Ultrasonics Sonochemistry ( IF 8.7 ) Pub Date : 2021-09-10 , DOI: 10.1016/j.ultsonch.2021.105750 Qihui Xu 1 , Hong Zhang 2 , Haoran Leng 1 , Hong You 3 , Yuhong Jia 2 , Shutao Wang 1
The novel system, consisting of composite oxidants (persulfate/chlorite, S2O82−/ClO2−) and stationary phase activator (zero-valent-iron foam, Fe0f) driven by ultrasonic (US) field, was applied to treat the triphenylmethane derivative effectively even at low temperature (≈ 289 K). By comparisons of sub-systems, the US roles to S2O82−, ClO2−, and Fe0f were seriatim analyzed. US made the reaction order of multi-component system tend to within 1 (leading to de-order reaction), and widened pH activating range of the Fe0f by sonicate-polishing during the process of ClO2− co-activating S2O82−. US and Fe0f were affected by fluid eddy on activating S2O82−/ClO2−. The Fe0f had slight effect on the temperature of US bubble-water interface but the addition of ClO2− lowered it. The partitioning capacity of the above US reactive zone increased during the reaction. US and ClO2− could enrich the kinds of degradation intermediates. The contributions of free radicals (ClOx-based radicals, sulfate radicals (SO4−), and hydroxyl radicals (OH)) and non-free radicals (ClO2, and O = FeIV/V from ionic Fe under “-O-O-” of S2O82− and cyclic adjustment reaction of ClO2−) processes by sonochemical induction were equally important by corresponding detection means. Especially, real-time and online high-resolution mass spectrum by self-developing further confirmed the chain transfers of different free radicals due to US role. The findings expanded the application of sono-persulfate-based systems and improved understanding on activation mechanism.
中文翻译:
超声波作用与泡沫零价铁活化过硫酸盐/亚氯酸盐:声化学应用和诱导机制
该新型系统由超声波(US)场驱动的复合氧化剂(过硫酸盐/亚氯酸盐,S 2 O 8 2− /ClO 2 − )和固定相活化剂(零价铁泡沫,Fe 0 f )组成。即使在低温(约 289 K)下也能有效处理三苯甲烷衍生物。通过子系统比较,依次分析了US对S 2 O 8 2− 、ClO 2 − 、Fe 0 f的作用。 US使多组分体系的反应级数趋于1以内(导致失序反应),并在ClO 2 -共活化S 2 O过程中通过超声抛光拓宽了Fe 0 f的pH活化范围8 2− . US和Fe 0 f在激活S 2 O 8 2− /ClO 2 −时受到流体涡流的影响。 Fe 0 f对US 气泡-水界面的温度影响较小,但ClO 2 -的添加降低了它。上述US反应区的分配能力在反应过程中增加。 US和ClO 2 -可以丰富降解中间体的种类。 自由基(ClO x基自由基、硫酸根(SO 4 − ) 和羟基自由基 ( OH)) 和非自由基(ClO 2 ,以及在 S 2 O 8 2−的“-OO-”下来自离子 Fe 的 O = Fe IV/V和 ClO 2 −的循环调节反应)通过声化学诱导的过程是相同的重要的是通过相应的检测手段。尤其是自主研发的实时在线高分辨率质谱进一步证实了美国作用下不同自由基的链式转移。这些发现扩大了基于声波过硫酸盐的系统的应用,并提高了对激活机制的理解。