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NOx emissions in China: historical trends and future perspectives

Nitrogen oxides (NOx) are key pollutants for the improvement of ambient air quality. Within this study we estimated the historical NOx emissions in China for the period 1995–2010, and calculated future NOx emissions every five years until 2030 under six emission scenarios. Driven by the fast growth of energy consumption, we estimate the NOx emissions in China increased rapidly from 11.0 Mt in 1995 to 26.1 Mt in 2010. Power plants, industry and transportation were major sources of NOx emissions, accounting for 28.4%, 34.0%, and 25.4% of the total NOx emissions in 2010, respectively. Two energy scenarios, a business as usual scenario (BAU) and an alternative policy scenario (PC), were developed to project future energy consumption. In 2030, total energy consumption is projected to increase by 64% and 27% from 2010 level respectively. Three sets of end-of-pipe pollution control measures, including baseline, progressive, and stringent control case, were developed for each energy scenario, thereby constituting six emission scenarios. By 2030, the total NOx emissions are projected to increase (compared to 2010) by 36% in the baseline while policy cases result in reduction up to 61% in the most ambitious case with stringent control measures. More than a third of the reduction achieved by 2030 between least and most ambitious scenario comes from power sector, and more than half is distributed equally between industry and transportation sectors. Selective catalytic reduction dominates the NOx emission reductions in power plants, while life style changes, control measures for industrial boilers and cement production are major contributors to reductions in industry. Timely enforcement of legislation on heavy-duty vehicles would contribute significantly to NOx emission reductions. About 30% of the NOx emission reduction in 2020 and 40% of the NOx emission reduction in 2030 could be treated as the ancillary benefit of energy conservation. Sensitivity analysis was conducted to explore the impact of key factors on future emissions.
Aircraft observations of cold pools under marine stratocumulus

Although typically associated with precipitating cumuli, cold pools also form under shallower stratocumulus. This study presents cold-pool observations as sampled by the NSF/NCAR C-130, which made cloud and boundary-layer measurements over the southeast Pacific stratocumulus region at an altitude of approximately 150 m during the VOCALS Regional Experiment. Ninety edges of cold pools are found in the C-130 measurements by identifying step-like changes in the potential temperature. Examination of their mesoscale environment shows that the observed cold pools tend to form under heavier precipitation, thicker clouds, and in cleaner environments. Cold pools are also found to form under clouds with high LWP values over the night of or before sampling. When they form, cold pools often form in clusters or on top of each other, rather than as separate, individual entities. Their sizes range from 2 km to 16 km (middle 50th percentile), where the largest of cold pools are associated with the greatest drops in temperature. Composites of various observed thermodynamic and chemical variables along the cold-pool edges indicate increased humidity, equivalent potential temperature, coarse-mode aerosol, and dimethyl sulfide concentration inside cold pools. The enhancements inside cold pools are consistent with increased static stability that traps fluxes from the ocean surface in the lowest levels of the boundary layer. By using pressure perturbations, the average cold pool is estimated to be approximately 300 m deep. The temperature depression in cold pools also leads to density-driven flows that drive convergence of horizontal winds and measurable, mechanically driven vertical wind velocity at the edges of cold pools.
Impact of transport model errors on the global and regional methane emissions estimated by inverse modelling

A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dynamique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion set-up (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr−1 at the global scale, representing 5% of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr−1 in North America to 7 Tg yr−1 in Boreal Eurasia (from 23 to 48%, respectively). At the model grid-scale, the spread of inverse estimates can reach 150% of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling, especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit the impact of transport model errors on estimated methane fluxes.
Biogenic isoprene and implications for oxidant levels in Beijing during the 2008 Olympic Games

As the host of the 2008 Summer Olympic Games, Beijing implemented a series of stringent, short-term air quality control measures to reduce the emissions of anthropogenic air pollutants. Large reductions in the daily average concentrations of primary pollutants, e.g., non-methane hydrocarbons (NMHCs) and nitrogen oxides (NOx) of approximately 50% were observed at the air quality observatory of Peking University. Nevertheless, high levels of ozone were present during the control period. Although anthropogenic precursors were greatly reduced, the meteorological conditions in summer, including high temperature and light flux, are conducive to the production of large amounts of biogenic isoprene, which is extremely reactive. The diurnal pattern of isoprene showed daily maximum mixing ratios of 0.83 ppbv at noon and a minimum at night, reflecting its primarily biogenic properties. Using the ratio of isoprene to vehicle exhaust tracers, approximately 92% of the daytime isoprene was estimated from biogenic sources, and only 8% was attributed to vehicular emissions. In terms of OH reactivity and the ozone formation potential (OFP), biogenic isoprene with its midday surge can contribute approximately 20% of the total OFPs and 40–50% of the total OH reactivities of the 65 measured NMHCs during the midday hours. The discrepancy between decreased precursor levels and the observed high ozone was most likely caused by a combination of many factors. The changes in the partition among the components of oxidation products (O3, NO2 and NOz) and the contribution of air pollutants from regional sources outside Beijing should be two primary reasons. Furthermore, the influences of biogenic isoprene as well as the non-linearity of O3-VOC-NOx chemistry are other major concerns that can reduce the effectiveness of the control measures for decreasing ozone formation. Although anthropogenic precursors were greatly reduced during the Olympic Games, sufficient biogenic isoprene and moderate NOx were still present in the conditions of high radiation flux and temperature during midday and early afternoon, which can still contribute a significant fraction of midday and early afternoon O3.
Technical Note: Estimating aerosol effects on cloud radiative forcing

Estimating anthropogenic aerosol effects on the planetary energy balance through the aerosol influence on clouds using the difference in cloud radiative forcing from simulations with and without anthropogenic emissions produces estimates that are positively biased. A more representative method is suggested using the difference in cloud radiative forcing calculated as a diagnostic with aerosol scattering and absorption neglected. The method also yields an aerosol radiative forcing decomposition that includes a term quantifying the impact of changes in surface albedo. The method requires only two additional diagnostic calculations: the whole-sky and clear-sky top-of-atmosphere radiative flux with aerosol scattering and absorption neglected.
The fine-scale structure of the trade wind cumuli over Barbados – an introduction to the CARRIBA project

The CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) project, focused on high resolution and collocated measurements of thermodynamic, turbulent, microphysical, and radiative properties of trade wind cumuli over Barbados, is introduced. The project is based on two one-month field campaigns in November 2010 (climatic wet season) and April 2011 (climatic dry season). Observations are based on helicopter-borne and ground-based measurements in an area of 100 km2 off the coast of Barbados. CARRIBA is accompanied by long-term observations at the Barbados Cloud Observatory located at the East coast of Barbados since early in 2010 and which provides a longer-term context for the CARRIBA measurements. The deployed instrumentation and sampling strategy are presented together with a classification of the meteorological conditions. The two campaigns were influenced by different air masses advected from the Caribbean area, the Atlantic Ocean, and the African continent which led to distinct aerosol conditions. Pristine conditions with low aerosol particle number concentrations of ~100 cm3 were alternating with periods influenced by Saharan dust or aerosol from biomass burning resulting in comparably high number concentrations of ~ 500 cm3. The biomass burning aerosol was originating from both the Caribbean area and Africa. The shallow cumulus clouds responded to the different aerosol conditions with a wide range of mean droplet sizes and number concentrations. Two days with different aerosol and cloud microphysical properties but almost identical meteorological conditions have been analyzed in detail. The differences in the droplet number concentration and droplet sizes appear not to show any significant change for turbulent cloud mixing, but the relative roles of droplet inertia and sedimentation in initiating coalescence, as well as the cloud reflectivity, do change substantially.
The impact of horizontal heterogeneities, cloud fraction, and liquid water path on warm cloud effective radii from CERES-like Aqua MODIS retrievals

The impact of horizontal heterogeneities, liquid water path (LWP from AMSR-E), and cloud fraction (CF) on MODIS cloud effective radius (re), retrieved from the 2.1 μm (re2.1) and 3.8 μm (re3.8) channels, is investigated for warm clouds over the southeast Pacific. Values of re retrieved using the CERES algorithms are averaged at the CERES footprint resolution (&sim;20 km), while heterogeneities (Hσ) are calculated as the ratio between the standard deviation and mean 0.64 μm reflectance. The value of re2.1 strongly depends on CF, with magnitudes up to 5 μm larger than those for overcast scenes, whereas re3.8 remains insensitive to CF. For cloudy scenes, both re2.1 and re3.8 increase with Hσ for any given AMSR-E LWP, but re2.1 changes more than for re3.8. Additionally, re3.8–re2.1 differences are positive (<1 μm) for homogeneous scenes (Hσ < 0.2) and LWP > 45 gm−2, and negative (up to −4 μm) for larger Hσ. While re3.8–re2.1 differences in homogeneous scenes are qualitatively consistent with in situ microphysical observations over the region of study, negative differences – particularly evinced in mean regional maps – are more likely to reflect the dominant bias associated with cloud heterogeneities rather than information about the cloud vertical structure. The consequences for MODIS LWP are also discussed.
Review and uncertainty assessment of size-resolved scavenging coefficient formulations for below-cloud snow scavenging of atmospheric aerosols

Theoretical parameterizations for the size-resolved scavenging coefficient for atmospheric aerosol particles scavenged by snow (Λsnow) need assumptions regarding (i) snow particle–aerosol particle collection efficiency E, (ii) snow-particle size distribution N(Dp), (iii) snow-particle terminal velocity VD, and (iv) snow-particle cross-sectional area A. Existing formulas for these parameters are reviewed in the present study, and uncertainties in Λsnow caused by various combinations of these parameters are assessed. Different formulations of E can cause uncertainties in Λsnow of more than one order of magnitude for all aerosol sizes for typical snowfall intensities. E is the largest source of uncertainty among all the input parameters, similar to rain scavenging of atmospheric aerosols (Λrain) as was found in a previous study by Wang et al. (2010). However, other parameters can also cause significant uncertainties in Λsnow, and the uncertainties from these parameters are much larger than for Λrain. Specifically, different N(Dp) formulations can cause one-order-of-magnitude uncertainties in Λsnow for all aerosol sizes, as is also the case for a combination of uncertainties from both VD and A. Assumptions about dominant snow-particle shape (and thus different VD and A) will cause an uncertainty of up to one order of magnitude in the calculated scavenging coefficient. In comparison, uncertainties in Λrain from N(Dp) are smaller than a factor of 5, and those from VD are smaller than a factor of 2. As expected, Λsnow estimated from empirical formulas generated from field measurements falls in the upper range of, or is higher than, the theoretically estimated values, which can be explained by additional processes/mechanisms that influence field-derived Λsnow but that are not considered in the theoretical Λsnow formulas. Predicted aerosol concentrations obtained by using upper range vs. lower range of Λsnow values (a difference of around two orders of magnitude in Λsnow) can differ by a factor of 2 for just a one-centimetre snowfall (liquid water equivalent of approximately 1 mm). Based on the median and upper range of theoretically generated Λsnow and Λsnow values, it is likely that, for typical rain and snow events, the removal of atmospheric aerosol particles by snow is more effective than removal by rain for equivalent precipitation amounts, although a firm conclusion requires much more evidence.
Laboratory and modeling studies on the effects of water and soot emissions and ambient conditions on the properties of contrail ice particles in the jet regime

Contrails and contrail-induced cirrus clouds are identified as the most uncertain components in determining aviation impacts on global climate change. Parameters affecting contrail ice particle formation immediately after the engine exit plane (< 5 s in plume age) may be critical to ice particle properties used in large-scale models predicting contrail radiative forcing. Despite this, detailed understanding of these parametric effects is still limited. In this paper, we present results from recent laboratory and modeling studies conducted to investigate the effects of water and soot emissions and ambient conditions on near-field formation of contrail ice particles and ice particle properties. The Particle Aerosol Laboratory (PAL) at the NASA Glenn Research Center and the Aerodyne microphysical parcel model for contrail ice particle formation were employed. Our studies show that exhaust water concentration has a significant impact on contrail ice particle formation and properties. When soot particles were introduced, ice particle formation was observed only when exhaust water concentration was above a critical level. When no soot or sulfuric acid was introduced, no ice particle formation was observed, suggesting that ice particle formation from homogeneous nucleation followed by homogeneous freezing of liquid water was unfavorable. Soot particles were found to compete for water vapor condensation, and higher soot concentrations emitted into the chamber resulted in smaller ice particles being formed. Chamber conditions corresponding to higher cruising altitudes were found to favor ice particle formation. The microphysical model captures trends of particle extinction measurements well, but discrepancies between the model and the optical particle counter measurements exist as the model predicts narrower ice particle size distributions and ice particle sizes nearly a factor of two larger than measured. These discrepancies are likely due to particle loss and scatter during the experimental sampling process and the lack of treatment of turbulent mixing in the model. Our combined experimental and modeling work demonstrates that formation of contrail ice particles can be reproduced in the NASA PAL facility, and the parametric understanding of the ice particle properties from the model and experiments can potentially be used in large-scale models to provide better estimates of the impact of aviation contrails on climate change.
Atmospheric inversion of the surface CO2 flux with 13CO2 constraint

Observations of 13CO2 at 73 sites compiled in the GLOBALVIEW database are used for an additional constraint in a global atmospheric inversion of the surface CO2 flux using CO2 observations at 210 sites for the 2002–2004 period for 39 land regions and 11 ocean regions. This constraint is implemented using the 13CO2/CO2 flux ratio modeled with a terrestrial ecosystem model and an ocean model. These models simulate 13CO2 discrimination rates of terrestrial photosynthesis and respiration and ocean-atmosphere diffusion processes. In both models, the 13CO2 disequilibrium between fluxes to and from the atmosphere is considered due to the historical change in atmospheric 13CO2 concentration. For the 2002–2004 period, the 13CO2 constraint on the inversion increases the total land carbon sink from 3.40 to 3.70 Pg C yr−1 and decreases the total oceanic carbon sink from 1.48 to 1.12 Pg C yr−1. The largest changes occur in tropical areas: a considerable decrease in the carbon source in the Amazon forest, and this decrease is mostly compensated by increases in the ocean region immediately west of the Amazon and the southeast Asian land region. Our further investigation through different treatments of the 13CO2/CO2 flux ratio used in the inversion suggests that variable spatial distributions of the 13CO2 isotopic discrimination rate simulated by the models over land and ocean have considerable impacts on the spatial distribution of the inverted CO2 flux over land and the inversion results are not sensitive to errors in the estimated disequilibria over land and ocean.