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Issue 31, 2017
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Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging

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Abstract

Aqueous surfaces after photochemical and dark reactions of glyoxal and hydrogen peroxide (H2O2) have been studied using a microfluidic reactor coupled with an in situ liquid time-of-flight secondary ion mass spectrometry (ToF-SIMS) for the first time. Spectral principal component analysis was used to determine similarities and differences among various photochemical aging and dark reaction samples and controls. Compared with previous results using bulk solutions, our unique liquid surface molecular imaging approach provided observations of glyoxal hydration (i.e., first and secondary products), oxidation products (i.e., glyoxylic acid, oxalic acid, formic acid, tartaric acid), oligomers, cluster ions, and water clusters with sub-micrometer spatial resolution. Observations of oxidation products give the physical foundation to deduce new reaction pathways at the aqueous surface. The first chemical mapping of water cluster changes between dark and photochemical aging suggests that glyoxal oxidation affects the hydrophobicity and water microenvironment at the surface, influencing the particle's ability of reactive uptake and subsequent cloud condensation nucleation and/or ice nucleation activation. Moreover, SIMS three-dimensional chemical mapping has made it possible to visualize the surface mixing state for the first time. We potentially provide a new method to investigate complex surface chemistry as an important source of aqueous secondary organic aerosol (aqSOA) formation in atmospheric chemistry.

Graphical abstract: Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging

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Publication details

The article was received on 31 Mar 2017, accepted on 23 May 2017 and first published on 23 May 2017


Article type: Paper
DOI: 10.1039/C7CP02071F
Citation: Phys. Chem. Chem. Phys., 2017,19, 20357-20366
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    Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging

    X. Sui, Y. Zhou, F. Zhang, J. Chen, Z. Zhu and X. Yu, Phys. Chem. Chem. Phys., 2017, 19, 20357
    DOI: 10.1039/C7CP02071F

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