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Effects of oxalate on Fe-catalyzed photooxidation of dissolved sulfur dioxide in atmospheric water

机译：草酸盐对铁催化大气水中溶解的二氧化硫的光氧化作用

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Fe-catalyzed photochemical oxidation of dissolved sulfur dioxide (SO_2), S(Ⅳ), in the presence of oxalate has been studied under the conditions typical for acidified atmospheric water. The Fe(Ⅲ)-catalyzed oxidation of S(Ⅳ) is first order with respect to S(Ⅳ) concentration in the absence of oxalate. The presence of oxalate strongly inhibits Fe(Ⅲ)-catalyzed S(Ⅳ) oxidation due to the formation of Fe(Ⅲ)-oxalato complexes both in the dark and under UV-visible light. However, under UV-visible light irradiation, the generation of photooxidants, such as H_2O_2 and OH radicals, by photochemical/chemical cycling of Fe(Ⅲ)/Fe(Ⅱ)-oxalato complexes, leads to the photochemical oxidation of S(Ⅳ). The initial oxidation rate increases with oxalate and Fe(Ⅲ) concentration in the concentration ranges studied. The rate of Fe(Ⅲ)-cataIyzed photochemical oxidation of S(Ⅳ) in the presence of oxalate increases with increasing pH value of reaction solution and with decreasing irradiation wavelength. The concentrations of oxalate and other organic ligands are sufficiently large to significantly change the rates of Fe-catalyzed oxidation of dissolved SO_2 in atmospheric water droplets during both day- and night time.
机译：在草酸存在的条件下，研究了铁在草酸盐存在下催化的可溶性二氧化硫（SO_2），S（Ⅳ）的光化学氧化。在草酸不存在下，Fe（Ⅲ）催化的S（Ⅳ）氧化相对于S（Ⅳ）浓度是一阶的。草酸盐的存在强烈抑制了Fe（Ⅲ）催化的S（Ⅳ）的氧化，这是由于在黑暗和紫外可见光下都形成了Fe（Ⅲ）-草酸络合物。然而，在紫外可见光照射下，Fe（Ⅲ）/ Fe（Ⅱ）-草酸酯络合物的光化学/化学循环产生H_2O_2和OH自由基等光氧化剂，导致S（Ⅳ）的光化学氧化。在所研究的浓度范围内，初始氧化速率随草酸盐和Fe（Ⅲ）浓度的增加而增加。草酸盐存在下，Fe（Ⅲ）催化的S（Ⅳ）光化学氧化速率随反应溶液pH值的增加和照射波长的减小而增加。草酸盐和其他有机配体的浓度足够大，足以在白天和晚上的时间内显着改变Fe催化的大气水滴中溶解的SO_2氧化的速率。

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