Impacts of Hydroperoxymethyl Thioformate on the Global Marine Sulfur Budget,ACS Earth and Space Chemistry

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Impacts of Hydroperoxymethyl Thioformate on the Global Marine Sulfur Budget
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2021-09-08 , DOI: 10.1021/acsearthspacechem.1c00218
M. Anwar H. Khan ₁ , Thomas J. Bannan ₂ , Rayne Holland ₁ , Dudley E. Shallcross ₁ , Alex T. Archibald _{3,

4} , Emily Matthews ₂ , Asan Back ₂ , James Allan _{2,

5} , Hugh Coe ₂ , Paulo Artaxo ₆ , Carl J. Percival _{2,

7}

Affiliation

Hydroperoxymethyl thioformate (HPMTF) is a newly identified major oxidation product of dimethyl sulfide (DMS). It is speculated that it could act as a major reservoir of marine sulfur, but its fate in the atmosphere is currently unknown. In this study, we have investigated the formation of HPMTF through the oxidation of DMS by OH, NO₃ and Cl radicals and its losses through photolysis, OH oxidation, dry deposition, and wet deposition using the global 3-dimensional chemical transport model, STOCHEM-CRI. The model results suggest that the distribution of loss processes for HPMTF are photolysis (46%) and wet deposition (31%) with additional contributions from dry deposition (13%) and OH oxidation (10%). The global burden and the tropospheric lifetime of HPMTF are found to be 0.052 Tg and 0.5 days, respectively. The model integrations agree well with both aircraft derived measurements of HPMTF over the ocean surface between 80 °N and 85 °S latitudes and ground-based measurements made in the central Amazon. These ground-based data reveal a clear diurnal cycle with a maximum during midday, consistent with other recently reported data and possibly due to the dominance of the photochemical production rather than the photolytic loss. Accounting for HPMTF chemistry results in a significant decrease in boundary layer levels of SO₂ and H₂SO₄ but increases in sulfate aerosol in the upper troposphere. We suggest that these changes could have important consequences on preindustrial to present-day radiative forcing from sulfate aerosol.

中文翻译：

硫代甲酸氢过氧甲酯对全球海洋硫收支的影响

氢过氧甲基硫代甲酸酯 (HPMTF) 是一种新发现的二甲硫醚 (DMS) 的主要氧化产物。据推测，它可能是海洋硫磺的主要储存库，但目前尚不清楚它在大气中的命运。在这项研究中，我们研究了通过 OH、NO ₃氧化 DMS 形成 HPMTF和 Cl 自由基及其通过光解、OH 氧化、干沉积和湿沉积的损失，使用全局 3 维化学传输模型，STOCHEM-CRI。模型结果表明 HPMTF 的损失过程分布是光解 (46%) 和湿沉积 (31%)，干沉积 (13%) 和 OH 氧化 (10%) 的额外贡献。HPMTF 的全球负荷和对流层寿命分别为 0.052 Tg 和 0.5 天。模型集成与飞机在 80 °N 和 85 °S 纬度之间的海面上对 HPMTF 进行的测量以及在亚马逊中部进行的地面测量都非常吻合。这些基于地面的数据揭示了一个清晰的昼夜循环，最大值在中午，与其他最近报道的数据一致，可能是由于光化学生产占主导地位而不是光解损失。考虑 HPMTF 化学导致 SO 边界层水平显着降低₂和 H ₂ SO _{4 ，}但在对流层上部的硫酸盐气溶胶中增加。我们认为，这些变化可能对工业化前到现代硫酸盐气溶胶的辐射强迫产生重要影响。

更新日期：2021-10-22

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