaks were frequently observed between 13:00-15:00. The observed daytime HONO concentrations were substantially higher than those predicted in the photostationary state in conditions of intensive solar radiation and high temperature. Strong or good correlations between the missing HONO production rate and temperature or photolysis frequency suggest a potential source of HONO from the photochemical conversions of nitrogen-containing compounds in sea microlayer. The source intensity strengthened quickly when the temperature was high. The abnormally high concentrations of daytime HONO contributed a considerable fraction to the primary OH radicals in the MBL.

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Implementation and refinement of a surface model for heterogeneous HONO formation in a 3-D chemical transport model

Cited by 14 publications

References 79 publications

High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

Improving the representation of HONO chemistry in CMAQ and examining its impact on haze over China

Nitrous acid in marine boundary layer over eastern Bohai Sea, China: Characteristics, sources, and implications

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Implementation and refinement of a surface model for heterogeneous HONO formation in a 3-D chemical transport model

Cited by 14 publications

References 79 publications

High-resolution vertical distribution and sources of HONO and NO&lt;sub&gt;2&lt;/sub&gt; in the nocturnal boundary layer in urban Beijing, China

High-resolution vertical distribution and sources of HONO and NO&lt;sub&gt;2&lt;/sub&gt; in the nocturnal boundary layer in urban Beijing, China

Improving the representation of HONO chemistry in CMAQ and examining its impact on haze over China

Nitrous acid in marine boundary layer over eastern Bohai Sea, China: Characteristics, sources, and implications

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Product

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High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

High-resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China