Elsevier

Atmospheric Research

Volume 248, 15 January 2021, 105227
Atmospheric Research

Spatial distribution and potential sources of methanesulfonic acid in High Asia glaciers

https://doi.org/10.1016/j.atmosres.2020.105227Get rights and content

Highlights

  • The highest level of methanesulfonic acid (MSA) was in Urumqi Glacier No.1 (TS).

  • MSA was correlated with ions from natural dust and biomass in continental glaciers.

  • MSA may be derived from marine environments in Yulong Snow Mountain.

  • The sources of MSA might be hypersaline soil environments and animal husbandry.

Abstract

As a receptor of atmospheric deposition, glaciers are considered an ideal archive in the study of climate change and geochemical cycles. The deposition of methanesulfonic acid (MSA) in the glaciers provides good opportunities to study the biogeochemical cycle of sulfur in the cryosphere. In the present work, snow samples were collected from six High Asia glaciers along a north-to-south transect to determine the spatial distribution of MSA and elucidate its potential sources. The median MSA concentration in the Urumqi Glacier No.1 of Tien Shan was 138.8 ng mL−1, which was distinctly higher than those observed in the Tibetan Plateau (TP) glaciers and polar regions. The levels of MSA in the interior TP glaciers were higher than those observed in the margins of northeastern and southeastern TP. Good correlations between MSA and K+ (r = 0.86, n = 30, α = 0.01), Mg2+ (r = 0.86), and NH4+ (r = 0.73) were observed in continental glaciers. Principal component analysis indicated that MSA may have terrigenous material inputs. At Yulong Snow Mountain, MSA was correlated with Na+ (r = 0.76, n = 8, α = 0.1), a sea-salt tracer ion, suggesting that MSA may be derived from marine environments. According to dimethyl sulfide (DMS) production and NH3 emissions in High Asia, we deduced that the high concentrations of MSA in continental glaciers are possibly related to the sources of hypersaline soil environments and animal husbandry in nomadic areas. This work is useful for further studies on regional sulfur cycling and the impacts of human activities on climate change.

Introduction

The study of climate change is widely accepted to require observation of atmospheric chemical components and exploration of the real significance of its signatures (Barbaro et al., 2017; Müller-Tautges et al., 2015). Glaciers are regarded as a natural reservoir and archive direct and detailed information on atmospheric compositions (Hood et al., 2009; Kang and Cong, 2006). Investigating chemical species deposited on glaciers reveal strategies to deduce their sources, evaluate atmospheric transport and study impacts on climate change. Methanesulfonic acid (CH3SO3H, MSA) is a dimethyl sulfide (DMS, (CH3)2S) oxidation product in the atmosphere (Saigne and Legrand, 1987; Saltzman et al., 1983). In sulfur cycles, sulfur in low valence states is oxidized to high valence states, which can be used as a sulfur source and an energy source by microorganisms (del Valle et al., 2009; Minero et al., 2007). Therefore, MSA, a stable and low-molecular-weight organic acid, is a critical intermediate in the biogeochemical cycle of sulfur (Kelly and Murrell, 1999; Ossola et al., 2019). In addition, MSA can affect new particle formation (NPF) mechanisms and reflection of solar radiation because the oxidation of DMS generates cloud-condensing nuclei and changes the cloud albedo (Dall'Osto et al., 2018; Yoch, 2002). Most MSA studies in snow/ice have been carried out in polar regions. Gibson et al. (1990) and Welch et al. (1993) proposed that MSA concentrations in Antarctic snow/ice were related to sea-ice extent in coastal area. Jaffrezo et al. (1994) found that the high concentrations of MSA in Greenland ice cores appeared in spring and summer due to marine biological activities in the surrounding ocean. Then, studies on ice core records in Antarctica and Svalbard confirmed that MSA can be considered a proxy of marine primary production (Abram et al., 2013; Weller et al., 2004). What's more, the related history records can reflect 10-year and low-frequency climate changes (Isaksson et al., 2001; Osman et al., 2017).

High Asia, located at low-middle latitudes of the Northern Hemisphere, is centered on the Tibetan Plateau (TP). Glaciers are widely distributed in High Asia and sensitive to climate change (Kang and Cong, 2006; Li et al., 2018). Understanding the characteristics and sources of MSA is helpful for the study on snow chemistry, regional sulfur cycling and glacial microbial activities. However, the lack of knowledge about MSA in terrestrial environments makes the understanding of its environmental behavior and significance incomplete. Thus far, only Sun et al. (1998) paid attention to MSA in Guliya ice cores, which was below the limit of detection. In the present work, we measured the concentrations of MSA in High Asia glaciers, determined its spatial distribution and elucidated its potential sources. The main goals are to supply the data of MSA in terrestrial environments, promote future studies on its real significance and reveal its impacts on climate change.

Section snippets

Snow sampling sites

Snow samples were collected over six highly representative glaciers in High Asia, extending from the dry region of the north to the moist region of the southeast (Fig. 1), including the Urumqi Glacier No.1 of Tien Shan (TS, outside the TP), the Laohugou Glacier No.12 (LHG, the margin of the northeastern TP), the Muztagh Glacier (MZTG, the northern TP), the Meikuang Glacier (MK, the northern TP), the Dongkemadi Glacier (DKMD, the central TP) and the Yulong Snow Mountain (YL, the margin of the

Spatial distribution of MSA in High Asia glaciers

The median MSA concentration was selected to avoid interference from outliers. As shown in Fig. 2, MSA was spatially distributed in the following decreasing order: TS (138.8 ng mL−1) > DKMD (33.67 ng mL−1) > MK (21.36 ng mL−1) > MZTG (15.95 ng mL−1) > LHG (9.71 ng mL−1) > YL (3.76 ng mL−1). MSA concentrations in TS were mostly between the lower quartile (132.18 ng mL−1, α = 0.01) and the upper quartile (160.11 ng mL−1), which were distinctly higher than those in the TP glaciers. In the TP

Conclusions

Snow samples were collected from High Asia glaciers, which were represented wet/dry deposition in spring and summer. The median MSA concentrations were spatially distributed in the decreasing order of TS > DKMD> MK > MZTG > LHG > YL. MSA concentrations decreased from south to north in continental TP glaciers. There was a considerable difference in concentration of MSA among TS, the TP glaciers and polar regions. In continental glaciers, positive correlations between MSA and some ions (K+, Mg2+

Author statement

Manuscript title: Spatial distribution and potential sources of methanesulfonic acid in High Asia glaciers.

Yao Li: Conceptualization, Formal analysis, Writing - Original Draft, Writing - Review & Editing.

Ninglian Wang: Resources.

Carlo Barbante: Resources.

Shichang Kang: Resources.

Hewen Niu: Investigation, Writing - Review & Editing.

Xiaobo Wu: Formal analysis, Writing - Review & Editing.

Elena Barbaro: Resources, Writing - Review & Editing.

Elena Argiriadis: Resources, Writing - Review & Editing.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

This work was funded by the National Natural Science Foundation of China [grant numbers 41971090, 41721091] and “Strategic priority research program” of the Chinese Academy of Sciences [grant number XDA19070503]. We gratefully thank the fieldwork staff for their hard and excellent glacier sampling work. The authors acknowledge the State Key Laboratory of Cryospheric Science for providing the space to run the instruments. The authors also acknowledge Ca’ Foscari University of Venice for the

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