The effect of cross-regional transport on ozone and particulate matter pollution in China: A review of methodology and current knowledge.

China is currently one of the countries impacted by severe atmospheric ozone (O3) and particulate matter (PM) pollution. Due to their moderately long lifetimes, O3 and PM can be transported over long distances, cross the boundaries of source regions and contribute to air pollution in other regions. The reported contributions of cross-regional transport (CRT) to O3 and fine PM (PM2.5) concentrations often exceed those of local emissions in the major regions of China, highlighting the important role of CRT in regional air pollution. Therefore, further improvement of air quality in China requires more joint efforts among regions to ensure a proper reduction in emissions while accounting for the influence of CRT. This review summarizes the methodologies employed to assess the influence of CRT on O3 and PM pollution as well as current knowledge of CRT influence in China. Quantifying CRT contributions in proportion to O3 and PM levels and studying detailed CRT processes of O3, PM and precursors can be both based on targeted observations and/or model simulations. Reported publications indicate that CRT contributes by 40-80 % to O3 and by 10-70 % to PM2.5 in various regions of China. These contributions exhibit notable spatiotemporal variations, with differences in meteorological conditions and/or emissions often serving as main drivers of such variations. Based on trajectory-based methods, transport pathways contributing to O3 and PM pollution in major regions of China have been revealed. Recent studies also highlighted the important role of horizontal transport in the middle/high atmospheric boundary layer or low free troposphere, of vertical exchange and mixing as well as of interactions between CRT, local meteorology and chemistry in the detailed CRT processes. Drawing on the current knowledge on the influence of CRT, this paper provides recommendations for future studies that aim at supporting ongoing air pollution mitigation strategies in China.

Submicron aerosol pollution in Greater Cairo (Egypt): A new type of urban haze?

Greater Cairo, the largest megacity of the Middle East North Africa (MENA) region, is currently suffering from major aerosol pollution, posing a significant threat to public health. However, the main sources of pollution remain insufficiently characterized due to limited atmospheric observations. To bridge this knowledge gap, we conducted a continuous 2-month field study during the winter of 2019-2020 at an urban background site, documenting for the first time the chemical and physical properties of submicron (PM1) aerosols. Crustal material from both desert dust and road traffic dust resuspension contributed as much as 24 % of the total PM1 mass (rising to 66 % during desert dust events), a figure not commonly observed in urban environments. Our observations showed significant decreases in black carbon concentrations and ammonium sulfate compared to data from 15 years ago, indicating an important reduction in both local and regional emissions as a result of effective mitigation measures. The diurnal variability of carbonaceous aerosols was attributed to emissions emanating from local traffic at rush hours and nighttime open biomass burning. Surprisingly, semi-volatile ammonium chloride (NH4Cl) originating from local open biomass and waste burning was found to be the main chemical species in PM1 over Cairo. Its nighttime formation contributed to aerosol water uptake during morning hours, thereby playing a major role in the build-up of urban haze. While our results confirm the persistence of a significant dust reservoir over Cairo, they also unveil an additional source of highly hygroscopic (semi-volatile) inorganic salts, leading to a unique type of urban haze. This haze, with dominant contributors present in both submicron (primarily as NH4Cl) and supermicron (largely as dust) modes, underscores the potential implications of heterogeneous chemical transformation of air pollutants in urban environments.

Reconciling a national methane emission inventory with in-situ measurements.

Reconciling top-down and bottom-up country-level greenhouse gas emission estimates remains a key challenge in the MRV (Monitoring, Reporting, Verification) paradigm. Here we propose to independently quantify cumulative emissions from a significant number of methane (CH4) emitters at national level and derive robust constraints for the national inventory. Methane emissions in Cyprus, an insular country, stem primarily from waste and agricultural activities. We performed 24 intensive survey days of mobile measurements of CH4 from October 2020 to September 2021 at emission 'hotspots' in Cyprus accounting together for about 28 % of national CH4 emissions. The surveyed areas include a large active landfill (Koshi, 8 % of total emissions), a large closed landfill (Kotsiatis, 18 %), and a concentrated cattle farm area (Aradippou, 2 %). Emission rates for each site were estimated using repeated downwind transects and a Gaussian plume dispersion model. The calculated methane emissions from landfills of Koshi and Kotsiatis (25.9 ± 6.4 Gg yr-1) and enteric fermentation of cattle (10.4 ± 4.4 Gg yr-1) were about 129 % and 40 % larger, respectively than the bottom-up sectorial annual estimates used in the national UNFCCC inventory. The parametrization of the Gaussian plume model dominates the uncertainty in our method, with a typical 21 % uncertainty. Seasonal variations have little influence on the results. We show that using an ensemble of in situ measurements targeting representative methane emission hotspots with consistent temporal and spatial coverage can contribute to the monitoring and validation of national bottom-up emission inventories.

Is atmospheric oxidation capacity better in indicating tropospheric O3 formation?

Tropospheric ozone (O3) concentration is increasing in China along with dramatic changes in precursor emissions and meteorological conditions, adversely affecting human health and ecosystems. O3 is formed from the complex nonlinear photochemical reactions from nitrogen oxides (NO x = NO + NO2) and volatile organic compounds (VOCs). Although the mechanism of O3 formation is rather clear, describing and analyzing its changes and formation potential at fine spatial and temporal resolution is still a challenge today. In this study, we briefly summarized and evaluated different approaches that indicate O3 formation regimes. We identify that atmospheric oxidation capacity (AOC) is a better indicator of photochemical reactions leading to the formation of O3 and other secondary pollutants. Results show that AOC has a prominent positive relationship to O3 in the major city clusters in China, with a goodness of fit (R 2) up to 0.6. This outcome provides a novel perspective in characterizing O3 formation and has significant implications for formulating control strategies of secondary pollutants.

Investigating missing sources of glyoxal over China using a regional air quality model (RAMS-CMAQ).

Currently, modeling studies tend to significantly underestimate observed space-based glyoxal (CHOCHO) vertical column densities (VCDs), implying the existence of missing sources of glyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors. In case 1, where the emissions of aromatic compounds were increased three-fold, improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were 3-5-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case 3, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of glyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes (a two-fold increase), the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July.

On the temporal and spatial variation of ozone in Cyprus.

More than sixteen years (1997-2013) of continuous ozone concentrations at the rural Agia Marina (EMEP, 532 ma.s.l.) station in Cyprus, together with a number of ancillary chemical and meteorological parameters have been analyzed on a multiannual, annual and diurnal basis. The observations reveal a) the presence of a prominent seasonality with maxima observed during summer (54±5 ppbv) and the minima in winter (39±3 ppbv) b) a relatively small diurnal variability with the noon levels (50±9 ppbv) being higher by ~4 pbbv compared to nighttime (46±9 ppbv) and c) a non-significant upward trend over the 16 years of 0.11±0.12 ppbv y(-1). To assess the spatial variability over Cyprus, simultaneous measurements in 2011-2012 have been performed at Inia, Stavrovouni and Cavo Greco, three remote marine monitoring sites located to the west, central and the east of the Island, respectively. Our results show that ambient ozone levels over Cyprus are mostly influenced by regional/transported ozone while the local precursor emissions play a minor role in ozone formation. On an annual basis a net ozone reduction of 1.5 and 1.0 ppbv occurs when the air masses originate from northerly and westerly directions, respectively, while this is 2.4 ppbv during southerly wind. This suggests continuous net ozone loss controlled by surface deposition and photochemical destruction, and highlights the importance of long-range transport in controlling ozone levels in Cyprus.