Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

Gouw, J. A. de; Parrish, D. D.; Brown, Steven S.; Edwards, P. M.; Gilman, J. B.; Graus, M.; Hanisco, T. F.; Kaiser, Jennifer; Keutsch, Frank N.; Kim, Si‐Wan; Lerner, B. M.; Neuman, J. A.; Nowak, John B.; Pollack, I. B.; Roberts, J. M.; Ryerson, Thomas B.; Veres, P. R.; Warneke, C.; Wolfe, G. M.

doi:10.1029/2019gl083044

Cited by 11 publications

(9 citation statements)

References 53 publications

(67 reference statements)

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“…The above comparison supports the current model treatment of OH chemistry in the presence of isoprene. In particular, it argues against any substantial missing OH recycling at low NO x 10 , 12 , 32 —instead, the modeled OH levels are modestly higher than implied by the satellite data. A sensitivity analysis using the Mini-CIM 8 isoprene oxidation mechanism supports this conclusion ( Supplementary Note IV ; Supplementary Fig.…”

Section: Cris Isoprene: Links To Emissions Ohmentioning

confidence: 88%

Satellite isoprene retrievals constrain emissions and atmospheric oxidation

Wells

Millet

Payne

et al. 2020

Nature

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SUMMARY: Isoprene is the dominant non-methane organic compound emitted to the atmosphere 1 – 3 . It drives ozone and aerosol production, modulates atmospheric oxidation, and interacts with the global nitrogen cycle 4 – 8 . Isoprene emissions are highly uncertain 1 , 9 , as is the non-linear chemistry coupling isoprene and the hydroxyl radical, OH—its primary sink 10 – 13 . Here we present the first global isoprene measurements from space, using the Cross-track Infrared Sounder (CrIS). These isoprene measurements, together with observations of its oxidation product formaldehyde, provide new constraints on isoprene emissions and atmospheric oxidation. We find that isoprene:formaldehyde relationships measured from space are broadly consistent with current understanding of isoprene-OH chemistry, with no indication of missing OH recycling at low-NO x . We analyze these datasets over four global isoprene hotspots in relation to model predictions, and present a first demonstration of isoprene emission quantification based directly on satellite measurements of isoprene itself. A major discrepancy emerges over Amazonia, where current underestimates of natural NO x emissions bias modeled OH and hence isoprene. Over southern Africa, we find that a prominent isoprene hotspot is missing from bottom-up predictions. A multi-year analysis sheds light on interannual isoprene variability, and suggests the role of El Niño.

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Section: Cris Isoprene: Links To Emissions Ohmentioning

confidence: 88%

Satellite isoprene retrievals constrain emissions and atmospheric oxidation

Wells

Millet

Payne

et al. 2020

Nature

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“…Further, OH concentrations are expected to depend nonlinearly on NO x , which can vary in concentration in the crosswind dimension …”

Section: Introductionmentioning

confidence: 99%

“…12 Further, OH concentrations are expected to depend nonlinearly on NO x , which can vary in concentration in the crosswind dimension. 14 Entrainment of background O 3 , as well as photochemical production, can provide O 3 for plume oxidation near the plume edges. 15 Further, NO can depress O 3 at the plume center in freshly emitted plumes.…”

Section: ■ Introductionmentioning

confidence: 99%

Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke

Decker

Wang

Bourgeois

et al. 2021

Environ. Sci. Technol.

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We present a novel method, the Gaussian observational model for edge to center heterogeneity (GOMECH), to quantify the horizontal chemical structure of plumes. GOMECH fits observations of short-lived emissions or products against a long-lived tracer (e.g., CO) to provide relative metrics for the plume width (w i /w CO ) and center (b i /w CO ). To validate GOMECH, we investigate OH and NO 3 oxidation processes in smoke plumes sampled during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality, a 2019 wildfire smoke study). An analysis of 430 crosswind transects demonstrates that nitrous acid (HONO), a primary source of OH, is narrower than CO (w HONO /w CO = 0.73−0.84 ± 0.01) and maleic anhydride (an OH oxidation product) is enhanced on plume edges (w maleicanhydride /w CO = 1.06−1.12 ± 0.01). By contrast, NO 3 production [P(NO 3 )] occurs mainly at the plume center (w P(NO 3 ) /w CO = 0.91−1.00 ± 0.01). Phenolic emissions, highly reactive to OH and NO 3 , are narrower than CO (w phenol /w CO = 0.96 ± 0.03, w catechol /w CO = 0.91 ± 0.01, and w methylcatechol /w CO = 0.84 ± 0.01), suggesting that plume edge phenolic losses are the greatest. Yet, nitrophenolic aerosol, their oxidation product, is the greatest at the plume center (w nitrophenolicaerosol /w CO = 0.95 ± 0.02). In a large plume case study, GOMECH suggests that nitrocatechol aerosol is most associated with P(NO 3 ). Last, we corroborate GOMECH with a large eddy simulation model which suggests most (55%) of nitrocatechol is produced through NO 3 in our case study.

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“…This could translate to much higher ozone production in the SEUS, however NOxlimitation and lower OH concentrations depress ozone production rates compared to Southern California. In addition, the lower OH in the SEUS extends the isoprene lifetime, increasing the observed reactivity 59 . Finally, the SOA formation potential for all the ROC species measured in CalNex is almost twice that estimated for SOAS, largely driven by aromatics.…”

Section: Discussionmentioning

confidence: 92%

Contrasting Reactive Organic Carbon Observations in the Southeast United States (SOAS) and Southern California (CalNex)

Heald

Gouw

Goldstein

et al. 2020

Environ. Sci. Technol.

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Despite the central role of reactive organic carbon (ROC) in the formation of secondary species that impact global air quality and climate, our assessment of ROC abundance and impacts is challenged by the diversity of species that contribute to it. We re-visit measurements of ROC species made during two field campaigns in the United States: the 2013 SOAS campaign in forested Centreville, AL, and the 2010 CalNex campaign in urban Pasadena, CA. We find that average measured ROC concentrations are about twice as high in Pasadena (73.8 µgCsm -3 ) than in Centreville (36.5 µgCsm -3 ). However, the OH reactivity (OHR) measured at these sites is similar (20.1 and 19.3 s -1 ). The shortfall in OHR when summing up measured contributions is 31%, at Pasadena and 14% at Centreville, suggesting that there may be a larger reservoir of unmeasured ROC at the former site. Estimated O3 production and SOA potential (defined as concentration x yield) are both higher during CalNex than SOAS. This analysis suggests that the ROC in urban California is less reactive, but due to higher concentrations of oxides of nitrogen and hydroxyl radicals, is more efficient in terms of O3 and SOA production, than in the forested southeastern U.S. S1 with reaction rates, SOA yields and ROC mass concentrations, cOHR, and SOA potential for each species measured during SOAS and CalNex. Supporting Information: Table

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Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

Cited by 11 publications

References 53 publications

Satellite isoprene retrievals constrain emissions and atmospheric oxidation

Satellite isoprene retrievals constrain emissions and atmospheric oxidation

Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke

Contrasting Reactive Organic Carbon Observations in the Southeast United States (SOAS) and Southern California (CalNex)

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