Moch, Jonathan

Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy. 2021. “Global modeling of heterogeneous hydroxymethanesulfonate chemistry.” Atmospheric Chemistry and Physics, 21, 1, Pp. 457–481. Publisher's VersionAbstract
Hydroxymethanesulfonate (HMS) has recently been identified as an abundant organosulfur compound in aerosols during winter haze episodes in northern China. It has also been detected in other regions although the concentrations are low. Because of the sparse field measurements, the global significance of HMS and its spatial and seasonal patterns remain unclear. Here, we modify and add to the implementation of HMS chemistry in the GEOS-Chem chemical transport model and conduct multiple global simulations. The model accounts for cloud entrainment and gas–aqueous mass transfer within the rate expressions for heterogeneous sulfur chemistry. Our simulations can generally reproduce quantitative HMS observations from Beijing and show that East Asia has the highest HMS concentration, followed by Europe and North America. The simulated HMS shows a seasonal pattern with higher values in the colder period. Photochemical oxidizing capacity affects the competition of formaldehyde with oxidants (such as ozone and hydrogen peroxide) for sulfur dioxide and is a key factor influencing the seasonality of HMS. The highest average HMS concentration (1–3 µg m−3) and HMS ∕ sulfate molar ratio (0.1–0.2) are found in northern China in winter. The simulations suggest that aqueous clouds act as the major medium for HMS chemistry while aerosol liquid water may play a role if its rate constant for HMS formation is greatly enhanced compared to cloud water.
Jonathan M. Moch, Eleni Dovrou, Loretta J. Mickley, Frank N. Keutsch, Yuan Cheng, Daniel J. Jacob, Jingkun Jiang, Meng Li, J. William Munger, Xiaohui Qiao, and Qiang Zhang. 2018. “Contribution of hydroxymethane sulfonate to ambient particulate matter: A potential explanation for high particulate sulfur during severe winter haze in Beijing.” Geophysical Research Letters, 45, Pp. 11969-11979. Publisher's VersionAbstract

PM 2.5 during severe winter haze in Beijing, China, has reached levels as high as 880μg/m3, with sulfur compounds contributing significantly to PM 2.5 composition. This sulfur has been traditionally assumed to be sulfate, although atmospheric chemistry models are unable to account for such large sulfate enhancements under dim winter conditions. Using a 1-D model, we show that well-characterized but previously overlooked chemistry of aqueous-phase HCHO and S(IV) in cloud droplets to form a S(IV)-HCHO adduct, hydroxymethane sulfonate, may explain high particulate sulfur in wintertime Beijing. We also demonstrate in the laboratory that methods of ion chromatography typically used to measure ambient particulates easily misinterpret hydroxymethane sulfonate as sulfate. Our findings suggest that HCHO and not SO2 has been the limiting factor in many haze events in Beijing and that to reduce severe winter pollution in this region, policymakers may need to address HCHO sources such as transportation.


GRL paper.pdf