Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m −3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO 2 , which is oxidized by NO 2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution.

Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

. Extreme haze episodes repeatedly shrouded Beijing during the winter of 2012–2013, causing major environmental and health problems. To better understand these extreme events, we performed a model-assisted analysis of the hourly observation data of PM2.5 and its major chemical compositions. The synthetic analysis shows that (1) the severe winter haze was driven by stable synoptic meteorological conditions over northeastern China, and not by an abrupt increase in anthropogenic emissions. (2) Secondary species, including organics, sulfate, nitrate, and ammonium, were the major constituents of PM2.5 during this period. (3) Due to the dimming effect of high loading of aerosol particles, gaseous oxidant concentrations decreased significantly, suggesting a reduced production of secondary aerosols through gas-phase reactions. Surprisingly, the observational data reveals an enhanced production rate of secondary aerosols, suggesting an important contribution from other formation pathways, most likely heterogeneous reactions. These reactions appeared to be more efficient in producing secondary inorganics aerosols than organic aerosols resulting in a strongly elevated fraction of inorganics during heavily polluted periods. (4) Moreover, we found that high aerosol concentration was a regional phenomenon. The accumulation process of aerosol particles occurred successively from cities southeast of Beijing. The apparent sharp increase in PM2.5 concentration of up to several hundred μg m−3 per hour recorded in Beijing represented rapid recovery from an interruption to the continuous pollution accumulation over the region, rather than purely local chemical production. This suggests that regional transport of pollutants played an important role during these severe pollution events.

/pdf/exploring-the-severe-winter-haze-in-beijing-the-impact-of-xph7x56h03.pdf

Exploring the severe winter haze in Beijing: the impact of synoptic weather, regional transport and heterogeneous reactions

China experienced severe haze pollution in January 2013. Here we have a detailed characterization of the sources and evolution mechanisms of this haze pollution with a focus on four haze episodes that occurred during 10–14 January in Beijing. The main source of data analyzed is from submicron aerosol measurements by an Aerodyne Aerosol Chemical Speciation Monitor. The average PM1 mass concentration during the four haze episodes ranged from 144 to 300 µg m−3, which was more than 10 times higher than that observed during clean periods. All submicron aerosol species showed substantial increases during haze episodes with sulfate being the largest. Secondary inorganic species played enhanced roles in the haze formation as suggested by their elevated contributions during haze episodes. Positive matrix factorization analysis resolved six organic aerosol (OA) factors including three primary OA (POA) factors from traffic, cooking, and coal combustion emissions, respectively, and three secondary OA (SOA) factors. Overall, SOA contributed 41–59% of OA with the rest being POA. Coal combustion OA (CCOA) was the largest primary source, on average accounting for 20–32% of OA, and showed the most significant enhancement during haze episodes. A regional SOA (RSOA) was resolved for the first time which showed a pronounced peak only during the record-breaking haze episode (Ep3) on 12–13 January. The regional contributions estimated based on the steep evolution of air pollutants were found to play dominant roles for the formation of Ep3, on average accounting for 66% of PM1 during the peak of Ep3 with sulfate, CCOA, and RSOA being the largest fractions (> ~ 75%). Our results suggest that stagnant meteorological conditions, coal combustion, secondary production, and regional transport are four main factors driving the formation and evolution of haze pollution in Beijing during wintertime.

https://agupubs.onlinelibrary.wiley.com/doi/pdf/10.1002/2014JD021641

Investigation of the sources and evolution processes of severe haze pollution in Beijing in January 2013

Aerosol-planetary boundary layer (PBL) interactions have been found to enhance air pollution in megacities in China. We show that black carbon (BC) aerosols play the key role in modifying the PBL meteorology and hence enhancing the haze pollution. With model simulations and data analysis from various field observations in December 2013, we demonstrate that BC induces heating in the PBL, particularly in the upper PBL, and the resulting decreased surface heat flux substantially depresses the development of PBL and consequently enhances the occurrences of extreme haze pollution episodes. We define this process as the “dome effect” of BC and suggest an urgent need for reducing BC emissions as an efficient way to mitigate the extreme haze pollution in megacities of China.

Enhanced haze pollution by black carbon in megacities in China

Air quality is concerned with pollutants in both the gas phase and solid or liquid phases. The latter are referred to as aerosols, which are multifaceted agents affecting air quality, weather and climate through many mechanisms. Unlike gas pollutants, aerosols interact strongly with meteorological variables with the strongest interactions taking place in the planetary boundary layer (PBL). The PBL hosting the bulk of aerosols in the lower atmosphere is affected by aerosol radiative effects. Both aerosol scattering and absorption reduce the amount of solar radiation reaching the ground and thus reduce the sensible heat fluxes that drive the diurnal evolution of the PBL. Moreover, aerosols can increase atmospheric stability by inducing a temperature inversion as a result of both scattering and absorption of solar radiation, which suppresses dispersion of pollutants and leads to further increases in aerosol concentration in the lower PBL. Such positive feedback is especially strong during severe pollution events. Knowledge of the PBL is thus crucial for understanding the interactions between air pollution and meteorology. A key question is how the diurnal evolution of the PBL interacts with aerosols, especially in vertical directions, and affects air quality. We review the major advances in aerosol measurements, PBL processes and their interactions with each other through complex feedback mechanisms, and highlight the priorities for future studies.

/pdf/aerosol-and-boundary-layer-interactions-and-impact-on-air-4u0ggedy1h.pdf

Aerosol and boundary-layer interactions and impact on air quality

The Nested Air Quality Prediction Model System (NAQPMS) was used to investigate the temporal and spatial variations of PM 2.5 over tropospheric central eastern China in January 2013. The impact of regional transport and its implications on pollution prevention and control were also examined. Comparison between simulated and observed PM 2.5 showed NAQPMS was able to reproduce the evolution of PM 2.5 during heavy haze episodes. The results indicated that regional transport of PM 2.5 played an important role in regional haze episodes in the city cluster including Hebei, Beijing and Tianjin (HBT). The cross-city clusters transport outside HBT and transport among cities inside HBT contributed 20%-35% and 26%-35% of PM 2.5 as compared with local emission, in HBT respectively. To meet the Air Quality Standards for Grade Ⅱ, 90%, 90% and 65% of emissions would have to be cut down in Hebei, Tianjin and Beijing, if non-control strategy was taken in the surrounding city clusters of HBT. This implicated that control of emissions in one city cluster is not sufficient to reduce regional haze events, and joint efforts among city clusters are essential. Besides regional transports, two-way feedback between boundary-layer evolution and PM 2.5 also significantly contributed to the formation of heavy hazes, which contributed 30% of monthly average PM 2.5 concentration in HBT.

Ning Lu

Papers

Modeling study of regional severe hazes over mid-eastern China in January 2013 and its implications on pollution prevention and control