Zhang Danna, Lv Guochun, Sun Xiaomin, Zhang Chenxi, Li Zhiqiang
Environment Research Institute, Shandong University Jinan 250100 China
College of Biological and Environmental Engineering, Binzhou University Binzhou 256600 China.
RSC Adv. 2019 Aug 30;9(47):27334-27340. doi: 10.1039/c9ra05193g. eCollection 2019 Aug 29.
Hydroxymethanesulfonate (HMS) is an important organosulfur compound in the atmosphere. In this work, we studied the formation mechanism of HMS the reaction of formaldehyde with dissolved SO using the quantum chemistry calculations. The results show that the barrier (9.7 kcal mol) of the HCHO + HSO reaction is higher than that (1.6 kcal mol) of the HCHO + SO reaction, indicating that the HCHO + SO reaction is easier to occur. For comparison, the reaction of acetaldehyde with dissolved SO also was discussed. The barriers for the CHCHO + HSO reaction and CHCHO + SO reaction are 16.6 kcal mol, 2.5 kcal mol, respectively. This result suggests that the reactivity of HCHO with dissolved SO is higher than that of CHCHO. The further oxidation of CH(OH)SO and CHCH(OH)SO by an OH radical and O shows that the SO˙ radical can be produced.
羟甲磺酸盐（HMS）是大气中一种重要的有机硫化合物。在本工作中，我们利用量子化学计算研究了HMS的形成机制——甲醛与溶解态SO的反应。结果表明，HCHO + HSO反应的势垒（9.7 kcal/mol）高于HCHO + SO反应的势垒（1.6 kcal/mol），这表明HCHO + SO反应更容易发生。为作比较，还讨论了乙醛与溶解态SO的反应。CH₃CHO + HSO反应和CH₃CHO + SO反应的势垒分别为16.6 kcal/mol、2.5 kcal/mol。该结果表明，HCHO与溶解态SO的反应活性高于CH₃CHO。CH(OH)SO₂⁻和CH₃CH(OH)SO₂⁻被OH自由基和O进一步氧化表明可以产生SO₂˙自由基。
