Yongchun Liu

Huzhou Vocational and Technical College

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Markku Kulmala

University of Helsinki

Chao Yan

Nanjing University

Hong He

Chinese Academy of Sciences

Biwu Chu

University of Chinese Academy of Sciences

Federico Bianchi

University of Helsinki

Veli‐Matti Kerminen

University of Helsinki

Jingkun Jiang

Tsinghua University

Feixue Zheng

Beijing University of Chemical Technology

Tuukka Petäjä

University of Helsinki

Kaspar R. Daellenbach

University of Helsinki

Cooperative Institutions

Chinese Academy of Sciences

187

University of Chinese Academy of Sciences

103

University of Helsinki

Beijing University of Chemical Technology

State Key Joint Laboratory of Environment Simulation and Pollution Control

Tsinghua University

Institute of Atmospheric Physics

Nanjing University

Research Center for Eco-Environmental Sciences

Peking University

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Size-resolved particle number emissions in Beijing determined from measured particle size distributions

Atmospheric chemistry and physics (2020)

Jenni Kontkanen Chenjuan Deng Yueyun Fu Lubna Dada Ying Zhou

Abstract. The climate and air quality effects of aerosol particles depend on the number and size of the particles. In urban environments, a large fraction of aerosol particles originates from anthropogenic emissions. To evaluate the effects of different pollution sources on air quality, knowledge of size distributions of particle number emissions is needed. Here we introduce a novel method for determining size-resolved particle number emissions, based on measured particle size distributions. We apply our method to data measured in Beijing, China, to determine the number size distribution of emitted particles in a diameter range from 2 to 1000 nm. The observed particle number emissions are dominated by emissions of particles smaller than 30 nm. Our results suggest that traffic is the major source of particle number emissions with the highest emissions observed for particles around 10 nm during rush hours. At sizes below 6 nm, clustering of atmospheric vapors contributes to calculated emissions. The comparison between our calculated emissions and those estimated with an integrated assessment model GAINS (Greenhouse Gas and Air Pollution Interactions and Synergies) shows that our method yields clearly higher particle emissions at sizes below 60 nm, but at sizes above that the two methods agree well. Overall, our method is proven to be a useful tool for gaining new knowledge of the size distributions of particle number emissions in urban environments and for validating emission inventories and models. In the future, the method will be developed by modeling the transport of particles from different sources to obtain more accurate estimates of particle number emissions.

Particle (ecology)

10.5194/acp-20-11329-2020

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Citations (52)

Resolving Atmospheric Oxygenated Organic Molecules in Urban Beijing Using Online Ultrahigh-Resolution Chemical Ionization Mass Spectrometry

Environmental Science & Technology (2024)

Yi Yuan Xin Chen Runlong Cai Xiaoxiao Li Yuyang Li

Gaseous oxygenated organic molecules (OOMs) are crucial precursors of atmospheric organic aerosols. OOMs in urban atmospheres have complex compositions, posing challenges to understanding their formation, evolution, and influences. In this study, we identify 2403 atmospheric gaseous OOMs in urban Beijing using online nitrate-based chemical ionization Orbitrap mass spectrometry based on one-year atmospheric measurements. We find that OOMs in urban atmospheres can be identified with higher accuracy and wider coverage, compared to previously used online mass spectrometry. With optimized OOM resolving capabilities, previous knowledge of OOMs in urban atmospheres can be expanded. First, clear homologous and oxygen-addition characteristics of the OOMs are revealed. Second, OOMs with lower concentrations or higher masses are identified and characterized with high confidence, e.g., OOMs with masses above 350 Da. In particular, dimers of OOMs (e.g., C

Atmospheric-pressure chemical ionization

Organic molecules

Desorption electrospray ionization

10.1021/acs.est.4c04214

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Ozonolysis of Trimethylamine Exchanged with Typical Ammonium Salts in the Particle Phase

Environmental Science & Technology (2016)

Yanli Ge Yongchun Liu Biwu Chu Hong He Tianzeng Chen

Alkylamines contribute to both new particle formation and brown carbon. The toxicity of particle-phase amines is of great concern in the atmospheric chemistry community. Degradation of particulate amines may lead to secondary products in the particle phase, which are associated with changes in the adverse health impacts of aerosols. In this study, O3 oxidation of particulate trimethylamine (TMA) formed via heterogeneous uptake of TMA by (NH4)2SO4, NH4HSO4, NH4NO3 and NH4Cl, was investigated with in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and proton transfer reaction mass spectrometry (PTR-MS). HCOOH, HCHO, CH3N═CH2, (CH3)2NCHO, CH3NO2, CH3N(OH)CHO, CH3NHOH and H2O were identified as products on all the substrates based upon IR (one-dimensional IR and two-dimensional correlation infrared spectroscopy), quantum chemical calculation and PTR-MS results. A reaction mechanism was proposed to explain the observed products. This work demonstrates that oxidation might be a degradation pathway of particulate amines in the atmosphere. This will aid in understanding the fate of particulate amines formed by nucleation and heterogeneous uptake and their potential health impacts during atmospheric aging.

Particle (ecology)

Attenuated total reflection

10.1021/acs.est.6b04375

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Citations (22)

Supplementary material to "Influence of organic aerosol composition determined by offline FIGAERO-CIMS on particle absorptive properties in autumn Beijing"

Jing Cai Cheng Wu Jiandong Wang Wei Du Feixue Zheng

Particle (ecology)

10.5194/acp-2021-528-supplement

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Precursor apportionment of atmospheric oxygenated organic molecules using a machine learning method

Environmental Science Atmospheres (2022)

Xiaohui Qiao Xiaoxiao Li Chao Yan Nina Sarnela Rujing Yin

Machine learning is a promising tool in atmospheric chemistry to connect atmospheric oxygenated organic molecules with their precursors.

Organic molecules

Apportionment

Atmospheric chemistry

Atmospheric Composition

10.1039/d2ea00128d

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Citations (4)

Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol-chemistry-radiation-boundary layer interaction

Zhuohui Lin Yonghong Wang Feixue Zheng Ying Zhou Yishuo Guo

Abstract. Despite the numerous studies investigating haze formation mechanism in China, it is still puzzling that intensive haze episodes could form within hours directly following relatively clean periods. Haze has been suggested to be initiated by the variation of meteorological parameters and then to be substantially enhanced by aerosol-radiation-boundary layer feedback. However, knowledge on the detailed chemical processes and the driving factors for extensive aerosol mass accumulation during the feedback is still scarce. Here, the dependency of the aerosol number size distribution, mass concentration and chemical composition on the daytime mixing layer height (MLH) in urban Beijing is investigated. The size distribution and chemical composition-resolved dry aerosol light extinction is also explored. The results indicate that the aerosol mass concentration and fraction of nitrate increased dramatically when the MLH decreased from high to low conditions, corresponding to relatively clean and polluted conditions, respectively. Particles having their dry diameters in the size of ~ 400–700 nm, and especially particle-phase ammonium nitrate and liquid water, contributed greatly to visibility degradation during the winter haze periods. The dependency of aerosol composition on the MLH revealed that ammonium nitrate and aerosol water content increased the most during low MLH conditions, which may have further triggered enhanced formation of sulphate and organic aerosol via heterogeneous reactions. As a result, more sulphate, nitrate and water soluble organics were formed, leading to an enhanced water uptake ability and increased light extinction by the aerosols. The results of this study contribute towards a more detailed understanding of the aerosol-chemistry-radiation-boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.

Haze

Extinction (optical mineralogy)

Ammonium nitrate

Particle (ecology)

Ammonium sulfate

Mass concentration (chemistry)

Liquid water content

10.5194/acp-2020-223

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The semi-solid phase of atmospheric particles facilitates the formation of secondary brown carbon: possible contribution of ionic strength to Maillard-like reactions

Atmospheric Environment (2024)

Jiali Xie Feixue Zheng Yusheng Zhang Yuzheng Wang Penghan Wang

Carbon fibers

10.1016/j.atmosenv.2024.120991

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Secondary aerosol formation and oxidation capacity in photooxidation in the presence of Al2O3 seed particles and SO2

Science China Chemistry (2015)

Biwu Chu Tengyu Liu Xiao Zhang Yongchun Liu Qingxin Ma

10.1007/s11426-015-5456-0

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Citations (16)

Influence of metal-mediated aerosol-phase oxidation on secondary organic aerosol formation from the ozonolysis and OH-oxidation of α-pinene

Scientific Reports (2017)

Biwu Chu John Liggio Yongchun Liu Hong He Hideto Takekawa

Abstract The organic component is the most abundant fraction of atmospheric submicron particles, while the formation mechanisms of secondary organic aerosol (SOA) are not fully understood. The effects of sulfate seed aerosols on SOA formation were investigated with a series of experiments carried out using a 9 m 3 smog chamber. The presence of FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols decreased SOA yields and increased oxidation levels in both ozonolysis and OH-oxidation of α-pinene compared to that in the presence of ZnSO 4 or (NH 4 ) 2 SO 4 . These findings were explained by metal-mediated aerosol-phase oxidation of organics: reactive radicals were generated on FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols and reacted further with the organic mass. This effect would help to explain the high O/C ratios of organics in ambient particles that thus far cannot be reproduced in laboratory and model studies. In addition, the gap in the SOA yields between experiments with different seed aerosols was more significant in OH-oxidation experiments compared to ozonolysis experiments, while the gap in estimated O/C ratios was less obvious. This may have resulted from the different chemical compositions and oxidation levels of the SOA generated in the two systems, which affect the branching ratio of functionalization and fragmentation during aerosol oxidation.

Pinene

10.1038/srep40311

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Citations (25)

The role of NOx in Co-occurrence of O3 and PM2.5 pollution driven by wintertime east Asian monsoon in Hainan

Journal of Environmental Management (2023)

Junlei Zhan Feixue Zheng Rongfu Xie Jun Liu Biwu Chu

Particulate Pollution

10.1016/j.jenvman.2023.118645

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Citations (5)