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High levels of ultrafine particles (UFPs; diameter of less than 50 nm) are frequently produced from new particle formation under urban conditions, with profound implications on human health, weather, and climate. However, the fundamental mechanisms of new particle formation remain elusive, and few experimental studies have realistically replicated the relevant atmospheric conditions. Previous experimental studies simulated oxidation of one compound or a mixture of a few compounds, and extrapolation of the laboratory results to chemically complex air was uncertain. Here, we show striking formation of UFPs in urban air from combining ambient and chamber measurements. By capturing the ambient conditions (i.e., temperature, relative humidity, sunlight, and the types and abundances of chemical species), we elucidate the roles of existing particles, photochemistry, and synergy of multipollutants in new particle formation. Aerosol nucleation in urban air is limited by existing particles but negligibly by nitrogen oxides. Photooxidation of vehicular exhaust yields abundant precursors, and organics, rather than sulfuric acid or base species, dominate formation of UFPs under urban conditions. Recognition of this source of UFPs is essential to assessing their impacts and developing mitigation policies. Our results imply that reduction of primary particles or removal of existing particles without simultaneously limiting organics from automobile emissions is ineffective and can even exacerbate this problem., Competing Interests: The authors declare no competing interest., (Copyright © 2020 the Author(s). Published by PNAS.)

Particle density is an important physical property of atmospheric particles. The information on high time-resolution size-resolved particle density is essential for understanding the atmospheric physical and chemical aging processes of aerosols particles. In the present study, a centrifugal particle mass analyzer (CPMA) combined with a differential mobility analyzer (DMA) was deployed to determine the size-resolved effective density of 50 to 350nm particles at a rural site of Beijing during summer 2016. The measured particle effective densities decreased with increasing particle sizes and ranged from 1.43 to 1.55g/cm 3 , on average. The effective particle density distributions were dominated by a mode peaked at around 1.5g/cm 3 for 50 to 350nm particles. Extra modes with peaks at 1.0, 0.8, and 0.6g/cm 3 for 150, 240, and 350nm particles, which might be freshly emitted soot particles, were observed during intensive primary emissions episodes. The particle effective densities showed a diurnal variation pattern, with higher values during daytime. A case study showed that the effective density of Aitken mode particles during the new particle formation (NPF) event decreased considerably, indicating the significant contribution of organics to new particle growth., (Copyright © 2018. Published by Elsevier B.V.)

Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO 2 by NO 2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH 3 neutralization or under cloud conditions. Under polluted environments, this SO 2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH 3 and NO 2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world., Competing Interests: The authors declare no conflict of interest.

As has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO3-) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM 1 (NR-PM 1) being up to 44 % during wintertime in Beijing. Based on this typical pNO3- -dominated haze event, the linkage between aerosol water uptake and pNO3- enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ∼10 % to 70 %, the aerosol particle liquid water increased from ∼1 µgm-3 at the beginning to ∼75 µgm-3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO3- is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP. [ABSTRACT FROM AUTHOR]

Abstract To investigate aerosol optical properties relevant to pollutant level controls in place in Beijing, particulate matters with diameter <2.5 μm (PM 2.5) mass concentration, aerosol absorption ( σ a p ) and scattering ( σ s p ) coefficients were continuously measured from January 2014 to March 2017 at an urban site Peking University Atmosphere Environment MonitoRing Station (PKUERS). Our results showed that PM 2.5 , σ a p , and σ s p all decreased, especially from 2014 to 2015. Note that, a significant decrease of σ a p in autumn and σ s p in winter was responsible for the decrease of the year by year average. PM 2.5 , σ a p and σ s p exhibited a pronounced bi-peak diurnal variation, which was attributed to the traffic emissions. The wind dependence analysis revealed that σ a p was mainly influenced by local emissions but σ s p was influenced by both local emissions and regional transport. The potential spatial source origins of σ s p in Beijing were investigated using the potential source contribution function (PSCF). The results indicated that the potential source regions that influence σ s p of Beijing were mainly from south and west of Beijing but slightly varied with different years and seasons. Highlights • 3-year aerosol optical property data of Beijing were analyzed to investigate aerosol optical properties relevant to pollutant level controls in place in Beijing. • Influencing factors of aerosol optical properties were explored. • PSCF was applied to identify the potential source origins of the aerosol optical properties. [ABSTRACT FROM AUTHOR]

Nitro-aromatic compounds (NACs), as important contributors to the light absorption by brown carbon, have been widely observed in various ambient atmospheres; however, their formation in the urban atmosphere was little studied. In this work, we report an intensive field study of NACs in summer 2016 at an urban Beijing site, characterized by both high- NOx and anthropogenic VOC dominated conditions. We investigated the factors that influence NAC formation (e.g., NO2 , VOC precursors, RH and photolysis) through quantification of eight NACs, along with major components in fine particulate matter, selected volatile organic compounds, and gases. The average total concentration of the quantified NACs was 6.63 ng m -3 , higher than those reported in other summertime studies (0.14–6.44 ng m -3). 4-Nitrophenol (4NP, 32.4 %) and 4-nitrocatechol (4NC, 28.5 %) were the top two most abundant NACs, followed by methyl-nitrocatechol (MNC), methyl-nitrophenol (MNP), and dimethyl-nitrophenol (DMNP). The oxidation of toluene and benzene in the presence of NOx was found to be a more dominant source of NACs than primary biomass burning emissions. The NO2 concentration level was found to be an important factor influencing the secondary formation of NACs. A transition from low- to high- NOx regimes coincided with a shift from organic- to inorganic-dominated oxidation products. The transition thresholds were NO2∼20 ppb for daytime and NO2∼25 ppb for nighttime conditions. Under low- NOx conditions, NACs increased with NO2 , while the NO3- concentrations and (NO3-)/NACs ratios were lower, implying organic-dominated products. Under high- NOx conditions, NAC concentrations did not further increase with NO2 , while the NO3- concentrations and (NO3-)/NACs ratios showed increasing trends, signaling a shift from organic- to inorganic-dominated products. Nighttime enhancements were observed for 3M4NC and 4M5NC, while daytime enhancements were noted for 4NP, 2M4NP, and DMNP, indicating different formation pathways for these two groups of NACs. Our analysis suggested that the aqueous-phase oxidation was likely the major formation pathway of 4M5NC and 3M5NC, while photo-oxidation of toluene and benzene in the presence of NO2 could be more important for the formation of nitrophenol and its derivatives. Using the (3M4NC + 4M5NC) / 4NP ratios as an indicator of the relative contribution of aqueous-phase and gas-phase oxidation pathways to NAC formation, we observed that the relative contribution of aqueous-phase pathways increased at elevated ambient RH and remained constant at RH > 30 %. We also found that the concentrations of VOC precursors (e.g., toluene and benzene) and aerosol surface area acted as important factors in promoting NAC formation, and photolysis as an important loss pathway for nitrophenols. [ABSTRACT FROM AUTHOR]

Gasoline vehicles significantly contribute to urban particulate matter (PM) pollution. Gasoline direct injection (GDI) engines, known for their higher fuel efficiency than that of port fuel injection (PFI) engines, have been increasingly employed in new gasoline vehicles. However, the impact of this trend on air quality is still poorly understood. Here, we investigated both primary emissions and secondary organic aerosol (SOA) formation from a GDI and a PFI vehicle under an urban-like driving condition, using combined approaches involving chassis dynamometer measurements and an environmental chamber simulation. The PFI vehicle emits slightly more volatile organic compounds, e.g., benzene and toluene, whereas the GDI vehicle emits more particulate components, e.g., total PM, elemental carbon, primary organic aerosols and polycyclic aromatic hydrocarbons. Strikingly, we found a much higher SOA production (by a factor of approximately 2.7) from the exhaust of the GDI vehicle than that of the PFI vehicle under the same conditions. More importantly, the higher SOA production found in the GDI vehicle exhaust occurs concurrently with lower concentrations of traditional SOA precursors, e.g., benzene and toluene, indicating a greater contribution of intermediate volatility organic compounds and semi-volatile organic compounds in the GDI vehicle exhaust to the SOA formation. Our results highlight the considerable potential contribution of GDI vehicles to urban air pollution in the future. [ABSTRACT FROM AUTHOR]