Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties.

Autor: Riva M; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States.; Department of Mechanical Engineering , University of Minnesota-Twin Cities , Minneapolis , Minnesota 55455 , United States., Chen Y; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Zhang Y; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States.; Aerodyne Research Inc. , Billerica , Massachusetts 01821 , United States., Lei Z; Department of Environmental Health Sciences , University of Michigan , Ann Arbor , Michigan 48109 , United States., Olson NE; Department of Chemistry , University of Michigan , Ann Arbor , Michigan 48109 , United States., Boyer HC; Department of Mechanical Engineering , University of Minnesota-Twin Cities , Minneapolis , Minnesota 55455 , United States., Narayan S; Department of Mechanical Engineering , University of Minnesota-Twin Cities , Minneapolis , Minnesota 55455 , United States., Yee LD; Department of Environmental Science, Policy, and Management , University of California , Berkeley , California 94720 , United States., Green HS; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Cui T; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Zhang Z; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Baumann K; Atmospheric Research & Analysis, Inc. , Cary , North Carolina 27513 , United States., Fort M; Atmospheric Research & Analysis, Inc. , Cary , North Carolina 27513 , United States., Edgerton E; Atmospheric Research & Analysis, Inc. , Cary , North Carolina 27513 , United States., Budisulistiorini SH; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Rose CA; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Ribeiro IO; Escola Superior de Tecnologia , Universidade do Estado do Amazonas , Manaus , Amazonas 69050 , Brazil., E Oliveira RL; Escola Superior de Tecnologia , Universidade do Estado do Amazonas , Manaus , Amazonas 69050 , Brazil., Dos Santos EO; Department of Chemistry , Federal University of Amazonas , Manaus , Amazonas 69067 , Brazil., Machado CMD; Department of Chemistry , Federal University of Amazonas , Manaus , Amazonas 69067 , Brazil., Szopa S; Laboratoire des Sciences du Climat et de l'Environnement , CEA-CNRS-UVSQ-IPSL , 91190 Gif-sur-Yvette , France., Zhao Y; Department of Atmospheric Sciences , University of Washington , Seattle , Washington 98195 , United States., Alves EG; Environment Dynamics Department , National Institute of Amazonian Research (INPA) , Manaus 69067 , Brazil., de Sá SS; John A. Paulson School of Engineering and Applied Sciences , Harvard University , Cambridge , Massachusetts 02138 , United States., Hu W; Department of Chemistry and Cooperative Institute for Research in Environmental Sciences , University of Colorado , Boulder , Colorado 80309 , United States., Knipping EM; Electric Power Research Institute , Washington , District of Columbia 20005 , United States., Shaw SL; Electric Power Research Institute , Palo Alto , California 94304 , United States., Duvoisin Junior S; Escola Superior de Tecnologia , Universidade do Estado do Amazonas , Manaus , Amazonas 69050 , Brazil., de Souza RAF; Escola Superior de Tecnologia , Universidade do Estado do Amazonas , Manaus , Amazonas 69050 , Brazil., Palm BB; Department of Chemistry and Cooperative Institute for Research in Environmental Sciences , University of Colorado , Boulder , Colorado 80309 , United States., Jimenez JL; Department of Chemistry and Cooperative Institute for Research in Environmental Sciences , University of Colorado , Boulder , Colorado 80309 , United States., Glasius M; Aarhus University , Department of Chemistry , 8000 Aarhus C , Denmark., Goldstein AH; Department of Environmental Science, Policy, and Management , University of California , Berkeley , California 94720 , United States., Pye HOT; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States.; National Exposure Research Laboratory , U.S. Environmental Protection Agency , Research Triangle Park , North Carolina 27711 , United States., Gold A; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Turpin BJ; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Vizuete W; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States., Martin ST; John A. Paulson School of Engineering and Applied Sciences , Harvard University , Cambridge , Massachusetts 02138 , United States.; Department of Earth and Planetary Sciences , Harvard University , Cambridge , Massachusetts 02138 , United States., Thornton JA; Department of Atmospheric Sciences , University of Washington , Seattle , Washington 98195 , United States., Dutcher CS; Department of Mechanical Engineering , University of Minnesota-Twin Cities , Minneapolis , Minnesota 55455 , United States., Ault AP; Department of Environmental Health Sciences , University of Michigan , Ann Arbor , Michigan 48109 , United States.; Department of Chemistry , University of Michigan , Ann Arbor , Michigan 48109 , United States., Surratt JD; Department of Environmental Sciences and Engineering, Gillings School of Global Public Health , The University of North Carolina at Chapel Hill , Chapel Hill , North Carolina 27599 , United States.
Jazyk: angličtina
Zdroj: Environmental science & technology [Environ Sci Technol] 2019 Aug 06; Vol. 53 (15), pp. 8682-8694. Date of Electronic Publication: 2019 Jul 23.
DOI: 10.1021/acs.est.9b01019
Abstrakt: Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), key isoprene oxidation products, with inorganic sulfate aerosol yields substantial amounts of secondary organic aerosol (SOA) through the formation of organosulfur compounds. The extent and implications of inorganic-to-organic sulfate conversion, however, are unknown. In this article, we demonstrate that extensive consumption of inorganic sulfate occurs, which increases with the IEPOX-to-inorganic sulfate concentration ratio (IEPOX/Sulf inorg ), as determined by laboratory measurements. Characterization of the total sulfur aerosol observed at Look Rock, Tennessee, from 2007 to 2016 shows that organosulfur mass fractions will likely continue to increase with ongoing declines in anthropogenic Sulf inorg , consistent with our laboratory findings. We further demonstrate that organosulfur compounds greatly modify critical aerosol properties, such as acidity, morphology, viscosity, and phase state. These new mechanistic insights demonstrate that changes in SO 2 emissions, especially in isoprene-dominated environments, will significantly alter biogenic SOA physicochemical properties. Consequently, IEPOX/Sulf inorg will play an important role in understanding the historical climate and determining future impacts of biogenic SOA on the global climate and air quality.
Databáze: MEDLINE