Insight into the in-cloud formation of oxalate based on in situ measurement by single particle mass spectrometry

Zhang, Guohua; Lin, Qinhao; Peng, Long; Yang, Yuxiang; Fu, Yuzhen; Bi, Xinhui; Li, Mei; Chen, Duohong; Chen, Jianxin; Cai, Zaisheng; Wang, Xinming; Peng, Ping’an; Sheng, Guoying; Zhou, Zhen

doi:10.5194/acp-17-13891-2017

Cited by 44 publications

(44 citation statements)

References 67 publications

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“…The aqueous oxidation pathway of organic precursors was an important contributor to the in-cloud formation of oxalate (Sorooshian et al, 2007;Zhang et al, 2017b (Ervens et al, 2004;Lim et al, 2005;Sorooshian et al, 2006). A peak at m/z −59 might also originate from the presence of [HCNO 2 ] − or levoglucosan (Bi et al, 2011).…”

Section: The Impact Of Cloud Processing On Oxalate Precursors and Oxamentioning

confidence: 99%

“…Iron (Fe)-containing particles were frequently detected in the atmosphere, with concentration ranging from 10 ng m −3 over remote marine environments to 28 µg m −3 near desert areas (Zhang et al, 2003;Fomba et al, 2013). The Fe-containing particles have an adverse effect on human health, causing issues such as DNA strand breakage and cell damage (See et al, 2007;Abbaspour et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

“…We have previously used a ground-based counterflow virtual impactor (GCVI) combined and a real-time singleparticle aerosol mass spectrometer (SPAMS) to characterize chemical composition or the mixing state of cloud residues (Lin et al, 2017), the mixing state and cloud scavenging of the EC-containing particles (Zhang et al, 2017a), and the in-cloud formation of oxalate (Zhang et al, 2017b) at a mountain site in southern China. In this study, the same combined technology was utilized to obtain information on the characteristics and potential sources of Fe-containing cloud residues.…”

Section: Introductionmentioning

confidence: 99%

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In-cloud formation of secondary species in iron-containing particles

Lin

Zhang

et al. 2019

Atmos. Chem. Phys.

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Abstract. The increase in secondary species through cloud processing potentially increases aerosol iron (Fe) bioavailability. In this study, a ground-based counterflow virtual impactor coupled with a real-time single-particle aerosol mass spectrometer was used to characterize the formation of secondary species in Fe-containing cloud residues (dried cloud droplets) at a mountain site in southern China for nearly 1 month during the autumn of 2016. Fe-rich, Fe-dust, Fe-elemental carbon (Fe-EC), and Fe-vanadium (Fe-V) cloud residual types were obtained in this study. The Fe-rich particles, related to combustion sources, contributed 84 % (by number) to the Fe-containing cloud residues, and the Fe-dust particles represented 12 %. The remaining 4 % consisted of the Fe-EC and Fe-V particles. It was found that above 90 % (by number) of Fe-containing particles had already contained sulfate before cloud events, leading to no distinct change in number fraction (NF) of sulfate during cloud events. Cloud processing contributed to the enhanced NFs of nitrate, chloride, and oxalate in the Fe-containing cloud residues. However, the in-cloud formation of nitrate and chloride in the Fe-rich type was less obvious relative to the Fe-dust type. The increased NF of oxalate in the Fe-rich cloud residues was produced via aqueous oxidation of oxalate precursors (e.g., glyoxylate). Moreover, Fe-driven Fenton reactions likely increase the formation rate of aqueous-phase OH, improving the conversion of the precursors to oxalate in the Fe-rich cloud residues. During daytime, the decreased NF of oxalate in the Fe-rich cloud residues was supposed to be due to the photolysis of Fe-oxalate complexes. This work emphasizes the role of combustion Fe sources in participating in cloud processing and has important implications for evaluating Fe bioavailability from combustion sources during cloud processing.

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Section: The Impact Of Cloud Processing On Oxalate Precursors and Oxamentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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In-cloud formation of secondary species in iron-containing particles

Lin

Zhang

et al. 2019

Atmos. Chem. Phys.

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“…Cloud INT particles were regarded as PM 2.5 during the cloud events. More detailed description on the sampling can be found in the companion papers Zhang et al, 2017).…”

Section: Sampling Setupmentioning

confidence: 99%

The single-particle mixing state and cloud scavenging of black carbon: a case study at a high-altitude mountain site in southern China

et al. 2017

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Abstract. In the present study, a ground-based counterflow virtual impactor (GCVI) was used to sample cloud droplet residual (cloud RES) particles, while a parallel PM 2.5 inlet was used to sample cloud-free or cloud interstitial (cloud INT) particles. The mixing state of black carbon (BC)-containing particles and the mass concentrations of BC in the cloud-free, RES and INT particles were investigated using a single-particle aerosol mass spectrometer (SPAMS) and two aethalometers, respectively, at a mountain site (1690 m a.s.l.) in southern China. The measured BCcontaining particles were extensively internally mixed with sulfate and were scavenged into cloud droplets (with number fractions of 0.05-0.45) to a similar (or slightly lower) extent as all the measured particles (0.07-0.6) over the measured size range of 0.1-1.6 µm. The results indicate the preferential activation of larger particles and/or that the production of secondary compositions shifts the BC-containing particles towards larger sizes. BC-containing particles with an abundance of both sulfate and organics were scavenged less than those with sulfate but limited organics, implying the importance of the mixing state on the incorporation of BCcontaining particles into cloud droplets. The mass scavenging efficiency of BC with an average of 33 % was similar for different cloud events independent of the air mass. This is the first time that both the mixing state and cloud scavenging of BC in China have been reported. Our results would improve the knowledge on the concentration, mixing state, and cloud scavenging of BC in the free troposphere.

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“…The aqueous oxidation pathway of organic precursors was an important contributor to the incloud formation of oxalate (Sorooshian et al, 2007;Zhang et al, 2017) suggested as the main precursors for the formation of oxalate in the atmospheric aqueous phase (Ervens et al, 2004;Lim et al, 2005;Sorooshian et al, 2006). Increased NFs of these precursors were clearly identified in the Fe-containing cloud residues (38%) and interstitial particles (35%) compared to cloud-free particles (26%) (Figure 3).…”

Section: The Impact Of Cloud Processing On Oxalate Precursors and Oxamentioning

confidence: 96%

In-cloud formation of secondary species in iron-containing particles

Lin¹,

Bi²,

Zhang³

et al. 2018

Preprint

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<p><strong>Abstract.</strong> The increase of secondary species through cloud processing potentially increases aerosol iron (Fe) bioavailability. In this study, a ground-based counterflow virtual impactor coupled with a real-time single-particle aerosol mass spectrometer was used to characterize the formation of secondary species in Fe-containing cloud residues (dried cloud droplets) at a mountain site in southern China for nearly one month during the autumn of 2016. Fe-rich, Fe-dust, Fe-elemental carbon (Fe-EC), and Fe-vanadium (Fe-V) cloud residual types were obtained in this study. The Fe-rich particles, related to combustion sources, contributed 84&#8201;% to the Fe-containing cloud residues, and the Fe-dust particles represented 12&#8201;%. The remaining 4&#8201;% consisted of the Fe-EC and Fe-V particles. It was found that extremely high amounts of sulfate had already accumulated on the Fe-containing particles before cloud events, leading to no distinct changes in sulfate during cloud events. Cloud processing contributed to the enhancement of nitrate, chloride, and oxalate in the Fe-containing cloud residues. However, the in-cloud formation of nitrate and chloride in the Fe-rich type was less obvious relative to the Fe-dust type. The enhancement of oxalate in the Fe-rich cloud residues was produced via aqueous oxidation of oxalate precursors (e.g., glyoxylate). Moreover, Fe chemistry involved in the Fenton reaction further promoted the conversion of the oxalate precursors to oxalate during cloud events, although the photolysis of Fe-oxalate complexes also existed in the Fe-rich cloud residues. This work emphasizes the role of combustion Fe sources in participating in cloud processing and has important implications for evaluating Fe bioavailability from combustion sources during cloud processing.</p>

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Insight into the in-cloud formation of oxalate based on in situ measurement by single particle mass spectrometry

Cited by 44 publications

References 67 publications

In-cloud formation of secondary species in iron-containing particles

In-cloud formation of secondary species in iron-containing particles

The single-particle mixing state and cloud scavenging of black carbon: a case study at a high-altitude mountain site in southern China

In-cloud formation of secondary species in iron-containing particles

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