scholarly journals Temporal variations in the hygroscopicity and mixing state of black carbon aerosols in a polluted megacity area

2018 ◽  
Vol 18 (20) ◽  
pp. 15201-15218 ◽  
Author(s):  
Kangning Li ◽  
Xingnan Ye ◽  
Hongwei Pang ◽  
Xiaohui Lu ◽  
Hong Chen ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Black Carbon ◽  
Single Particle ◽  
Radiative Forcing ◽  
Temporal Variations ◽  
Mixing State ◽  
Atmospheric Aging ◽  
Secondary Organic Carbon ◽  
Bc Aerosols ◽  
Mixing States

Abstract. Black carbon (BC) aerosols in the atmosphere strongly affect radiative forcing. They are mainly removed from the air by wet deposition, and their lifetime is controlled by their water uptake ability or hygroscopicity, which is a function of aerosol mixing states. It is well known that atmospheric aging processes coat various materials on BC aerosols and affect their mixing states and hygroscopicity. However, detailed relations between the aging processes and the hygroscopicity and mixing state of BC aerosol particles in polluted city areas are not well understood. Here, we studied the temporal variation in hygroscopicity and its correlation with the mixing state of ambient BC particles during the summer of 2017 in Shanghai, China, using a hygroscopic tandem differential mobility analyzer inline with a single-particle soot photometer (HTDMA–SP2 system) as well as a single-particle aerosol mass spectrometer (SPAMS). BC particles with 120, 240, and 360 nm in dry diameter were humidified at relative humidity (RH)  =  85 %. After humidification, particles with growth factors (GFs) of 1.0, 1.2, and 1.4, representing the BC particles with different hygroscopicities (hydrophobic, transition, and hydrophilic modes, respectively), were analyzed with a SP2 to obtain their BC mixing states. The diurnal trends in coating thickness and chemical mixing state show that coating materials of BC particles were distinct between daytime and nighttime. The differences were associated with the hygroscopicity of BC particles. Single-particle mass spectrometry and other chemical characterization techniques revealed that with lower temperature and higher RH during nighttime, formation or condensation of nitrates resulted in an enhanced hygroscopicity of BC particles. During daytime, secondary organic carbon formation was mainly responsible for the change of hygroscopicity of BC particles. Due to the high hygroscopicity of inorganic nitrate, a thinner nitrate coating on BC particles could convert fresh BC particles to aged hygroscopic ones during nighttime while a thicker coating layer of secondary materials was required to reach the same overall hygroscopicity during daytime because of the participation of secondary organic carbon. Different atmospheric aging processes between daytime and nighttime led to the change of BC particles' mixing states, which play a fundamental role in determining their hygroscopicity. To our knowledge, this is the first report of links between temporal variations in the hygroscopic growth of BC particles and atmospheric aging processes in polluted environments. These findings have significant ramifications in understanding the aging process, wet removal, and climate effects of BC particles.

scholarly journals Temporal variations of the hygroscopicity and mixing state of black carbon aerosols in a polluted megacity area

2018 ◽  
Author(s):  
Kangning Li ◽  
Xingnan Ye ◽  
Hongwei Pang ◽  
Xiaohui Lu ◽  
Hong Chen ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Black Carbon ◽  
Single Particle ◽  
Radiative Forcing ◽  
Temporal Variations ◽  
Mixing State ◽  
Atmospheric Aging ◽  
Secondary Organic Carbon ◽  
Bc Aerosols ◽  
Mixing States

Abstract. Black carbon (BC) aerosols in the atmosphere strongly affect radiative forcing. They are mainly removed from the air by wet deposition, and their lifetime is controlled by their water uptake ability or hygroscopicity, which is a function of the aerosol mixing states. It is well known that atmospheric aging processes coat various materials on BC aerosols and affect their mixing states and hygroscopicity. However, detailed relations between the aging processes, the hygroscopicity and mixing state of BC aerosol particles in polluted city areas are not well understood. Here, we studied the temporal variation of the hygroscopicity and its correlation with the mixing state of ambient BC particles during 2017 summer in Shanghai, China using a hygroscopicity tandem differential mobility analyzer in-line with a single particle soot photometer (HTDMA-SP2 system) as well as a single particle aerosol mass spectrometer (SPAMS). BC particles with 120 nm, 240 nm and 360 nm dry diameter were humidified at RH = 85 %. After humidification, particles with growth factors (GFs) of 1.0, 1.2 and 1.4, representing the BC particles with different hygroscopicities (hydrophobic, transition and hydrophilic modes, respectively), were analyzed by a SP2 to obtain their BC mixing states. The diurnal trends of coating thickness and chemical mixing state show that coating materials of BC particles were distinct between daytime and nighttime. The differences were associated with the hygroscopicity of BC particles. Single particle mass spectrometry and other chemical characterization techniques revealed that during nighttime with lower temperature and higher relative humidity (RH), formation or condensation of nitrates resulted in an enhanced hygroscopicity of BC particles. During daytime, secondary organic carbon formation was mainly responsible for the change of hygroscopicity of BC particles. Due to the high hygroscopicity of inorganic nitrate, a thinner nitrate coating on BC particles could convert fresh BC particles to aged hygroscopic ones during nighttime while a thicker coating layer of secondary materials was required to reach the same overall hygroscopicity during daytime since the participation of secondary organic carbon. Different atmospheric aging processes between daytime and nighttime led to the change of BC particles' mixing states, which play a fundamental role in determining their hygroscopicity. To our knowledge, this is the first report of links between temporal variations of the hygroscopic growth of BC particles and atmospheric aging processes in polluted environment. These findings have significant ramification of understanding the aging process, wet removal as well as climate effects of BC particles.

scholarly journals Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

2019 ◽  
Vol 19 (4) ◽  
pp. 2183-2207 ◽  
Author(s):  
Ghislain Motos ◽  
Julia Schmale ◽  
Joel C. Corbin ◽  
Marco Zanatta ◽  
Urs Baltensperger ◽  
...  
Keyword(s):  
Black Carbon ◽  
Single Particle ◽  
Radiative Forcing ◽  
Mixing State ◽  
Scanning Mobility Particle Sizer ◽  
Carbon Particles ◽  
Kohler Theory ◽  
Droplet Activation ◽  
Aerosol Cloud Interactions ◽  
A Minor

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased diameter and hygroscopicity, facilitating droplet activation. This affects BC radiative forcing through aerosol–cloud interactions (ACIs) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015–2016 in a residential area of Zurich which aimed at establishing relations between the size and mixing state of BC particles and their activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single-particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that in the morning hours of weekdays, the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles, which do not act as CCN within the CCNC. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 % and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 % to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have very similar activation behaviour to BC-free particles. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core–shell particle geometry constrained with single-particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size- and mixing-state-resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

scholarly journals Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

2018 ◽  
Author(s):  
Ghislain Motos ◽  
Julia Schmale ◽  
Joel Christopher Corbin ◽  
Marco Zanatta ◽  
Urs Baltensperger ◽  
...  
Keyword(s):  
Black Carbon ◽  
Single Particle ◽  
Radiative Forcing ◽  
Cloud Condensation Nuclei ◽  
Mixing State ◽  
Scanning Mobility Particle Sizer ◽  
Carbon Particles ◽  
Hygroscopic Properties ◽  
Droplet Activation ◽  
Aerosol Cloud Interactions

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased hygroscopicity as well as diameter, facilitating droplet activation. This affects BC radiative forcing through aerosol-cloud interactions (aci) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015/16 in a residential area of Zurich which aimed at distinguishing different particle mixing states regarding hygroscopic properties in the cloud condensation nuclei (CCN)-activated fraction spectrum of urban aerosol and establishing relations between the mixing state of BC and its activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that, depending on the time of the day, we sampled both heavily aged internally mixed BC from background air advected to the site and freshly emitted externally mixed BC from local or regional traffic sources. During rush hours in the morning of weekdays, we found clear evidence that the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles which do not act as CCN within the CCNC. The mixing state of BC particles was also found to play a key role in their ability to form fog droplets. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have a very similar activation behavior as BC-free particles. The threshold coating thickness required for activation was shown to decrease with increasing BC core size. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core-shell particle geometry constrained with single particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size and mixing state resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

scholarly journals The single-particle mixing state and cloud scavenging of black carbon at a high-altitude mountain site in southern China

2017 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Xinhui Bi ◽  
Duohong Chen ◽  
...  
Keyword(s):  
Black Carbon ◽  
Single Particle ◽  
Southern China ◽  
Climate Impacts ◽  
Limited Information ◽  
Mixing State ◽  
Cloud Droplets ◽  
Mountain Site ◽  
Cloud Scavenging ◽  
Scavenging Efficiency

Abstract. In the present study, a ground-based counterflow virtual impactor (GCVI) was used to sample cloud droplet residual (cloud RES) particles, while a parallel PM2.5 inlet was used to sample cloud-free or cloud interstitial (cloud INT) particles. The mixing state of black carbon (BC)-containing particles in a size range of 0.1–1.6 µm and the mass concentrations of BC in the cloud-free, RES and INT particles were investigated using a single particle aerosol mass spectrometer (SPAMS) and two aethalometers, respectively, at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and were activated into cloud droplets to the same extent as all the measured particles. The results indicate the preferential activation of larger particles and/or that the production of secondary compositions shifts the BC-containing particles towards larger sizes. BC-containing particles with an abundance of both sulfate and organics were activated less than those with sulfate but limited organics, implying the importance of the mixing state on the incorporation of BC-containing particles into cloud droplets. The mass scavenging efficiency of BC with an average of 33 % was similar for different cloud events independent of the air mass. This is the first time that both the mixing state and cloud scavenging of BC in China have been reported. Since limited information on BC-containing particles in the free troposphere is available, the results also provide an important reference for the representation of BC concentrations, properties, and climate impacts in modeling studies.

scholarly journals Size distribution and coating thickness of black carbon from the Canadian oil sands operations

2017 ◽  
Author(s):  
Yuan Cheng ◽  
Shao-Meng Li ◽  
Mark Gordon ◽  
Peter Liu
Keyword(s):  
Size Distribution ◽  
Black Carbon ◽  
Coating Thickness ◽  
Oil Sands ◽  
Radiative Forcing ◽  
Climate Models ◽  
Source Area ◽  
Size Distributions ◽  
Mixing State ◽  
Earth’S Climate

Abstract. Black carbon (BC) plays an important role in the Earth’s climate system. However, parameterization of BC size and mixing state have not been well addressed in aerosol-climate models, introducing substantial uncertainties into the estimation of radiative forcing by BC. In this study, we focused on BC emissions from the massive oil sands (OS) industry in northern Alberta, based on an aircraft campaign conducted over the Athabasca OS region in 2013. A total of 14 flights were made over the OS source area, in which the aircraft was typically flown in a 4- or 5-sided polygon pattern along flight tracks encircling an OS facility. Another 3 flights were performed downwind of the OS source area, each of which involved at least three intercepting locations where the well-mixed OS plume was measured along flight tracks perpendicular to the wind direction. Comparable size distributions were observed for refractory black carbon (rBC) over and downwind of the OS facilities, with rBC mass median diameters (MMD) between ~ 135 and 145 nm that were characteristic of fresh urban emissions. This MMD range corresponded to rBC number median diameters (NMD) of ~ 60–70 nm, approximately 100 % higher than the NMD settings in some aerosol-climate models. The typical in- and out-of-plume segments of a flight, which had different rBC concentrations and photochemical ages, showed consistent rBC size distributions. Moreover, rBC size distributions remained unchanged at different downwind distances from the source area, suggesting that atmospheric aging would not necessarily change rBC size distribution. However, aging indeed influenced rBC mixing state. Coating thickness for rBC cores in the diameter range of 130–160 nm was nearly doubled within three hours when the OS plume was transported over a distance of 90 km from the source area.

scholarly journals Simulations of Black Carbon Over Indian Region: Improvements and Implications of Diurnality in Emissions

2019 ◽  
Author(s):  
Gaurav Govardhan ◽  
Sreedharan Krishnakumari Satheesh ◽  
Krishnaswamy Krishna Moorthy ◽  
Ravi Nanjundiah
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Regional Scale ◽  
Early Morning ◽  
Temporal Variations ◽  
Indian Region ◽  
Near Surface ◽  
Aerosol Radiative Forcing ◽  
Convective Mixing

Abstract. With a view to improving the performance of WRF-Chem over the Indian region in simulating BC (black Carbon) mass concentrations as well as its short-term variations, especially on diurnal scale, a region-specific diurnal variation scheme has been introduced in the model emissios and the performance of the modified simulations has been evaluated against high-resolution measurements carried out over 8 ARFI (Aerosol Radiative Forcing over India) network observatories spread across India for distinct seasons; pre-monsoon (represented by May), post-monsoon (represented by October) and winter (represented by December). In addition to an overall improvement in the simulated concentrations and their temporal variations, it has also been found that the effects of prescribing diurnally varying emissions on the simulated near-surface concentrations largely depend on the boundary layer turbulence. The effects are perceived fast (within about 2–3 hours) during the evening–early morning hours when the atmospheric boundary layer is shallow and convective mixing is weak, while they are delayed, taking as much as about 5–6 hours, during periods when the boundary layer is deep and convective mixing is strong. This information would also serve as an important input for agencies concerned with urban planning and pollution mitigation. Despite these improvements in the near-surface concentrations, the simulated columnar aerosol optical depth (AOD) still remains largely underestimated vis-a-vis the satellite retrieved products. These modifications will serve as a guideline for further model-improvement initiatives at regional scale.

scholarly journals Simulations of black carbon over the Indian region: improvements and implications of diurnality in emissions

2019 ◽  
Vol 19 (12) ◽  
pp. 8229-8241 ◽  
Author(s):  
Gaurav Govardhan ◽  
Sreedharan Krishnakumari Satheesh ◽  
Krishnaswamy Krishna Moorthy ◽  
Ravi Nanjundiah
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Regional Scale ◽  
Early Morning ◽  
Temporal Variations ◽  
Indian Region ◽  
Near Surface ◽  
Aerosol Radiative Forcing ◽  
Convective Mixing

Abstract. With a view to improving the performance of WRF-Chem over the Indian region in simulating BC (black carbon) mass concentrations as well as its short-term variations, especially on a diurnal scale, a region-specific diurnal variation scheme has been introduced in the model emissions and the performance of the modified simulations has been evaluated against high-resolution measurements carried out over eight ARFI (Aerosol Radiative Forcing over India) network observatories spread across India for distinct seasons: pre-monsoon (represented by May), post-monsoon (represented by October) and winter (represented by December). In addition to an overall improvement in the simulated concentrations and their temporal variations, we have also found that the effects of prescribing diurnally varying emissions on the simulated near-surface concentrations largely depend on the boundary layer turbulence. The effects are perceived quickly (within about 2–3 h) during the evening–early morning hours when the atmospheric boundary layer is shallow and convective mixing is weak, while they are delayed, taking as much as about 5–6 h, during periods when the boundary layer is deep and convective mixing is strong. This information would also serve as an important input for agencies concerned with urban planning and pollution mitigation. Despite these improvements in the near-surface concentrations, the simulated columnar aerosol optical depth (AOD) still remains largely underestimated vis-à-vis the satellite-retrieved products. These modifications will serve as a guideline for further model-improvement initiatives at a regional scale.

scholarly journals Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments

2016 ◽  
Vol 113 (16) ◽  
pp. 4266-4271 ◽  
Author(s):  
Jianfei Peng ◽  
Min Hu ◽  
Song Guo ◽  
Zhuofei Du ◽  
Jing Zheng ◽  
...  
Keyword(s):  
Developing Countries ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Urban Environments ◽  
Absorption Enhancement ◽  
Ambient Conditions ◽  
Climatic Impact ◽  
Atmospheric Aging ◽  
Enhanced Absorption ◽  
Direct Radiative Forcing

Black carbon (BC) exerts profound impacts on air quality and climate because of its high absorption cross-section over a broad range of electromagnetic spectra, but the current results on absorption enhancement of BC particles during atmospheric aging remain conflicting. Here, we quantified the aging and variation in the optical properties of BC particles under ambient conditions in Beijing, China, and Houston, United States, using a novel environmental chamber approach. BC aging exhibits two distinct stages, i.e., initial transformation from a fractal to spherical morphology with little absorption variation and subsequent growth of fully compact particles with a large absorption enhancement. The timescales to achieve complete morphology modification and an absorption amplification factor of 2.4 for BC particles are estimated to be 2.3 h and 4.6 h, respectively, in Beijing, compared with 9 h and 18 h, respectively, in Houston. Our findings indicate that BC under polluted urban environments could play an essential role in pollution development and contribute importantly to large positive radiative forcing. The variation in direct radiative forcing is dependent on the rate and timescale of BC aging, with a clear distinction between urban cities in developed and developing countries, i.e., a higher climatic impact in more polluted environments. We suggest that mediation in BC emissions achieves a cobenefit in simultaneously controlling air pollution and protecting climate, especially for developing countries.

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