Relative Contributions of Boundary-Layer Meteorological Factors to the Explosive Growth of PM2.5 during the Red-Alert Heavy Pollution Episodes in Beijing in December 2016

Based on observations of urban mass concentration of fine particulate matter smaller than 2.5 μm in diameter （PM2.5）, ground meteorological data, vertical measurements of winds, temperature, and relative humidity （RH）, and ECMWF reanalysis data, the major changes in the vertical structures of meteorological factors in the boundary layer （BL） during the heavy aerosol pollution episodes （HPEs） that occurred in winter 2016 in the urban Beijing area were analyzed. The HPEs are divided into two stages： the transport of pollutants under prevailing southerly winds, known as the transport stage （TS）, and the PM2.5 explosive growth and pollution accumulation period characterized by a temperature inversion with low winds and high RH in the lower BL, known as the cumulative stage （CS）. During the TS, a surface high lies south of Beijing, and pollutants are transported northwards. During the CS, a stable BL forms and is characterized by weak winds, temperature inversion, and moisture accumulation. Stable atmospheric stratifica- tion featured with light/calm winds and accumulated moisture （RH 〉 80%） below 250 m at the beginning of the CS is closely associated with the inversion, which is strengthened by the considerable decrease in near-surface air temperat- ure due to the interaction between aerosols and radiation after the aerosol pollution occurs. A significant increase in the PLAM （Parameter Linking Aerosol Pollution and Meteorological Elements） index is found, which is linearly re- lated to PM mass change. During the first 10 h of the CS, the more stable BL contributes approximately 84% of the explosive growth of PM2.5 mass. Additional accumulated near-surface moisture caused by the ground temperature de- crease, weak turbulent diffusion, low BL height, and inhibited vertical mixing of water vapor is conducive to the sec- ondary aerosol formation through chemical reactions, including liquid phase and heterogeneous reactions, which fur- ther increases the PM2.5 concentration levels. The contribution of these reaction mechanisms to the explosive growth of PM2,5 mass during the early CS and subsequent pollution accumulation requires further investigation.

Influences of Meteorological Conditions on Interannual Variations of Particulate Matter Pollution during Winter in the Beijing–Tianjin–Hebei Area

To investigate the interannual variations of particulate matter （PM） pollution in winter, this paper examines the pollution characteristics of PM with aerodynamic diameters of less than 2.5 and 10 μm （i.e., PM2.5 and PM10）, and their relationship to meteorological conditions over the Beijing municipality, Tianjin municipality, and Hebei Province--an area called Jing-Jin-Ji （JJJ, hereinafter）-in December 2013-16. The meteorological conditions during this period are also analyzed. The regional average concentrations of PM2.5 （PM10） over the JJJ area during this period were 148.6 （236.4）, 100.1 （166.4）, 140.5 （204.5）, and 141.7 （203.1） μg m^-3, respectively. The high occurrence frequencies of cold air outbreaks, a strong Siberian high, high wind speeds and boundary layer height, and low temperature and relative humidity, were direct meteorological causes of the low PM concentration in December 2014. A combined analysis of PM pollution and meteorological conditions implied that control measures have resulted in an effective improvement in air quality. Using the same emissions inventory in December 2013-16, a modeling analysis showed emissions of PM2.5 to decrease by 12.7%, 8.6%, and 8.3% in December 2014, 2015, and 2016, respectively, each compared with the previous year, over the JJJ area.

Temporal Variation and Source Identification of Black Carbon at Lin'an and Longfengshan Regional Background Stations in China

Black carbon （BC） is a component of fine particulate matter （PM2.5）, associated with climate, weather, air quality, and people＇s health. However, studies on temporal variation of atmospheric BC concentration at background stations in China and its source area identification are lacking. In this paper, we use 2-yr BC observations from two background stations, Lin＇an （LAN） and Longfengshan （LFS）, to perform the investigation. The results show that the mean diurnal variation of BC has two significant peaks at LAN while different characteristics are found in the BC vari- ation at LFS, which are probably caused by the difference in emission source contributions. Seasonal variation of monthly BC shows double peaks at LAN but a single peak at LFS. The annual mean concentrations of BC at LAN and LFS decrease by 1.63 and 0.26 μg m 3 from 2009 to 2010, respectively. The annual background concentration of BC at LAN is twice higher than that at LFS. The major source of the LAN BC is industrial emission while the source of the LFS BC is residential emission. Based on transport climatology on a 7-day timescale, LAN and LFS stations are sensitive to surface emissions respectively in belt or approximately circular area, which are dominated by summer monsoon or colder land air flows in Northwest China. In addition, we statistically analyze the BC source regions by using BC observation and FLEXible PARTicle dispersion model （FLEXPART） simulation. In summer, the source regions of BC are distributed in the northwest and south of LAN and the southwest of LFS. Low BC concentration is closely related to air mass from the sea. In winter, the source regions of BC are concentrated in the west and south of LAN and the northeast of the threshold area of stot at LFS. The cold air mass in the northwest plays an important role in the purification of atmospheric BC. On a yearly scale, sources of BC are approximately from five provinces in the northwest/southeast of LAN and the west of LFS. These findings are helpful in reducing BC emission and con- trolling air pollution.

Comparison of Submicron Particles at a Rural and an Urban Site in the North China Plain during the December 2016 Heavy Pollution Episodes

An extensive field experiment for measurement of physical and chemical properties of aerosols was conducted at an urban site in the Chinese Academy of Meteorological Sciences（CAMS） in Beijing and at a rural site in Gucheng（GC）, Hebei Province in December 2016. This paper compares the number size distribution of submicron particle matter（PM1, diameter 〈 1 μm） between the two sites. The results show that the mean PM1 number concentration at GC was twice that at CAMS, and the mass concentration was three times the amount at CAMS. It is found that the accumulation mode（100–850 nm） particles constituted the largest fraction of PM1 at GC, which was significantly correlated with the local coal combustion, as confirmed by a significant relationship between the accumulation mode and the absorption coefficient of soot particles. The high PM1 concentration at GC prevented the occurrence of new particle formation（NPF） events, while eight such events were observed at CAMS. During the NPF events, the mass fraction of sulfate increased significantly, indicating that sulfate played an important role in NPF. The contribution of regional transport to PM1 mass concentration was approximately 50% at both sites, same as that of the local emission. However, during the red-alert period when emission control took place, the contribution of regional transport was notably higher.

Chemical Components, Variation, and Source Identification of PM1 during the Heavy Air Pollution Episodes in Beijing in December 2016

Air pollution is a current global concern. The heavy air pollution episodes（HPEs） in Beijing in December 2016 severely influenced visibility and public health. This study aims to survey the chemical compositions, sources, and formation processes of the HPEs. An aerodyne quadruple aerosol mass spectrometer（Q-AMS） was utilized to measure the non-refractory PM1（NR-PM1） mass concentration and size distributions of the main chemical components including organics, sulfate, nitrate, ammonium, and chloride in situ during 15–23 December 2016. The NR-PM1 mass concentration was found to increase from 6 to 188 μg m–3 within 5 days. During the most serious polluted episode, the PM1 mass concentration was about 2.6 times that during the first pollution stage and even 40 times that of the clean days. The formation rates of PM2.5 in the five pollution stages were 26, 22, 22, 32, and 67 μg m^（–3） h–1, respectively. Organics and nitrate occupied the largest proportion in the polluted episodes, whereas organics and sulfate dominated the submicron aerosol during the clean days. The size distribution of organics is always broader than those of other species, especially in the clean episodes. The peak sizes of the interested species grew gradually during different HPEs. Aqueous reaction might be important in forming sulfate and chloride, and nitrate was formed via oxidization and condensation processes. PMF（positive matrix factorization） analysis on AMS mass spectra was employed to separate the organics into different subtypes. Two types of secondary organic aerosol with different degrees of oxidation consisted of 43% of total organics. By contrast, primary organics from cooking, coal combustion, and traffic emissions comprised 57% of the organic aerosols during the HPEs.

Equilibrium Climate Response of the East Asian Summer Monsoon to Forcing of Anthropogenic Aerosol Species

We used an online aerosol-climate model to study the equilibrium climate response of the East Asian summer monsoon （EASM） to increases in anthropogenic emissions of sulfate, organic carbon, and black carbon aerosols from 1850 to 2000. Our results show that each of these aerosol species has a different effect on the EASM as a result of changes in the local sea-land thermal contrast and atmospheric circulation. The increased emission of sulfate aerosol leads to a decrease in the thermal contrast between the land and ocean, a southward shift of the East Asian subtropical jet, and significant northerly wind anomalies at 850 hPa over eastern China and the ambient oceans, markedly dampening the EASM. An increase in organic carbon aerosol results in pronounced surface cooling and the forma- tion of an anomalous anticyclone over the oceans north of 30°N. These effects cause a slight increase in the sea-land thermal contrast and southerly flow anomalies to the west of the anticyclonic center, strengthening the northern EASM. An increase in organic carbon emission decreases the sea-land thermal contrast over southern China, which weakens the southern EASM. The response of the summer 850-hPa winds and rainfall over the East Asian monsoon region to an increase in black carbon emission is generally consistent with the response to an increase in organic carbon. The increase in black carbon emission leads to a strengthening of the northern EASM north of 35°N and a slight weakening of the southern EASM south of 35°N. The simulated response of the EASM to the increase in black carbon emission is unchanged when the emission of black carbon is scaled up by five times its year 2000 levels, although the intensities of the response is enhanced. The increase in sulfate emission primarily weakens the EASM, whereas the increases in black carbon and organic carbon emissions mitigate weakening of the northern EASM.

Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation,Condensation/Coagulation, and Deposition with the GRAPES–CUACE

A coupled aerosol–cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission,which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES–CUACE [Global/Regional Assimilation and Pr Ediction System–China Meteorological Administration（CMA） Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES–CUACE simulations were verified against observational data during 1–31 January 2013, when a series of heavy regional haze–fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced,leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient grew from 0.35 to 0.61, and the mean mass concentration went up from 43% to 87.5% of the observed value. Thus, the simulation of particulate matters in these areas has been improved considerably.