【摘 要】
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Mineral particles are ubiquitous in the atmosphere and exhibit an important effect on the photooxidation of volatile organic compounds(VOCs).However,the role of
【机 构】
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Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control
【基金项目】
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supported by National Natu-ral Science Foundation of China(Nos.41675122,42077189 and 41907184),Natural Science Foundation of Guangdong Province,China(No.2019B151502064),Local Innovative and Research T
论文部分内容阅读
Mineral particles are ubiquitous in the atmosphere and exhibit an important effect on the photooxidation of volatile organic compounds(VOCs).However,the role of mineral particles in the photochemical oxidation mechanism of VOCs remains unclear.Hence,the photooxi-dation reactions of acrolein(ARL)with OH radical(OH)in the presence and absence of SiO2 were investigated by theoretical approach.The gas-phase reaction without SiO2 has two distinct pathways(H-abstraction and OH-addition pathways),and carbonyl-H-abstraction is the dominant pathway.In the presence of SiO2,the reaction mechanism is changed,i.e.,the dominant pathway from carbonyl-H-abstraction to OH-addition to carbonyl C-atom.The en-ergy barrier of OH-addition to carbonyl C-atom deceases 21.33 kcal/mol when SiO2 is added.Carbonyl H-atom of ARL is occupied by SiO2 via hydrogen bond,and carbonyl C-atom is ac-tivated by SiO2.Hence,the main product changes from H-abstraction product to OH-adduct in the presence of SiO2.The OH-adduct exhibits a thermodynamic feasibility to yield HO2 radical and carboxylic acid via the subsequent reactions with O2,with implications for O3 formation and surface acidity of mineral particles.
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