Global nitrogen fixation contributes 413 Tg of reactive nitrogen (Nr) to terrestrial and marine ecosystems annually of which anthropogenic activities are responsible for half, 210 Tg N. The majority of the transformations of anthropogenic Nr are on land (240 Tg N yr−1) within soils and vegetation where reduced Nr contributes most of the input through the use of fertilizer nitrogen in agriculture. Leakages from the use of fertilizer Nr contribute to nitrate (NO3−) in drainage waters from agricultural land and emissions of trace Nr compounds to the atmosphere. Emissions, mainly of ammonia (NH3) from land together with combustion related emissions of nitrogen oxides (NOx), contribute 100 Tg N yr−1 to the atmosphere, which are transported between countries and processed within the atmosphere, generating secondary pollutants, including ozone and other photochemical oxidants and aerosols, especially ammonium nitrate (NH4NO3) and ammonium sulfate (NH4)2SO4. Leaching and riverine transport of NO3 contribute 40–70 Tg N yr−1 to coastal waters and the open ocean, which together with the 30 Tg input to oceans from atmospheric deposition combine with marine biological nitrogen fixation (140 Tg N yr−1) to double the ocean processing of Nr. Some of the marine Nr is buried in sediments, the remainder being denitrified back to the atmosphere as N2 or N2O. The marine processing is of a similar magnitude to that in terrestrial soils and vegetation, but has a larger fraction of natural origin. The lifetime of Nr in the atmosphere, with the exception of N2O, is only a few weeks, while in terrestrial ecosystems, with the exception of peatlands (where it can be 102–103 years), the lifetime is a few decades. In the ocean, the lifetime of Nr is less well known but seems to be longer than in terrestrial ecosystems and may represent an important long-term source of N2O that will respond very slowly to control measures on the sources of Nr from which it is produced.

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The global nitrogen cycle in the twenty-first century

Increasing quantities of atmospheric anthropogenic fixed nitrogen entering the open ocean could account for up to about a third of the ocean's external (nonrecycled) nitrogen supply and up to 3% of the annual new marine biological production, 0.3 petagram of carbon per year. This input could account for the production of up to 1.6 teragrams of nitrous oxide (N2O) per year. Although 10% of the ocean's drawdown of atmospheric anthropogenic carbon dioxide may result from this atmospheric nitrogen fertilization, leading to a decrease in radiative forcing, up to about two-thirds of this amount may be offset by the increase in N2O emissions. The effects of increasing atmospheric nitrogen deposition are expected to continue to grow in the future.

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Impacts of atmospheric anthropogenic nitrogen on the open ocean.

Atmospheric amines - Part I. A review

Atmospheric composition change: Ecosystems–Atmosphere interactions

. The knowledge of the lightning-induced nitrogen oxides (LNOx) source is important for understanding and predicting the nitrogen oxides and ozone distributions in the troposphere and their trends, the oxidising capacity of the atmosphere, and the lifetime of trace gases destroyed by reactions with OH. This knowledge is further required for the assessment of other important NOx sources, in particular from aviation emissions, the stratosphere, and from surface sources, and for understanding the possible feedback between climate changes and lightning. This paper reviews more than 3 decades of research. The review includes laboratory studies as well as surface, airborne and satellite-based observations of lightning and of NOx and related species in the atmosphere. Relevant data available from measurements in regions with strong LNOx influence are identified, including recent observations at midlatitudes and over tropical continents where most lightning occurs. Various methods to model LNOx at cloud scales or globally are described. Previous estimates are re-evaluated using the global annual mean flash frequency of 44±5 s−1 reported from OTD satellite data. From the review, mainly of airborne measurements near thunderstorms and cloud-resolving models, we conclude that a "typical" thunderstorm flash produces 15 (2–40)×1025 NO molecules per flash, equivalent to 250 mol NOx or 3.5 kg of N mass per flash with uncertainty factor from 0.13 to 2.7. Mainly as a result of global model studies for various LNOx parameterisations tested with related observations, the best estimate of the annual global LNOx nitrogen mass source and its uncertainty range is (5±3) Tg a−1 in this study. In spite of a smaller global flash rate, the best estimate is essentially the same as in some earlier reviews, implying larger flash-specific NOx emissions. The paper estimates the LNOx accuracy required for various applications and lays out strategies for improving estimates in the future. An accuracy of about 1 Tg a−1 or 20%, as necessary in particular for understanding tropical tropospheric chemistry, is still a challenging goal.

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The global lightning-induced nitrogen oxides source

Organic nitrogen deposition on land and coastal environments: a review of methods and data

Published observations of organic nitrogen (N) compounds in precipitation go back almost a century. Several different methods have been used to measure both the total and ionic concentrations of N. There is therefore some uncertainty as to whether reported “organic N” is real, or simply the result of uncertainties in chemical analyses or inadequate sampling methods. We found that the materials from which the collector was made (polypropylene, steel, or glass) had no significant effect on the composition of dissolved organic N (DON). The use of a biocide was found to be very important during sampling and storage of samples before analysis. We set up a network of seven collectors across the U.K., from the Cairngorms to Dorset, all operating to the same protocol, and including a biocide. Samples were analysed centrally, using proven methods. Over 6 months, organic N contributed about 20% to the total N in U.K. precipitation, but with a large variation across the country. This means that current estimates of wet deposited N to the U.K., which are based only on the ammonium and nitrate concentrations, are too small. Organic N is not an artefact, but a real problem that needs to be addressed.

Organic nitrogen in precipitation: real problem or sampling artefact?

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A. P. Rowland

Papers

Organic nitrogen deposition on land and coastal environments: a review of methods and data

Organic nitrogen in precipitation: real problem or sampling artefact?

Organic nitrogen in precipitation: real problem or sampling artefact?