Investigating the chemical nature of humic-like substances (HULIS) in North American atmospheric aerosols by liquid chromatography tandem mass spectrometry |
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| Authors: | Elizabeth A Stone Curtis J Hedman Rebecca J Sheesley Martin M Shafer James J Schauer |
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| Institution: | 1. Environmental Chemistry and Technology Program, Civil and Environmental Engineering, University of Wisconsin-Madison, 660 N. Park St, Madison, WI 53706, USA;2. Wisconsin State Laboratory of Hygiene, University of Wisconsin-Madison, 2601 Agriculture Dr., Madison, WI 53718, USA;1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China;2. Department of Atmospheric Science, Colorado State University, Fort Collins, CO, 80523, USA;3. Department of Environmental Science and Analytical Chemistry (ACES) and the Bolin Centre for Climate Research, Stockholm University, 10691, Stockholm, Sweden;1. College of Resource and Environment, Anhui Science and Technology University, Fengyang, 233100, PR China;2. State Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, 510640, PR China;3. Anhui Province Key Laboratory of Biochar and Cropland Pollution Prevention, Bengbu, Anhui, 233400, PR China;4. University of Chinese Academy of Sciences, Beijing, 100049, PR China;5. State Environmental Protection Key Laboratory of Water Environment Simulation and Pollution Control, Key Laboratory of Water and Atmosphere of Guangdong Province, South China Institute of Environmental Sciences, Ministry of Environmental Protection Guangzhou, 510655, China |
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| Abstract: | The high-molecular weight water-soluble organic compounds present in atmospheric aerosols underwent functional-group characterization using liquid chromatography tandem mass spectrometry (LC-MS/MS), with a focus on understanding the chemical structure and origins of humic-like substances (HULIS) in the atmosphere. Aerosol samples were obtained from several locations in North America at times when primary sources contributing to organic aerosol were well-characterized: Riverside, CA, Fresno, CA, urban and peripheral Mexico City, Atlanta, GA, and Bondville, IL. Chemical analysis targeted identification and quantification of functional groups, such as aliphatic, aromatic, and bulk carboxylic acids, organosulfates, and carbohydrate-like substances that comprise species with molecular weights (MW) 200–600 amu. Measured high-MW functional groups were compared to modeled primary sources with the purpose of identifying associations between aerosol sources, high-MW aerosol species, and HULIS. Mobile source emissions were linked to high-molecular weight carboxylic acids, especially aromatic acids, biomass burning was associated with carboxylic acids and carbohydrate-like substances, and secondary organic aerosol (SOA) correlated well with the total amount of HULIS measured, whereas organosulfates showed no correlation with aerosol sources and exhibited unique spatial trends. These results suggested the importance of motor vehicles, biomass burning, and SOA as important sources of precursors to HULIS. Structural characteristics of atmospheric HULIS were compared to terrestrial humic and fulvic acids and revealed striking similarities in chemical structure, with the exception of organosulfates which were unique to atmospheric HULIS. |
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