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Anthropogenic enhancements to production of highly oxygenated molecules from autoxidation.

Abstract：

:Atmospheric oxidation of natural and anthropogenic volatile organic compounds (VOCs) leads to secondary organic aerosol (SOA), which constitutes a major and often dominant component of atmospheric fine particulate matter (PM2.5). Recent work demonstrates that rapid autoxidation of organic peroxy radicals (RO2) formed during VOC oxidation results in highly oxygenated organic molecules (HOM) that efficiently form SOA. As NOx emissions decrease, the chemical regime of the atmosphere changes to one in which RO2 autoxidation becomes increasingly important, potentially increasing PM2.5, while oxidant availability driving RO2 formation rates simultaneously declines, possibly slowing regional PM2.5 formation. Using a suite of in situ aircraft observations and laboratory studies of HOM, together with a detailed molecular mechanism, we show that although autoxidation in an archetypal biogenic VOC system becomes more competitive as NOx decreases, absolute HOM production rates decrease due to oxidant reductions, leading to an overall positive coupling between anthropogenic NOx and localized biogenic SOA from autoxidation. This effect is observed in the Atlanta, Georgia, urban plume where HOM is enhanced in the presence of elevated NO, and predictions for Guangzhou, China, where increasing HOM-RO2 production coincides with increases in NO from 1990 to 2010. These results suggest added benefits to PM2.5 abatement strategies come with NOx emission reductions and have implications for aerosol-climate interactions due to changes in global SOA resulting from NOx interactions since the preindustrial era.

journal_name

Proc Natl Acad Sci U S A

journal_title

Proceedings of the National Academy of Sciences of the United States of America

authors

Pye HOT,D'Ambro EL,Lee BH,Schobesberger S,Takeuchi M,Zhao Y,Lopez-Hilfiker F,Liu J,Shilling JE,Xing J,Mathur R,Middlebrook AM,Liao J,Welti A,Graus M,Warneke C,de Gouw JA,Holloway JS,Ryerson TB,Pollack IB,Thornton

doi

10.1073/pnas.1810774116

subject

Has Abstract

pub_date

2019-04-02 00:00:00

pages

6641-6646

issue

eissn

0027-8424

issn

1091-6490

pii

1810774116

journal_volume

116

pub_type

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Anthropogenic enhancements to production of highly oxygenated molecules from autoxidation.