Abstract

Abstract. Human activities have substantially increased atmospheric deposition of reactive nitrogen to the Earth's surface, inducing unintentional effects on ecosystems with complex environmental and climate consequences. One consequence remaining unexplored is how surface air quality might respond to the enhanced nitrogen deposition through surface–atmosphere exchange. Here we combine a chemical transport model (GEOS-Chem) and a global land model (Community Land Model, CLM) to address this issue with a focus on ozone pollution in the Northern Hemisphere. We consider three processes that are important for surface ozone and can be perturbed by the addition of atmospheric deposited nitrogen – namely, emissions of biogenic volatile organic compounds (VOCs), ozone dry deposition, and soil nitrogen oxide (NOx) emissions. We find that present-day anthropogenic nitrogen deposition (65 Tg N a−1 to the land), through enhancing plant growth (represented as increases in vegetation leaf area index, LAI, in the model), could increase surface ozone from increased biogenic VOC emissions (e.g., a 6.6 Tg increase in isoprene emission), but it could also decrease ozone due to higher ozone dry deposition velocities (up to 0.02–0.04 cm s−1 increases). Meanwhile, deposited anthropogenic nitrogen to soil enhances soil NOx emissions. The overall effect on summer mean surface ozone concentrations shows general increases over the globe (up to 1.5–2.3 ppbv over the western US and South Asia), except for some regions with high anthropogenic NOx emissions (0.5–1.0 ppbv decreases over the eastern US, western Europe, and North China). We compare the surface ozone changes with those driven by the past 20-year climate and historical land use changes. We find that the impacts from anthropogenic nitrogen deposition can be comparable to the climate- and land-use-driven surface ozone changes at regional scales and partly offset the surface ozone reductions due to land use changes reported in previous studies. Our study emphasizes the complexity of biosphere–atmosphere interactions, which can have important implications for future air quality prediction.

Highlights

  • Reactive nitrogen, in the forms of reduced (NHx) and oxidized nitrogen (NOy), is an essential nutrient to the biosphere

  • In this study we present an exploratory study aiming to quantify the influences of anthropogenic nitrogen deposition on surface ozone air quality by using the GEOS-Chem chemical transport model asynchronously coupled with the Community Land Model (CLM) land model

  • We simulate in GEOS-Chem global atmospheric nitrogen deposition fluxes for the present-day and the preindustrial conditions, and we conduct near-equilibrium CLM simulations with these fluxes to estimate terrestrial vegetation LAI, soil NOx emissions, and their changes due to anthropogenic nitrogen deposition

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Summary

Introduction

In the forms of reduced (NHx) and oxidized nitrogen (NOy), is an essential nutrient to the biosphere. Reactive nitrogen is mainly fixed from inert nitrogen gas (N2) through natural biological fixation, lightning, and wildfires (Galloway et al, 2004; Fowler et al, 2013) Human activities such as urbanization, industrialization, and agricultural development have led to the emission of large amounts of reactive nitrogen in the forms of nitrogen oxides (NOx = NO + NO2) and ammonia (NH3) since the preindustrial period. Near-surface ozone is a harmful air pollutant that results in detrimental effects on human health and vegetation (Bates, 2005; Jerrett et al, 2009; Avnery et al, 2011) It is mainly formed in the troposphere by photochemical oxidation of carbon monoxide (CO) and volatile organic compounds (VOCs) in the presence of NOx. Tropospheric ozone burden has more than doubled since preindustrial times, mainly driven by rising anthropogenic emissions of ozone precursors (NOx, CO, and VOCs) and the recent equatorward shift of emission patterns (Young et al, 2013; Zhang et al, 2016). To evaluate the relative importance of nitrogen deposition, we estimate the surface ozone changes driven by historical climate and land use changes which have been better constrained in recent studies as described above

Model description
The GEOS-Chem chemical transport model
The Community Land Model
Asynchronous coupling and model experiments
Global emissions and deposition of reactive nitrogen
Changes in vegetation LAI and subsequent responses
Changes in soil NOx emissions
Surface ozone concentration
Comparisons with climate- and land-use-driven surface ozone changes
Conclusions
Soil NOx emissions
NH3 volatilization
Findings
Plant nitrogen uptake
Full Text
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