Soil surface acidity plays a determining role in the atmospheric-terrestrial exchange of nitrous acid

Donaldson, Melissa A.; Bish, David L.; Raff, Jonathan D.

doi:10.1073/pnas.1418545112

Cited by 93 publications

(98 citation statements)

References 71 publications

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“…In these diffusion-limited environments, the accumulation of microbial metabolic products (e.g., NH 4 + , NO 2 − , and NO 3 − ) may maintain a flux of NO even as soils dry (23,26,32,37). NO 2 − , in particular, is chemically reactive (38) and, in dry soils, may be less likely to be oxidized by nitrifiers but may still chemodenitrify (10,29,39). At our site, NO 2 − concentrations averaged 0.6 μg NO 2 − -N g −1 (Fig.…”

Section: Discussionmentioning

confidence: 99%

“…Chemodenitrification encompasses all of the abiotic nonenzymatic processes that produce NO, including chemical decomposition of nitrous acid as well as reactions between N substrates with reduced metals and humic substances (9)(10)(11). The biological processes that produce NO, however, are numerous [e.g., nitrification, denitrification, nitrifier denitrification, dissimilatory nitrate reduction to ammonium, and anaerobic ammonium oxidation (9)], but nitrification is generally considered the dominant driver of NO emissions under aerobic conditions (12).…”

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Aridity and plant uptake interact to make dryland soils hotspots for nitric oxide (NO) emissions

Homyak

Blankinship

Marchus

et al. 2016

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

100

103

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Nitric oxide (NO) is an important trace gas and regulator of atmospheric photochemistry. Theory suggests moist soils optimize NO emissions, whereas wet or dry soils constrain them. In drylands, however, NO emissions can be greatest in dry soils and when dry soils are rewet. To understand how aridity and vegetation interact to generate this pattern, we measured NO fluxes in a California grassland, where we manipulated vegetation cover and the length of the dry season and measured [δ 15 -N]NO and [δ 18 -O]NO following rewetting with 15 N-labeled substrates. Plant N uptake reduced NO emissions by limiting N availability. In the absence of plants, soil N pools increased and NO emissions more than doubled. In dry soils, NO-producing substrates concentrated in hydrologically disconnected microsites. Upon rewetting, these concentrated N pools underwent rapid abiotic reaction, producing large NO pulses. Biological processes did not substantially contribute to the initial NO pulse but governed NO emissions within 24 h postwetting. Plants acted as an N sink, limiting NO emissions under optimal soil moisture. When soils were dry, however, the shutdown in plant N uptake, along with the activation of chemical mechanisms and the resuscitation of soil microbial processes upon rewetting, governed N loss. Aridity and vegetation interact to maintain a leaky N cycle during periods when plant N uptake is low, and hydrologically disconnected soils favor both microbial and abiotic NO-producing mechanisms. Under increasing rates of atmospheric N deposition and intensifying droughts, NO gas evasion may become an increasingly important pathway for ecosystem N loss in drylands.nitric oxide | chemodenitrification | drylands | NO pulses | N cycling N itric oxide (NO) is an important trace gas; it regulates the oxidative capacity of the atmosphere and indirectly influences Earth's climate (1). In the troposphere, NO catalyzes the production of hydroxyl radical, a powerful oxidant and cleanser of atmospheric contaminants. High concentrations of NO also favor the production of ozone (O 3 ), an urban pollutant and contributor to radiative forcing (1). Globally, fossil fuel combustion and biomass burning are major sources of NO, but soils are also a substantial source (2). Roughly 25-60% of terrestrial NO emissions originate from drylands (arid and semiarid environments) (3), which cover one-third of the terrestrial land surface (4), suggesting arid environments are important to global NO production. Climate models predict an expansion of drylands and intensifying droughts in existing arid regions (5), and when coupled with increasing rates of nitrogen (N) deposition and changes in the magnitude and frequency of precipitation events (6), increased soil NO emissions are possible (7). Paradoxically, arid soils are often described as infertile because biological processes are limited by water and N (8), raising the questions of why drylands are NO emission "hotspots."NO is produced in soils through both abiotic and biotic processes (2). Chemodeni...

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Section: Discussionmentioning

confidence: 99%

mentioning

confidence: 99%

Aridity and plant uptake interact to make dryland soils hotspots for nitric oxide (NO) emissions

Homyak

Blankinship

Marchus

et al. 2016

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

100

103

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“…These results stimulated laboratory investigations on potential HONO precursors from which the most frequently discussed mechanisms are (i) the photosensitized reduction of nitrogen dioxide (NO 2 ) by organic material, e.g. humic acids (George et al, 2005;Stemmler et al, 2006;2007, Sosedova et al, 2011Han et al, 2016), (ii) the photolysis of adsorbed nitric acid (Zhou et al, , 2011Laufs and Kleffmann, 2016), (iii) biogenic production of nitrite in soil (Su et al, 2011;Ostwald et al, 2013;Maljanen et al, 2013;Oswald et al, 2015;Scharko et al, 2015;Weber, 2015) and (iv) release of adsorbed HONO from soil surfaces after deposition of strong acids (VandenBoer et al, 2013(VandenBoer et al, , 2014(VandenBoer et al, , 2015Donaldson et al, 2014). Another discussed source, the reaction of excited gaseous NO 2 with water (Li et al, 2008), is of minor importance as demonstrated by laboratory (Crowley and Carl, 1997;Carr et al, 2009;Amedro et al, 2011) and modelling studies (Sörgel et al, 2011b;Czader et al, 2012).…”

Section: Introductionmentioning

confidence: 96%

Diurnal fluxes of HONO above a crop rotation

Laufs¹,

Cazaunau²,

Stella³

et al. 2017

Atmos. Chem. Phys.

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Abstract. Nitrous acid (HONO) fluxes were measured above an agricultural field site near Paris during different seasons. Above bare soil, different crops were measured using the aerodynamic gradient (AG) method. Two LOPAPs (LOng Path Absorption Photometer) were used to determine the HONO gradients between two heights. During daytime mainly positive HONO fluxes were observed, which showed strong correlation with the product of the NO 2 concentration and the long wavelength UV light intensity, expressed by the photolysis frequency J (NO 2 ). These results are consistent with HONO formation by photosensitized heterogeneous conversion of NO 2 on soil surfaces as observed in recent laboratory studies. An additional influence of the soil temperature on the HONO flux can be explained by the temperature-dependent HONO adsorption on the soil surface. A parameterization of the HONO flux at this location with NO 2 concentration, J (NO 2 ), soil temperature and humidity fits reasonably well all flux observations at this location.

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“…However, it has been shown that the nature of the surface, and particularly surface charge, plays an important role in the uptake and release of HONO from soils. 232 For example, as shown in Fig. 8b, soil surface components such as aluminum and iron oxides/hydroxides are present in a number of different forms such as MO À , M-OH and MOH 2 + (M ¼ metal) which interact with oxides of nitrogen, changing the pH at which HONO is released to more basic conditions compared to pure water by as much as several pH units.…”

Section: -218mentioning

confidence: 99%

Introductory lecture: atmospheric chemistry in the Anthropocene

Finlayson-Pitts

2017

Faraday Discuss.

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The term “Anthropocene” was coined by Professor Paul Crutzen in 2000 to describe an unprecedented era in which anthropogenic activities are impacting planet Earth on a global scale. Greatly increased emissions into the atmosphere, reflecting the advent of the Industrial Revolution, have caused significant changes in both the lower and upper atmosphere. Atmospheric reactions of the anthropogenic emissions and of those with biogenic compounds have significant impacts on human health, visibility, climate and weather. Two activities that have had particularly large impacts on the troposphere are fossil fuel combustion and agriculture, both associated with a burgeoning population. Emissions are also changing due to alterations in land use. This paper describes some of the tropospheric chemistry associated with the Anthropocene, with emphasis on areas having large uncertainties. These include heterogeneous chemistry such as those of oxides of nitrogen and the neonicotinoid pesticides, reactions at liquid interfaces, organic oxidations and particle formation, the role of sulfur compounds in the Anthropocene and biogenic–anthropogenic interactions. A clear and quantitative understanding of the connections between emissions, reactions, deposition and atmospheric composition is central to developing appropriate cost-effective strategies for minimizing the impacts of anthropogenic activities. The evolving nature of emissions in the Anthropocene places atmospheric chemistry at the fulcrum of determining human health and welfare in the future.

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Soil surface acidity plays a determining role in the atmospheric-terrestrial exchange of nitrous acid

Cited by 93 publications

References 71 publications

Aridity and plant uptake interact to make dryland soils hotspots for nitric oxide (NO) emissions

Aridity and plant uptake interact to make dryland soils hotspots for nitric oxide (NO) emissions

Diurnal fluxes of HONO above a crop rotation

Introductory lecture: atmospheric chemistry in the Anthropocene

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