title: Uptake of methacrolein into aqueous solutions of sulfuric acid and hydrogen peroxide.
abstract: Multiphase acid-catalyzed oxidation by hydrogen peroxide has been suggested to be a potential route to secondary organic aerosol (SOA) formation from isoprene and its gas-phase oxidation products, but the kinetics and chemical mechanism remain largely uncertain. Here we report the first measurement of uptake of methacrolein into aqueous solutions of sulfuric acid and hydrogen peroxide in the temperature range of 253-293 K. The steady-state uptake coefficients were acquired and increased quickly with increasing sulfuric acid concentration and decreasing temperature. Propyne, acetone, and 2,3-dihydroxymethacrylic acid were suggested as the products. The chemical mechanism is proposed to be the oxidation of carbonyl group and C═C double bonds by peroxide hydrogen in acidic environment, which could explain the large content of polyhydroxyl compounds in atmospheric fine particles. These results indicate that multiphase acid-catalyzed oxidation of methacrolein by hydrogen peroxide can contribute to SOA mass in the atmosphere, especially in the upper troposphere.
authors.affiliation: Beijing National Laboratory for Molecular Science (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China.
authors.forename: Ze
authors.initials: Z
authors.lastname: Liu
authors.forename: Ling-Yan
authors.initials: LY
authors.lastname: Wu
authors.forename: Tian-He
authors.initials: TH
authors.lastname: Wang
authors.forename: Mao-Fa
authors.initials: MF
authors.lastname: Ge
authors.forename: Wei-Gang
authors.initials: WG
authors.lastname: Wang
mesh_terms: D000171:Acrolein / Q000031:analogs & derivatives* / Q000737:chemistry; D000336:Aerosols; D000393:Air Pollutants / Q000737:chemistry*; D002070:Butadienes / Q000737:chemistry; D002384:Catalysis; D005740:Gases; D045782:Hemiterpenes / Q000737:chemistry; D006861:Hydrogen Peroxide / Q000737:chemistry*; D007700:Kinetics; D010084:Oxidation-Reduction; D010420:Pentanes / Q000737:chemistry; D012996:Solutions; D013055:Spectrophotometry, Infrared; D013464:Sulfuric Acids / Q000737:chemistry*; D013696:Temperature; D014867:Water / Q000737:chemistry*
chemical_list: D000336:Aerosols; D000393:Air Pollutants; D002070:Butadienes; D005740:Gases; D045782:Hemiterpenes; D010420:Pentanes; D012996:Solutions; D013464:Sulfuric Acids; D014867:Water; C005059:isoprene; D000171:Acrolein; C039175:methacrylaldehyde; D006861:Hydrogen Peroxide; C033158:sulfuric acid