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Chemical Analysis Methods for Particle-Phase Pollutants
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Chemical Analysis Methods for Particle-Phase Pollutants

A special issue of Atmosphere (ISSN 2073-4433). This special issue belongs to the section "Aerosols".

Deadline for manuscript submissions: closed (26 June 2020) | Viewed by 28885

Special Issue Editor

Dr. Guenter Engling

E-Mail Website
Guest Editor
California Air Resources Board, Riverside, CA, USA
Interests: atmospheric aerosol; environmental analytical chemistry; biomass burning; bioaerosol; vehicle emissions
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Atmospheric aerosol particles affect human and ecosystem health, geochemical cycles, and the Earth’s climate. The chemical composition of airborne particulate matter (PM) determines the type and severity of the environmental impact. The varied formation and transformation processes result in complex PM composition, rendering the characterization of ambient PM very challenging. Meanwhile, great advances have been made in terms of more detailed PM characterization at the molecular level.

This Special Issue of Atmosphere is focused on the state-of-the-art of chemical analysis methods for aerosol particles, including recently developed methods, especially advanced mass spectrometric (MS) methods, as well as applications of existing analytical methods. Authors are invited to submit manuscripts reporting measurement approaches for both ambient aerosol and source emissions, including those of biogenic and anthropogenic origin. Specifically, characterization of secondary organic aerosols (SOA) warrants more efforts, which are a particularly welcome contribution to this Special Issue. Methods applied for real-time in situ PM characterization, including utilization of low-cost sensors, as well as filter-based time-integrated laboratory analyses, can be presented here. Ultimately, this Special Issue wants to give an overview of the latest chemical characterization methods that provide a more comprehensive and accurate understanding of atmospheric aerosol properties, as well as their formation and transformation processes. Prospective authors are welcome to contact the guest editor with questions regarding their chosen topics for this Special Issue.

Dr. Guenter Engling
Guest Editor

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Keywords

  • Atmospheric aerosol
  • PM2.5
  • Chemical speciation
  • Mass spectrometry
  • Source emissions

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Published Papers (7 papers)

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Research

22 pages, 5535 KiB  
Article
Minimizing Contamination from Plastic Labware in the Quantification of C16 and C18 Fatty Acids in Filter Samples of Atmospheric Particulate Matter and Their Utility in Apportioning Cooking Source Contribution to Urban PM2.5
by Yuk Ying Cheng and Jian Zhen Yu
Atmosphere 2020, 11(10), 1120; https://doi.org/10.3390/atmos11101120 - 19 Oct 2020
Cited by 12 | Viewed by 4381
Abstract
Palmitic acid (C16:0) and stearic acid (C18:0) are among the most abundant products in cooking emission, and thus could serve as potential molecular tracers in estimating the contributions of cooking emission to particulate matter (PM2.5) pollution in the atmosphere. Organic tracer [...] Read more.
Palmitic acid (C16:0) and stearic acid (C18:0) are among the most abundant products in cooking emission, and thus could serve as potential molecular tracers in estimating the contributions of cooking emission to particulate matter (PM2.5) pollution in the atmosphere. Organic tracer analysis in filter-based samples generally involves extraction by organic solvents, followed by filtration. In these procedures, disposable plastic labware is commonly used due to convenience and as a precaution against sample-to-sample cross contamination. However, we observed contamination for both C16:0 and C18:0 fatty acids, their levels reaching 6–8 ppm in method blanks and leading to their detection in 9% and 42% of PM2.5 samples from Hong Kong, indistinguishable from the blank. We present in this work the identification of plastic syringe and plastic syringe filter disc as the contamination sources. We further demonstrated that a new method procedure using glass syringe and stainless-steel syringe filter holder offers a successful solution. The new method has reduced the contamination level from 6.6 ± 1.2 to 2.6 ± 0.9 ppm for C16:0 and from 8.9 ± 2.1 to 1.9 ± 0.8 ppm for C18:0 fatty acid. Consequently, the limit of detection (LOD) for C16:0 has decreased by 57% from 1.8 to 0.8 ppm and 56% for C18:0 fatty acid from 3.2 to 1.4 ppm. Reductions in both LOD and blank variability has allowed the increase in quantification rate of the two fatty acids in ambient samples and thereby retrieving more data for estimating the contribution of cooking emission to ambient PM2.5. With the assistance of three cooking related tracers, palmitic acid (C16:0), stearic acid (C18:0) and cholesterol, positive matrix factorization analysis of a dataset of PM2.5 samples collected from urban Hong Kong resolved a cooking emission source. The results indicate that cooking was a significant local PM2.5 source, contributing to an average of 2.2 µgC/m3 (19%) to organic carbon at a busy downtown roadside location and 1.8 µgC/m3 (15%) at a general urban site. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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18 pages, 5475 KiB  
Article
Characterization of Atmospheric PM2.5 Inorganic Aerosols Using the Semi-Continuous PPWD-PILS-IC System and the ISORROPIA-II
by Thi-Cuc Le, Yun-Chin Wang, David Y. H. Pui and Chuen-Jinn Tsai
Atmosphere 2020, 11(8), 820; https://doi.org/10.3390/atmos11080820 - 4 Aug 2020
Cited by 10 | Viewed by 3969
Abstract
A semi-continuous monitoring system, a parallel plate wet denuder and particle into liquid sampler coupled with ion chromatography (PPWD-PILS-IC), was used to measure the hourly precursor gases and water-soluble inorganic ions in ambient particles smaller than 2.5 µm in diameter (PM2.5) [...] Read more.
A semi-continuous monitoring system, a parallel plate wet denuder and particle into liquid sampler coupled with ion chromatography (PPWD-PILS-IC), was used to measure the hourly precursor gases and water-soluble inorganic ions in ambient particles smaller than 2.5 µm in diameter (PM2.5) for investigating the thermodynamic equilibrium of aerosols using the ISORROPIA-II thermodynamic equilibrium model. The 24-h average PPWD-PILS-IC data showed very good agreement with the daily data of the manual 5 L/min porous-metal denuder sampler with R2 ranging from 0.88 to 0.98 for inorganic ions (NH4+, Na+, K+, NO3−, SO42−, and Cl−) and 0.89 to 0.98 for precursor gases (NH3, HNO3, HONO, and SO2) and slopes ranging from 0.94 to 1.17 for ions and 0.87 to 0.95 for gases, respectively. In addition, the predicted ISORROPIA-II results were in good agreement with the hourly observed data of the PPWD-PILS-IC system for SO42− (R2 = 0.99 and slope = 1.0) and NH3 (R2 = 0.97 and slope = 1.02). The correlation of the predicted results and observed data was further improved for NH4+ and NO3− with the slope increasing from 0.90 to 0.96 and 0.95 to 1.09, respectively when the HNO2 and NO2− were included in the total nitrate concentration (TN = [NO3−] + [HNO3] + [HONO] + [NO2−]). The predicted HNO3 data were comparable to the sum of the observed [HNO3] and [HONO] indicating that HONO played an important role in the thermodynamic equilibrium of ambient PM2.5 aerosols but has not been considered in the ISORROPIA-II thermodynamic equilibrium model. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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14 pages, 1549 KiB  
Article
A Quantitative Method to Measure and Speciate Amines in Ambient Aerosol Samples
by Amy P. Sullivan, Katherine B. Benedict, Christian M. Carrico, Manvendra K. Dubey, Bret A. Schichtel and Jeffrey L. Collett
Atmosphere 2020, 11(8), 808; https://doi.org/10.3390/atmos11080808 - 30 Jul 2020
Cited by 8 | Viewed by 4171
Abstract
Ambient reactive nitrogen is a mix of nitrogen-containing organic and inorganic compounds. These various compounds are found in both aerosol- and gas-phases with oxidized and reduced forms of nitrogen. Aerosol-phase reduced nitrogen is predominately thought to include ammonium and amines. In ambient samples, [...] Read more.
Ambient reactive nitrogen is a mix of nitrogen-containing organic and inorganic compounds. These various compounds are found in both aerosol- and gas-phases with oxidized and reduced forms of nitrogen. Aerosol-phase reduced nitrogen is predominately thought to include ammonium and amines. In ambient samples, the ammonium concentration is routinely determined, but the contribution of amines is not. We developed a method to discretely measure amines from ambient aerosol samples. It employs ion chromatography using a Thermo Scientific IonPac Dionex CS-19 column with conductivity detection and a three-step separation using a methanesulfonic acid eluent. This method allows for the quantification of 18 different amines, including the series of methylamines and the different isomers of butylamine. Almost all amines quantifiable by this technique were measured regularly when applying this method to ambient filter samples collected in Rocky Mountain National Park (RMNP) and Greeley, CO. The sum of the amines was ~0.02 µg m−3 at both sites. This increased to 0.04 and 0.09 µg m−3 at RMNP and Greeley, respectively, at the same time they were impacted by smoke. Analysis of separate, fresh biomass burning source samples, however, suggests that smoke is likely a minor emission source of amines in most environments. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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11 pages, 1003 KiB  
Article
A Novel Method for Carbonate Quantification in Atmospheric Particulate Matter
by Denise C. Napolitano, Hilairy E. Hartnett and Pierre Herckes
Atmosphere 2020, 11(6), 661; https://doi.org/10.3390/atmos11060661 - 20 Jun 2020
Viewed by 3262
Abstract
Inorganic carbonate can be an important component of atmospheric particulate matter in arid environments where mineral dust components contribute significantly to air particulate matter. Carbonate carbon (CC) is only rarely quantified in atmospheric studies and methods to quantify carbonate in atmospheric samples are [...] Read more.
Inorganic carbonate can be an important component of atmospheric particulate matter in arid environments where mineral dust components contribute significantly to air particulate matter. Carbonate carbon (CC) is only rarely quantified in atmospheric studies and methods to quantify carbonate in atmospheric samples are rare. In this manuscript, we present a novel protocol for quantifying carbonate carbon in atmospheric particulate matter samples, through the acidification of aerosol filters at ambient pressure and temperature and subsequent measurement of carbon dioxide (CO2) released upon acidification. This method is applicable to a variety of filter media used in air pollution studies, such as Teflon, cellulose, or glass fiber filters. The method allows the customization of the filter area used for analysis (up to 24 cm2) so that sufficient CO2 can be detected when released and to assure that the sample aliquot is representative of the whole filter. The resulting detection limits can be as low as 0.12 µg/cm2. The analysis of a known amount of sodium bicarbonate applied to a filter resulted in a relative error within 15% of the known mass of bicarbonate when measured 20 min after acidification. A particulate matter sample with aerodynamic diameter larger than 2.5 µm (PM>2.5) collected via cascade impaction on a high-volume aerosol sampler yielded good precision, with a CC concentration of 4.4 ± 0.3 µgC/cm2 for six replicates. The precision, accuracy, and reproducibility of this method of CC measurement make it a good alternative to existing quantification methods. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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17 pages, 3715 KiB  
Article
Significant Contribution of Primary Sources to Water-Soluble Organic Carbon During Spring in Beijing, China
by Yali Jin, Caiqing Yan, Amy P. Sullivan, Yue Liu, Xinming Wang, Huabin Dong, Shiyi Chen, Limin Zeng, Jeffrey L. Collett, Jr. and Mei Zheng
Atmosphere 2020, 11(4), 395; https://doi.org/10.3390/atmos11040395 - 16 Apr 2020
Cited by 17 | Viewed by 3889
Abstract
Despite the significant role water-soluble organic carbon (WSOC) plays in climate and human health, sources and formation mechanisms of atmospheric WSOC are still unclear; especially in some heavily polluted areas. In this study, near real-time WSOC measurement was conducted in Beijing for the [...] Read more.
Despite the significant role water-soluble organic carbon (WSOC) plays in climate and human health, sources and formation mechanisms of atmospheric WSOC are still unclear; especially in some heavily polluted areas. In this study, near real-time WSOC measurement was conducted in Beijing for the first time with a particle-into-liquid-sampler coupled to a total organic carbon analyzer during the springtime, together with collocated online measurements of other chemical components in fine particulate matter with a 1 h time resolution, including elemental carbon (EC), organic carbon (OC), multiple metals, and water-soluble ions. Good correlations of WSOC with primary OC, as well as carbon monoxide, indicated that major sources of WSOC were primary instead of secondary during the study period. The positive matrix factorization model-based source apportionment results quantified that 68 ± 19% of WSOC could be attributed to primary sources, with predominant contributions by biomass burning during the study period. This finding was further confirmed by the estimate with the modified EC-tracer method, suggesting significant contribution of primary sources to WSOC. However, the relative contribution of secondary source to WSOC increased during haze episodes. The WSOC/OC ratio exhibited similar diurnal distributions with O3 and correlated well with secondary WSOC, suggesting that the WSOC/OC ratio might act as an indicator of secondary formation when WSOC was dominated by primary sources. This study provided evidence that primary sources could be major sources of WSOC in some polluted megacities, such as Beijing. From this study, it can be seen that WSOC cannot be simply used as a surrogate of secondary organic aerosol, and its major sources could vary by season and location. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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16 pages, 3455 KiB  
Article
Simultaneous Measurements of Chemical Compositions of Fine Particles during Winter Haze Period in Urban Sites in China and Korea
by Minhan Park, Yujue Wang, Jihyo Chong, Haebum Lee, Jiho Jang, Hangyul Song, Nohhyeon Kwak, Lucille Joanna S. Borlaza, Hyunok Maeng, Enrique Mikhael R. Cosep, Ma. Cristine Faye J. Denna, Shiyi Chen, Ilhwa Seo, Min-Suk Bae, Kyoung-Soon Jang, Mira Choi, Young Hwan Kim, Moonhee Park, Jong-Sik Ryu, Sanghee Park, Min Hu and Kihong Parkadd Show full author list remove Hide full author list
Atmosphere 2020, 11(3), 292; https://doi.org/10.3390/atmos11030292 - 16 Mar 2020
Cited by 9 | Viewed by 4503
Abstract
We performed simultaneous measurements of chemical compositions of fine particles in Beijing, China and Gwangju, Korea to better understand their sources during winter haze period. We identified PM2.5 events in Beijing, possibly caused by a combination of multiple primary combustion sources (biomass [...] Read more.
We performed simultaneous measurements of chemical compositions of fine particles in Beijing, China and Gwangju, Korea to better understand their sources during winter haze period. We identified PM2.5 events in Beijing, possibly caused by a combination of multiple primary combustion sources (biomass burning, coal burning, and vehicle emissions) and secondary aerosol formation under stagnant conditions and/or dust sources under high wind speeds. During the PM2.5 events in Gwangju, the contribution of biomass burning and secondary formation of nitrate and organics to the fine particles content significantly increased under stagnant conditions. We commonly observed the increases of nitrogen-containing organic compounds and biomass burning inorganic (K+) and organic (levoglucosan) markers, suggesting the importance of biomass burning sources during the winter haze events (except dust event cases) at both sites. Pb isotope ratios indicated that the fraction of Pb originated from possibly industry and coal combustion sources increased during the PM2.5 events in Gwangju, relative to nonevent days. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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15 pages, 3662 KiB  
Article
Source Identification of Trace Elements in PM2.5 at a Rural Site in the North China Plain
by Lei Liu, Yusi Liu, Wei Wen, Linlin Liang, Xin Ma, Jiao Jiao and Kun Guo
Atmosphere 2020, 11(2), 179; https://doi.org/10.3390/atmos11020179 - 9 Feb 2020
Cited by 29 | Viewed by 3925
Abstract
An intensive sampling of PM2.5 was conducted at a rural site (Gucheng) in the North China Plain from 22 October to 23 November 2016. A total of 25 elements (Al, Na, Cl, Mg, P, S, K, Ca, Ti, V, Cr, Mn, Fe, [...] Read more.
An intensive sampling of PM2.5 was conducted at a rural site (Gucheng) in the North China Plain from 22 October to 23 November 2016. A total of 25 elements (Al, Na, Cl, Mg, P, S, K, Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Br, Sr, Cd, Ba, Pb, and Sb) from PM2.5 filter samples collected daily were measured using a wavelength dispersive X-ray fluorescence spectrometer. Cl, S, and K were the most abundant elements, with average concentrations of 2077.66 ng m−3 (range 118.88–4638.96 ng m−3), 1748.78 ng m−3 (range 276.67–4335.59 ng m−3), and 1287.07 ng m−3 (range 254.90–2748.63 ng m−3), respectively. Among noncrustal trace metal elements, the concentration of Zn was the highest, with an average of 397.74 ng m−3 (range 36.45–1602.96 ng m−3), followed by Sb and Pb, on average, of 299.20 ng m−3 and 184.52 ng m−3, respectively. The morphologies of PM2.5 samples were observed using scanning electron microscopy. The shape of the particles was predominantly spherical, chain-like, and irregular. Positive matrix factorization analysis revealed that soil dust, following by industry, secondary formation, vehicle emissions, biomass and waste burning, and coal combustion, were the main sources of PM2.5. The results of cluster, potential source contribution function, and concentration weighted trajectory analyses suggested that local emissions from Hebei Province, as well as regional transport from Beijing, Tianjin, Shandong, and Shanxi Province, and long-range transport from Inner Mongolia, were the main contributors to PM2.5 pollution. Full article
(This article belongs to the Special Issue Chemical Analysis Methods for Particle-Phase Pollutants)
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