Unexpected Oligomerization of Small ?-Dicarbonyls for Secondary Organic Aerosol and Brown Carbon Formation
نویسندگان
چکیده
Large amounts of small ?-dicarbonyls (glyoxal and methylglyoxal) are produced in the atmosphere from photochemical oxidation biogenic isoprene anthropogenic aromatics, but fundamental mechanisms leading to secondary organic aerosol (SOA) brown carbon (BrC) formation remain elusive. Methylglyoxal is commonly believed be less reactive than glyoxal because unreactive methyl substitution, available laboratory measurements showed negligible growth methylglyoxal. Herein, we present experimental results demonstrate striking oligomerization SOA BrC on sub-micrometer aerosols. Significantly more efficient browning aerosols occur upon exposure methylglyoxal under atmospherically relevant concentrations absence/presence gas-phase ammonia formaldehyde, nonvolatile oligomers light-absorbing nitrogen-heterocycles identified as dominant particle-phase products. The distinct light absorption attributed carbenium ion-mediated nucleophilic addition, interfacial electric field-induced attraction, synergetic involving organic/inorganic species, surface- or volume-limited reactions that dependent reactivity gaseous concentrations. Our findings resolve an outstanding discrepancy concerning multiphase chemistry unravel a new avenue for abundant, ubiquitous carbonyls ammonia/ammonium sulfate.
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ژورنال
عنوان ژورنال: Environmental Science & Technology
سال: 2021
ISSN: ['1520-5851', '0013-936X']
DOI: https://doi.org/10.1021/acs.est.0c08066