High levels of ammonia do not raise fine particle pH sufficiently to yield nitrogen oxide-dominated sulfate production

被引:168
作者
Guo, Hongyu [1 ]
Weber, Rodney J. [1 ]
Nenes, Athanasios [1 ,2 ,3 ,4 ]
机构
[1] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[2] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[3] Fdn Res & Technol Hellas, Inst Chem Engn Sci, GR-26504 Patras, Greece
[4] Natl Observ Athens, Inst Environm Res & Sustainable Dev, GR-15236 Palea Penteli, Greece
基金
美国国家科学基金会;
关键词
THERMODYNAMIC-EQUILIBRIUM MODEL; MINERAL DUST; AEROSOL; ACID; ISORROPIA; EMISSIONS; POLLUTION; WATER; IRON;
D O I
10.1038/s41598-017-11704-0
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
High levels of ammonia (NH3) have been suggested to elevate ambient particle pH levels to near neutral acidity (pH = 7), a condition that promotes rapid SO2 oxidation by NO2 to form aerosol sulfate concentration consistent with "London fog" levels. This postulation is tested using aerosol data from representative sites around the world to conduct a thorough thermodynamic analysis of aerosol pH and its sensitivity to NH3 levels. We find that particle pH, regardless of ammonia levels, is always acidic even for the unusually high NH3 levels found in Beijing (pH = 4.5) and Xi'an (pH = 5), locations where sulfate production from NOx is proposed. Therefore, major sulfate oxidation through a NO2-mediated pathway is not likely in China, or any other region of the world (e.g., US, Mediterranean) where the aerosol is consistently more acidic. The limited alkalinity from the carbonate buffer in dust and seasalt can provide the only likely set of conditions where NO2-mediated oxidation of SO2 outcompetes with other well-established pathways. The mildly acidic levels associated with excessive amounts of ammonia can promote high rates of SO2 oxidation through transition metal chemistry, this may be an alternative important aerosol chemical contributor to the extreme pollution events.
引用
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页数:7
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