Glyoxal and methylglyoxal in Atlantic seawater and marine aerosol particles: method development and first application during the Polarstern cruise ANT XXVII/4

Pinxteren, Manuela van; Herrmann, Hartmut

doi:10.5194/acpd-13-15301-2013

Cited by 6 publications

(16 citation statements)

References 45 publications

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“…Thus, based on the data presented herein, it is likely that an additional source of glyoxal is still necessary to explain the MBL background mixing ratios, even if they are lower than previously reported [Sinreich et al, 2010]. There is growing evidence for a seawater source of glyoxal [Pinxteren and Herrmann, 2013], although there is still no clear picture on the exact nature of the source or its strength.…”

Section: 1002/2013jd021388mentioning

confidence: 68%

Glyoxal observations in the global marine boundary layer

et al. 2014

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Glyoxal is an important intermediate species formed by the oxidation of common biogenic and anthropogenic volatile organic compounds such as isoprene, toluene, and acetylene. Although glyoxal has been shown to play an important role in urban and forested environments, its role in the open ocean environment is still not well understood, with only a few observations showing evidence for its presence in the open ocean marine boundary layer (MBL). In this study, we report observations of glyoxal from 10 field campaigns in different parts of the world's oceans. These observations together represent the largest database of glyoxal in the MBL. The measurements are made with similar instruments that have been used in the past, although the open ocean values reported here, average of about 25 parts per trillion by volume (pptv) with an upper limit of 40 pptv, are much lower than previously reported observations that were consistently higher than 40 pptv and had an upper limit of 140 pptv, highlighting the uncertainties in the differential optical absorption spectroscopy method for the retrieval of glyoxal. Despite retrieval uncertainties, the results reported in this work support previous suggestions that the currently known sources of glyoxal are insufficient to explain the average MBL concentrations. This suggests that there is an additional missing source, more than a magnitude larger than currently known sources, which is necessary to account for the observed atmospheric levels of glyoxal. Therefore, it could play a more important role in the MBL than previously considered.

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Section: 1002/2013jd021388mentioning

confidence: 68%

Glyoxal observations in the global marine boundary layer

et al. 2014

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“…Proposed oceanic sources of glyoxal include reactions in the sea‐surface microlayer and the gas‐phase oxidation of marine‐derived volatile organic carbon in the atmosphere (Chiu et al, 2017; Zhou et al, 2014). Due to the high solubility of dicarbonyl compounds in seawater (Zhou & Mopper, 1990), the sea‐to‐air flux through gas exchange at the sea surface is highly unlikely, since measured surface dicarbonyl concentrations are quite low (0.3–5.6 and 0.1–3.4 nM, respectively) and highly undersaturated in the surface oceans (Takeda et al, 2014; van Pinxteren & Herrmann, 2013; Zhou & Mopper, 1990, 1997; Zhu & Kieber, 2019). As an added uncertainty, dicarbonyl compound cycling is poorly described in the surface ocean, with no documented marine source except for their photochemical production (Kieber et al, 1990; Zhou & Mopper, 1997; Zhu & Kieber, 2018).…”

Section: Introductionmentioning

confidence: 99%

Global Model for Depth‐Dependent Carbonyl Photochemical Production Rates in Seawater

Zhu

Kieber

2020

Global Biogeochemical Cycles

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A photochemical model was used to quantify the global contribution of carbonyl photoproduction in the photodegradation of marine dissolved organic carbon (DOC). As model input, wavelength-and temperature-dependent apparent quantum yields (AQYs) for the photochemical production of carbonyl compounds were determined in seawater collected from the Northwest Atlantic Ocean. These AQY data and published AQY data from the North Pacific were used with remotely sensed seawater optical properties and solar irradiance data in a global model to calculate depth-resolved, mixed-layer photochemical fluxes of acetaldehyde and glyoxal in seawater. Based on this model, the annual global surface mixed-layer photochemical production is 89.7 ± 36 Tg year −1 for acetaldehyde and 20.0 ± 8.0 Tg year −1 for glyoxal. This work significantly improves our understanding of the impact of photochemistry on the cycling of DOC in the surface oceans. Low-molecular-weight carbonyl compounds represent the second largest carbon flux among all known carbon products that are produced during the photolysis of DOC. The annual photoproduction of carbonyl-compound carbon is~110 ± 23 Tg C year −1 , comprising approximately 9.6% of the total carbon and 22% of the biologically labile carbon that are produced globally from the photolysis of marine DOC.Plain Language Summary Ultraviolet and visible solar irradiation absorbed by dissolved organic matter in seawater causes a myriad of chemical transformations including the photochemical production of atmospherically important and biologically labile organic compounds. In the current study, we determined the photochemical production of acetaldehyde, glyoxal, and methylglyoxal, in the surface oceans. A global-scale seasonal model of surface and depth-dependent photochemical production rates was developed for acetaldehyde and glyoxal using wavelength-and temperature-dependent photoproduction data determined in open ocean, oligotrophic seawater from the North Pacific and Northwest Atlantic Oceans, along with modeled solar irradiance and satellite-retrieved optical properties of seawater. Methylglyoxal was not modeled because its wavelength-dependent photochemical production could not be determined in open ocean waters. Results of this study were used to show that the photochemical production of carbonyl compounds represents an important fraction of marine organic matter that is photochemically degraded on an annual basis. Key Points:• Wavelength and temperature dependence for carbonyl photoproduction was determined in seawater from four stations in the NW Atlantic Ocean • Depth-integrated, surface mixed-layer rates of acetaldehyde and glyoxal photochemical production were calculated globally • Carbonyl compounds represent 9.6% and 22% of the total and biologically labile carbon produced from the photolysis of marine organic carbon Supporting Information:• Supporting Information S1

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“…Because SBSE is an equilibrium technique based on the partitioning of the analyte between the aqueous phase and the PDMS phase, the stirring times to reach equilibrium during extraction and liquid desorption were determined. Different extraction times (1,2,5,10, and 22 h) were tested for both G-and MG-bis-oximes. A stirring speed of 1,000 rpm was used and liquid desorption parameters were set as follows: stirring time 3 h, stripping solvent 1.5 mL ACN, stirring speed 500 rpm.…”

Section: Time Course Of Extraction and Liquid Desorptionmentioning

confidence: 99%

“…Besides secondary formation, G and MG can also be emitted directly into the atmosphere by biomass burning [1]. The lifetime of the alphadicarbonyls in the gas phase is rather short (about 2 h) [5]. However, due to their high Henry's law coefficients, G and MG efficiently partition into the (aqueous) particle phase.…”

Section: Introductionmentioning

confidence: 99%

“…A commonly used derivatization approach is pentafluorobenzyl hydroxylamine (PFBHA) derivatization with GC-ECD detection [20]. A study using PFBHA derivatization in combination with GC-MS was recently presented for the analysis of G and MG in seawater and marine aerosol [5]. Derivatization with BF 3 /n-butanol, which yields the corresponding dibutyl acetals, was applied for the measurement of G and MG in rain and snow, also using GC and GC-MS ( [21]).…”

Section: Introductionmentioning

confidence: 99%

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A new sensitive method for the quantification of glyoxal and methylglyoxal in snow and ice by stir bar sorptive extraction and liquid desorption-HPLC-ESI-MS

et al. 2014

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In this study, the development of a new sensitive method for the analysis of alpha-dicarbonyls glyoxal (G) and methylglyoxal (MG) in environmental ice and snow is presented. Stir bar sorptive extraction with in situ derivatization and liquid desorption (SBSE-LD) was used for sample extraction, enrichment, and derivatization. Measurements were carried out using high-performance liquid chromatography coupled to electrospray ionization tandem mass spectrometry (HPLC-ESI-MS/MS). As part of the method development, SBSE-LD parameters such as extraction time, derivatization reagent, desorption time and solvent, and the effect of NaCl addition on the SBSE efficiency as well as measurement parameters of HPLC-ESI-MS/MS were evaluated. Calibration was performed in the range of 1-60 ng/mL using spiked ultrapure water samples, thus incorporating the complete SBSE and derivatization process. 4-Fluorobenzaldehyde was applied as internal standard. Inter-batch precision was <12 % RSD. Recoveries were determined by means of spiked snow samples and were 78.9 ± 5.6 % for G and 82.7 ± 7.5 % for MG, respectively. Instrumental detection limits of 0.242 and 0.213 ng/mL for G and MG were achieved using the multiple reaction monitoring mode. Relative detection limits referred to a sample volume of 15 mL were 0.016 ng/mL for G and 0.014 ng/mL for MG. The optimized method was applied for the analysis of snow samples from Mount Hohenpeissenberg (close to the Meteorological Observatory Hohenpeissenberg, Germany) and samples from an ice core from Upper Grenzgletscher (Monte Rosa massif, Switzerland). Resulting concentrations were 0.085-16.3 ng/mL for G and 0.126-3.6 ng/mL for MG. Concentrations of G and MG in snow were 1-2 orders of magnitude higher than in ice core samples. The described method represents a simple, green, and sensitive analytical approach to measure G and MG in aqueous environmental samples.

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Glyoxal and methylglyoxal in Atlantic seawater and marine aerosol particles: method development and first application during the Polarstern cruise ANT XXVII/4

Cited by 6 publications

References 45 publications

Glyoxal observations in the global marine boundary layer

Glyoxal observations in the global marine boundary layer

Global Model for Depth‐Dependent Carbonyl Photochemical Production Rates in Seawater

A new sensitive method for the quantification of glyoxal and methylglyoxal in snow and ice by stir bar sorptive extraction and liquid desorption-HPLC-ESI-MS

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