Foliar uptake of atmospheric organic nitrates

Lockwood, A. L.; Filley, Timothy R.; Rhodes, David; Shepson, P. B.

doi:10.1029/2008gl034714

Cited by 41 publications

(45 citation statements)

References 47 publications

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“…The data demonstrate that organic nitrogen is an important fraction of the oxidized nitrogen dry deposition flux, similar to wet deposition (85). The organic nitrogen may be taken up by foliage (86,87) and incorporated into the synthesis of leaf nutrients. As the effects of organic nitrogen on carbon sequestration are inadequately represented in most ecological models, these data motivate further inquiry into the ecosystem ramifications of OVOC deposition.…”

Section: Resultsmentioning

confidence: 78%

Rapid deposition of oxidized biogenic compounds to a temperate forest

Nguyen

Crounse

Teng

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

247

433

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We report fluxes and dry deposition velocities for 16 atmospheric compounds above a southeastern United States forest, including: hydrogen peroxide (H 2 O 2 ), nitric acid (HNO 3 ), hydrogen cyanide (HCN), hydroxymethyl hydroperoxide, peroxyacetic acid, organic hydroxy nitrates, and other multifunctional species derived from the oxidation of isoprene and monoterpenes. The data suggest that dry deposition is the dominant daytime sink for small, saturated oxygenates. Greater than 6 wt %C emitted as isoprene by the forest was returned by dry deposition of its oxidized products. Peroxides account for a large fraction of the oxidant flux, possibly eclipsing ozone in more pristine regions. The measured organic nitrates comprise a sizable portion (15%) of the oxidized nitrogen input into the canopy, with HNO 3 making up the balance. We observe that water-soluble compounds (e.g., strong acids and hydroperoxides) deposit with low surface resistance whereas compounds with moderate solubility (e.g., organic nitrates and hydroxycarbonyls) or poor solubility (e.g., HCN) exhibited reduced uptake at the surface of plants. To first order, the relative deposition velocities of water-soluble compounds are constrained by their molecular diffusivity. From resistance modeling, we infer a substantial emission flux of formic acid at the canopy level (∼1 nmol m −2 ·s −1 ). GEOS−Chem, a widely used atmospheric chemical transport model, currently underestimates dry deposition for most molecules studied in this work. Reconciling GEOS−Chem deposition velocities with observations resulted in up to a 45% decrease in the simulated surface concentration of trace gases.biosphere−atmosphere exchange | isoprene | dry deposition | OVOCs | fluxes

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Section: Resultsmentioning

confidence: 78%

Rapid deposition of oxidized biogenic compounds to a temperate forest

Nguyen

Crounse

Teng

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

247

433

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“…The measured Henry's law coefficients of some of the more soluble individual hydroxy nitrates (∼ 10 3 -10 5 M atm −1 , Shepson et al, 1996;Treves et al, 2000) are orders of magnitude lower than that of HNO 3 (1 × 10 14 M atm −1 at pH ∼ 6.5, Seinfeld and Pandis, 2006). Still, these measured Henry's law coefficients of hydroxy nitrates indicate that wet deposition is a significant loss process and a recent study indicates that foliar uptake of organic nitrates is possible (Lockwood et al, 2008 Min, personal communication, 2012). Although the exact magnitude of the depositional loss likely depends on the specific composition of ANs, as well as the partitioning between gas and aerosol, we assume that a similar result exists for the boreal forest since recent measurements of speciated organic nitrates using chemical ionization mass spectrometry at the ponderosa pine forest (Beaver et al, 2012) indicate a similar composition of ANs as assumed here from the instantaneous production rate.…”

Section: Depositionmentioning

confidence: 65%

Observations of total RONO2 over the boreal forest: NOx sinks and HNO3 sources

et al. 2013

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Abstract. In contrast with the textbook view of remote chemistry where HNO3 formation is the primary sink of nitrogen oxides, recent theoretical analyses show that formation of RONO2 (ΣANs) from isoprene and other terpene precursors is the primary net chemical loss of nitrogen oxides over the remote continents where the concentration of nitrogen oxides is low. This then increases the prominence of questions concerning the chemical lifetime and ultimate fate of ΣANs. We present observations of nitrogen oxides and organic molecules collected over the Canadian boreal forest during the summer which show that ΣANs account for ~20% of total oxidized nitrogen and that their instantaneous production rate is larger than that of HNO3. This confirms the primary role of reactions producing ΣANs as a control over the lifetime of NOx (NOx = NO + NO2) in remote, continental environments. However, HNO3 is generally present in larger concentrations than ΣANs indicating that the atmospheric lifetime of ΣANs is shorter than the HNO3 lifetime. We investigate a range of proposed loss mechanisms that would explain the inferred lifetime of ΣANs finding that in combination with deposition, two processes are consistent with the observations: (1) rapid ozonolysis of isoprene nitrates where at least ~40% of the ozonolysis products release NOx from the carbon backbone and/or (2) hydrolysis of particulate organic nitrates with HNO3 as a product. Implications of these ideas for our understanding of NOx and NOy budget in remote and rural locations are discussed.

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“…Since many areas are nitrogen limited, introduction of nitrogen will also affect the carbon storage capacity of an ecosystem (e.g., Holland et al, 1997;Thornton et al, 2007Thornton et al, , 2009Bonan and Levis, 2010). A recent study observed the direct foliar uptake of RONO 2 and subsequent incorporation of the nitrogen into amino acids (Lockwood et al, 2008), indicating that (at least some) RONO 2 will affect plant growth.…”

Section: Discussionmentioning

confidence: 99%

Effects of biogenic nitrate chemistry on the NOx lifetime in remote continental regions

2012

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Abstract.We present an analysis of the NO x budget in conditions of low NO x (NO x = NO + NO 2 ) and high biogenic volatile organic compound (BVOC) concentrations that are characteristic of most continental boundary layers. Using a steady-state model, we show that below 500 pptv of NO x , the NO x lifetime is extremely sensitive to organic nitrate (RONO 2 ) formation rates. We find that even for RONO 2 formation values that are an order of magnitude smaller than is typical for continental conditions significant reductions in NO x lifetime, and consequently ozone production efficiency, are caused by nitrate forming reactions. Comparison of the steady-state box model to a 3-D chemical transport model (CTM) confirms that the concepts illustrated by the simpler model are a useful approximation of predictions provided by the full CTM. This implies that the regional and global budgets of NO x , OH, and ozone will be sensitive to assumptions regarding organic nitrate chemistry. Changes in the budgets of these species affect the representation of processes important to air quality and climate. Consequently, CTMs must include an accurate representation of organic nitrate chemistry in order to provide accurate assessments of past, present, and future air quality and climate. These findings suggest the need for further experimental constraints on the formation and fate of biogenic RONO 2 .

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Foliar uptake of atmospheric organic nitrates

Cited by 41 publications

References 47 publications

Rapid deposition of oxidized biogenic compounds to a temperate forest

Rapid deposition of oxidized biogenic compounds to a temperate forest

Observations of total RONO<sub>2</sub> over the boreal forest: NO<sub>x</sub> sinks and HNO<sub>3</sub> sources

Effects of biogenic nitrate chemistry on the NO<sub>x</sub> lifetime in remote continental regions

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Foliar uptake of atmospheric organic nitrates

Cited by 41 publications

References 47 publications

Rapid deposition of oxidized biogenic compounds to a temperate forest

Rapid deposition of oxidized biogenic compounds to a temperate forest

Observations of total RONO&lt;sub&gt;2&lt;/sub&gt; over the boreal forest: NO&lt;sub&gt;x&lt;/sub&gt; sinks and HNO&lt;sub&gt;3&lt;/sub&gt; sources

Effects of biogenic nitrate chemistry on the NO&lt;sub&gt;x&lt;/sub&gt; lifetime in remote continental regions

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Observations of total RONO<sub>2</sub> over the boreal forest: NO<sub>x</sub> sinks and HNO<sub>3</sub> sources

Effects of biogenic nitrate chemistry on the NO<sub>x</sub> lifetime in remote continental regions