scholarly journals Characterising mass-resolved mixing state of black carbon in Beijing using a morphology-independent measurement method

2020 ◽  
Vol 20 (6) ◽  
pp. 3645-3661 ◽  
Author(s):  
Chenjie Yu ◽  
Dantong Liu ◽  
Kurtis Broda ◽  
Rutambhara Joshi ◽  
Jason Olfert ◽  
...  
Keyword(s):  
Black Carbon ◽  
Atmospheric Aerosols ◽  
Particle Morphology ◽  
Urban Site ◽  
Inversion Method ◽  
Mixing State ◽  
State Index ◽  
Cloud Scavenging ◽  
Highly Correlated ◽  
State Mixing

Abstract. Refractory black carbon (rBC) in the atmosphere is known for its significant impacts on climate. The relationship between the microphysical and optical properties of rBC remains poorly understood and is influenced by its size and mixing state. Mixing state also influences its cloud scavenging potential and thus atmospheric lifetime. This study presents a coupling of a centrifugal particle mass analyser (CPMA) and a single-particle soot photometer (SP2) for the morphology-independent quantification of the mixing state of rBC-containing particles, used in the urban site of Beijing as part of the Air Pollution and Human Health–Beijing (APHH-Beijing) project during winter (10 November–10 December 2016) and summer (18 May–25 June 2017). This represents a highly dynamic polluted environment with a wide variety of conditions that could be considered representative of megacity area sources in Asia. An inversion method (used for the first time on atmospheric aerosols) is applied to the measurements to present two-variable distributions of both rBC mass and total mass of rBC-containing particles and calculate the mass-resolved mixing state of rBC-containing particles, using previously published metrics. The mass ratio between non-rBC material and rBC material (MR) is calculated to determine the thickness of a hypothetical coating if the rBC and other material followed a concentric sphere model (the equivalent coating thickness). The bulk MR (MRbulk) was found to vary between 2 and 12 in winter and between 2 and 3 in summer. This mass-resolved mixing state is used to derive the mass-weighted mixing state index for the rBC-containing particles (χrBC). χrBC quantifies how uniformly the non-rBC material is distributed across the rBC-containing-particle population, with 100 % representing uniform mixing. The χrBC in Beijing varied between 55 % and 70 % in winter depending on the dominant air masses, and χrBC was highly correlated with increased MRbulk and PM1 mass concentration in winter, whereas χrBC in summer varied significantly (ranging 60 %–75 %) within the narrowly distributed MRbulk and was found to be independent of air mass sources. In some model treatments, it is assumed that more atmospheric ageing causes the BC to tend towards a more homogeneous mixture, but this leads to the conclusion that the MRbulk may only act as a predictor of χrBC in winter. The particle morphology-independent and mass-based information on BC mixing used in this and future studies can be applied to mixing-state-aware models investigating atmospheric rBC ageing.

scholarly journals Characterising Mass-resolved Mixing State of Black Carbon in Beijing Using a Morphology-Independent Measurement Method

2019 ◽  
Author(s):  
Chenjie Yu ◽  
Dantong Liu ◽  
Kurtis Broda ◽  
Rutambhara Joshi ◽  
Jason Olfert ◽  
...  
Keyword(s):  
Black Carbon ◽  
Formation Mechanism ◽  
Coating Thickness ◽  
Process Models ◽  
Urban Site ◽  
Pollution Level ◽  
Inversion Method ◽  
Mixing State ◽  
Coating Formation ◽  
Coating Formation Mechanism

Abstract. Refractory Black Carbon (rBC) in the atmosphere is known for its significant impact on the climate system in the atmosphere. The relationship between the microphysical and optical properties of rBC remain uncertain and are largely influenced by the size, coating thickness and mixing state of particles. This study presents a coupling of a centrifugal particle mass analyser (CPMA) and a single particle soot photometer (SP2) for the morphology-independent quantification of the mixing state of rBC-containing particles, used in the urban site of Beijing as part of the Air Pollution and Human Health-Beijing (APHH-Beijing) project during winter (10th Nov–10th Dec) and summer (18th May–25th June). An inversion method is applied to the measurements to present a two-variable distribution of both rBC core mass and total mass of rBC-containing particles and present the mass-resolved mixing state of rBC-containing particles. The mass ratio between non-rBC coating and rBC core (MR) is calculated to determine the coating thickness of the rBC-containing particles. The bulk MR was found to vary between 2–12 in winter and between 2–3 in summer. This mass-resolved mixing state is used to derive the mixing state index (χ) for the rBC-containing particles. χ quantifies whether the coating is evenly distributed across the rBC-containing particle population and is used to determine the degree of internal and external mixture of rBC-containing particles. The rBC-containing particles in Beijing were found to be 55%–70 % internally mixed in winter depending on the dominant air masses. χ of rBC-containing particles was highly positively associated with increased bulk MR, rBC mass loading or pollution level in winter, whereas χ of rBC-containing particles in summer varied significantly (ranging 60 %–75 %) within the narrowly-distributed bulk MR and was found to be independent of air mass sources. This concludes that the bulk MR may only act as a predictor of mixing state in winter, and χ is better to quantify the mixing state of rBC-containing particles. The same level of bulk MR corresponded with a higher χ in summer than in winter and this tended to suggest a limited formation of coatings on rBC largely depended on primary sources. However, with the higher Non-refractory PM1 (NR-PM1) concentration in winter, the coagulation process may still lead relative thick coatings. In summer the higher secondary compounds made the rBC-containing particles more homogeneous. But due to the higher temperatures and limited pollution level, the coating thickness in summer is limited. The mixing state of rBC-containing particles should also depend on the coating formation mechanism, both primary source influence and secondary coating formation mechanism should be considered in interpreting the rBC-containing particles mixing state in the atmosphere. This particle morphology-independent and mass-based data format as introduced in this study could be conviently applied in particle-resolved or other process models to investigate atmospheric rBC aging and mixing state properties.

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 Mixing characteristics of refractory black carbon aerosols determined by a tandem CPMA-SP2 system at an urban site in Beijing

2019 ◽  
Author(s):  
Hang Liu ◽  
Xiaole Pan ◽  
Dantong Liu ◽  
Xiaoyong Liu ◽  
Xueshun Chen ◽  
...  
Keyword(s):  
Black Carbon ◽  
Fractal Structure ◽  
Particle Mass ◽  
Shell Structures ◽  
Absorption Enhancement ◽  
Urban Site ◽  
Core Shell ◽  
Mixing State ◽  
Carbon Aerosols ◽  
Black Carbon Aerosols

Abstract. Black carbon aerosols play an important role in climate change by absorbing solar radiation and degrading visibility. In this study, the mixing state of refractory black carbon (rBC) at an urban site in Beijing was studied with a single particle soot photometer (SP2), as well as a tandem observation system with a centrifugal particle mass analyzer (CPMA) and a differential mobility analyzer (DMA), in early summer of 2018. The results demonstrated that the mass-equivalent size distribution of rBC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 171.2 nm. When the site experienced prevailing southerly winds, the MMD of rBC increased notably by 19 %. During the observational period, the ratio of the diameter of rBC-containing particles (Dp) to the rBC core (Dc) was 1.20 on average for Dc = 180 nm, indicating that the majority of rBC particles were thinly coated. The Dp / Dc value exhibited a clear diurnal pattern, with a maximum at 1400 LST and an enhancing rate of 0.013/h; higher Ox conditions increased the coating enhancing rate. Bare rBC particles were primarily in a fractal structure with a mass fractal dimension (Dfm) of 2.35, with limited variation during both clean and pollution periods, indicating significant impacts from on-road vehicle emissions. The morphology of rBC-containing particles vairied with aging processes. The mixing state of rBC particles could be indicated by the mass ratio of non-refractory matter to rBC (MR). In the present study, rBC-containing particles were primarily found in an external fractal structure when MR  6, at which the measured scattering cross section of rBC-containing particles was consistent with that based on the Mie-scattering simulation. We found only 9 % of the rBC-containing particles were in core-shell structures on clean days with a particle mass of 10 fg, and the number fraction of core-shell structures increased considerably to 32 % on pollution days. Considering the morphology change, the absorption enhancement (Eabs) was 11.7 % higher based on core-shell structures. This study highlights the combined effects of morphology and coating thickness on the Eabs of rBC-containing particles, which will be helpful for determining the climatic effects of BC.

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

2017 ◽  
Vol 17 (24) ◽  
pp. 14975-14985 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Xinhui Bi ◽  
Duohong Chen ◽  
...  
Keyword(s):  
Black Carbon ◽  
Single Particle ◽  
Southern China ◽  
Cloud Droplet ◽  
Mixing State ◽  
Cloud Droplets ◽  
Aerosol Mass ◽  
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 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 extensively internally mixed with sulfate and were scavenged into cloud droplets (with number fractions of 0.05–0.45) to a similar (or slightly lower) extent as all the measured particles (0.07–0.6) over the measured size range of 0.1–1.6 µm. 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 scavenged 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. Our results would improve the knowledge on the concentration, mixing state, and cloud scavenging of BC in the free troposphere.

scholarly journals Single particle diversity and mixing state measurements

2014 ◽  
Vol 14 (12) ◽  
pp. 6289-6299 ◽  
Author(s):  
R. M. Healy ◽  
N. Riemer ◽  
J. C. Wenger ◽  
M. Murphy ◽  
M. West ◽  
...  
Keyword(s):  
Species Diversity ◽  
Ammonium Nitrate ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Mass Fractions ◽  
State Index

Abstract. A newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulfate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0 and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France, 2010. Di values are low (~ 2) for fresh traffic and wood-burning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (~ 4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulfate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150–1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and wood-burning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulfate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.

scholarly journals Single particle diversity and mixing state measurements

2014 ◽  
Vol 14 (3) ◽  
pp. 3973-4005 ◽  
Author(s):  
R. M. Healy ◽  
N. Riemer ◽  
J. C. Wenger ◽  
M. Murphy ◽  
M. West ◽  
...  
Keyword(s):  
Species Diversity ◽  
Ammonium Nitrate ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Mass Fractions ◽  
State Index

Abstract. A newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulphate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0% and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France 2010. Di values are low (∼2) for fresh traffic and woodburning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (∼4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulphate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150–1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and woodburning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulphate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.

scholarly journals Morphology and mixing of black carbon particles collected in central California during the CARES field study

2016 ◽  
Vol 16 (22) ◽  
pp. 14515-14525 ◽  
Author(s):  
Ryan C. Moffet ◽  
Rachel E. O'Brien ◽  
Peter A. Alpert ◽  
Stephen T. Kelly ◽  
Don Q. Pham ◽  
...  
Keyword(s):  
Black Carbon ◽  
Central Valley ◽  
Photochemical Activity ◽  
Urban Site ◽  
Mixing State ◽  
Data Set ◽  
Carbon Particles ◽  
Aerosol Absorption ◽  
Scanning Transmission ◽  
Rural Sites

Abstract. Aerosol absorption is strongly dependent on the internal heterogeneity (mixing state) and morphology of individual particles containing black carbon (BC) and other non-absorbing species. Here, we examine an extensive microscopic data set collected in the California Central Valley during the CARES 2010 field campaign. During a period of high photochemical activity and pollution buildup, the particle mixing state and morphology were characterized using scanning transmission X-ray microscopy (STXM) at the carbon K-edge. Observations of compacted BC core morphologies and thick organic coatings at both urban and rural sites provide evidence of the aged nature of particles, highlighting the importance of highly aged particles at urban sites during periods of high photochemical activity. Based on the observation of thick coatings and more convex BC inclusion morphology, either the aging was rapid or the contribution of fresh BC emissions at the urban site was relatively small compared to background concentrations. Most particles were observed to have the BC inclusion close to the center of the host. However, host particles containing inorganic rich inclusions had the BC inclusion closer to the edge of the particle. These measurements of BC morphology and mixing state provide important constraints for the morphological effects on BC optical properties expected in aged urban plumes.

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