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

Sui, Xiao; Zhou, Yufan; Zhang, Fei; Chen, Jianmin; Zhu, Zihua; Yu, Xiao‐Ying

doi:10.1039/c7cp02071f

Cited by 33 publications

(40 citation statements)

References 48 publications

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“…For UV aging, the device was set 10 cm away from a light source. 30 As soon as the desired aging time was reached, the device was immediately put into ToF-SIMS for analysis. More detailed information is described in Supplementary Methods.…”

Section: Salvi Enabled Liquid Sims Characterizationmentioning

confidence: 99%

“…We recently demonstrated that in situ liquid SIMS can be used to study the a-l interface in photochemical ultraviolet (UV) aging conditions simulated by the vacuum-liquid interface. 30,31 Furthermore, weak interaction formation, such as ion pairs and ion solvation at the interface was monitored by in situ liquid SIMS. 32 We explore interfacial chemistry relevant to aqSOA formation in dark aging in this work ( Supplementary Fig.…”

Section: Introductionmentioning

confidence: 99%

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Dark air–liquid interfacial chemistry of glyoxal and hydrogen peroxide

Zhang

Chen

et al. 2019

npj Clim Atmos Sci

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The air-liquid (a-l) interfacial chemistry of glyoxal is of great interest in atmospheric chemistry. We present molecular imaging of glyoxal and hydrogen peroxide (H 2 O 2) dark aging using in situ time-of-flight secondary ion mass spectrometry (ToF-SIMS). More organic peroxides and cluster ions are observed at the a-l interface in dark aging compared to UV aging. Cluster ions formed with more water molecules in dark aging indicate that the aqueous secondary organic aerosol (aqSOA) could form hydrogen bond with water molecules, suggesting that aqSOAs at the aqueous phase are more hydrophilic. Thus the interfacial aqSOA in dark aging could increase hygroscopic growth. Strong contribution of cluster ions and large water clusters in dark aging indicates change of solvation shells at the a-l interface. The observation of organic peroxides and cluster ions indicates that the aqueous surface could be a reservoir of organic peroxides and odd hydrogen radicals at night. Our findings provide new understandings of glyoxal a-l interfacial chemistry and fill in the gap between field measurements and the climate model simulation of aqSOAs.

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Section: Salvi Enabled Liquid Sims Characterizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Dark air–liquid interfacial chemistry of glyoxal and hydrogen peroxide

Zhang

Chen

et al. 2019

npj Clim Atmos Sci

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“…Nevertheless, oxalic acid and tartaric acid were more likely to be observed in liquid samples. In addition, oligomers formed from hydration products, including C 6 H 9 O 7 + (m/z + 193), C 6 H 9 O 9 + (m/z + 225), C 8 H 15 O 13 + (m/z + 319), C 12 H 17 O 15 + (m/z + 401), and C 14 H 21 O 17 + (m/z + 461) in the positive mode and C 4 H 9 O 8 − (m/z − 185), C 6 H 7 O 9 − (m/z − 223), C 8 H 9 O 10 − (m/z − 265) in Figure , C 9 H 11 O 12 − (m/z − 311), and C 14 H 14 O 15 − (m/z − 422) in Figure in the negative mode, were observed in wet samples . In contrast, oligomers formed from dehydrated products were found in the dry surface analysis, such as C 8 H 9 O 12 + (m/z + 297), C 10 H 13 O 12 + (m/z + 325), and C 8 H 9 O 12 − (m/z − 297).…”

Section: Resultsmentioning

confidence: 99%

ToF‐SIMS characterization of glyoxal surface oxidation products by hydrogen peroxide: A comparison between dry and liquid samples

Sui

Zhou

Zhang

et al. 2017

Surface & Interface Analysis

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Funding information Pacific Northwest National LaboratoryAs one of the simplest volatile organic compounds, glyoxal and its oxidation products were considered to be important precursors to aqueous secondary organic aerosol formation. Herein, we analyzed products from glyoxal oxidation by hydrogen peroxide in dry and liquid samples using time-of-flight secondary ion mass spectrometry (ToF-SIMS). ToF-SIMS spectra and spectral principal component analysis (PCA) were used to investigate surface oxidation products. Dry samples were prepared on clean silicon wafers. Liquid samples consisting of glyoxal and hydrogen peroxide (H 2 O 2 ) were introduced to a vacuum compatible microfluidic reactor prior to UV illumination or dark aging followed by in situ liquid SIMS analysis. A number of reaction products were observed in both dry and liquid samples; different oligomers and carboxylic acids could be formed depending on reaction conditions. In addition, hydrolyzed products were observed in the liquid samples, but not in the dry samples. Although dry samples reveal some products of the aqueous process, they are not fully representative as results from those of the aqueous samples. Our findings suggest that the ability to characterize the liquid surface reaction products provides more realistic information of the reaction products associated with aqueous secondary organic aerosol formation in the atmosphere. Meanwhile, the high mass resolution spectra from the dry sample SIMS measurement are helpful to identify oxidation products in the liquid samples.the reaction of OH radicals with glyoxal leads to SOA formation. 3,5 In this study, H 2 O 2 was used as the oxidizing agent to study glyoxal oxidation in the aqueous phase. 3,5,6 Recent research efforts have focused on the pathways and complex chemical compounds formation in the aqueous aerosol using different detection techniques. Existing results suggested the observed products may be affected by sample preparation methods. Specifically, the type of reaction vessels or droplet formation may contribute to observational differences. 5,7 For example, open-chain glyoxal oligomers were observed in evaporating droplets by Fourier transform infrared spectroscopy. 7 Other studies used pretreated glyoxal solution injected into an electrospray ionization-mass spectrometer to investigate glyoxal oxidation pathways. 6,8-10 Their results indicated larger multifunctional products could contribute to the SOA formation, including carbonic acids, polymers, and high-mass oligomers. In addition, a box model 11 was used to simulate UV-visible absorption spectra of uptake by glyoxal. Although there was a general consensus in the pathways of glyoxal oxidation, the observed products were different among previous studies.As a powerful surface analysis tool, time-of-flight secondary ion mass spectrometry (ToF-SIMS) has been extensively used in surface characterization by taking advantage of its high mass resolution, sensitivity, and mass range. [12][13][14] Although one of ToF-SIMS unique capabilitie...

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“…PCA has been applied for processing the ToF-SIMS data in the research of many fields, such as materials, biology, and medicine. [26][27][28][29][30][31][32] In this study, we collected atmospheric aerosols on different air quality level days of each season in 2015 in an urban area of Beijing and analyzed these aerosols by ToF-SIMS. Since winter is the season with most frequent haze, we compared the mass spectral aerosol data acquired on various pollution level days in winter and analyzed by PCA.…”

Section: Funding Informationmentioning

confidence: 99%

“…Using PCA, the most useful and significant information can be effectively extracted. PCA has been applied for processing the ToF‐SIMS data in the research of many fields, such as materials, biology, and medicine …”

Section: Introductionmentioning

confidence: 99%

ToF‐SIMS analysis of chemical composition of atmospheric aerosols in Beijing

Jia

Che

et al. 2019

Surface & Interface Analysis

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Atmospheric aerosols collected from each season in urban Beijing have been studied using time‐of‐flight secondary ion mass spectrometry (ToF‐SIMS). The chemical composition of atmospheric aerosol particles during various atmospheric pollution levels was analyzed and distinguished by principal component analysis (PCA). The differences and sources of the components of the aerosol particles were explored. The results showed that the fine particulate matter from heavily polluted days mainly consists of inorganic salts and organic compounds, such as hydrocarbons, nitrogen‐ or sulfur‐containing hydrocarbons, and their oxides. Samples collected from clean days in the four seasons were also analyzed. Only the samples collected in spring showed a significant difference from the other three seasons. We concluded that the main source of pollution in the Beijing urban area was fossil fuel combustion from motor vehicles.

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

Cited by 33 publications

References 48 publications

Dark air–liquid interfacial chemistry of glyoxal and hydrogen peroxide

Dark air–liquid interfacial chemistry of glyoxal and hydrogen peroxide

ToF‐SIMS characterization of glyoxal surface oxidation products by hydrogen peroxide: A comparison between dry and liquid samples

ToF‐SIMS analysis of chemical composition of atmospheric aerosols in Beijing

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