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超声激活过硫酸盐/亚氯酸盐与泡沫零价铁的作用:声化学应用和诱导机制。

Ultrasonic role to activate persulfate/chlorite with foamed zero-valent-iron: Sonochemical applications and induced mechanisms.

机构信息

State Key Laboratory of Urban Water Resources and Environment, Harbin Institute of Technology, Harbin 150090, China.

School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, China.

出版信息

Ultrason Sonochem. 2021 Oct;78:105750. doi: 10.1016/j.ultsonch.2021.105750. Epub 2021 Sep 10.

Abstract

The novel system, consisting of composite oxidants (persulfate/chlorite, SO/ClO) and stationary phase activator (zero-valent-iron foam, Fe) 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 SO, ClO, and Fe 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 Fe by sonicate-polishing during the process of ClO co-activating SO. US and Fe were affected by fluid eddy on activating SO/ClO. The Fe had slight effect on the temperature of US bubble-water interface but the addition of ClO lowered it. The partitioning capacity of the above US reactive zone increased during the reaction. US and ClO could enrich the kinds of degradation intermediates. The contributions of free radicals (ClO-based radicals, sulfate radicals (SO), and hydroxyl radicals (OH)) and non-free radicals (ClO, and O = Fe from ionic Fe under "-O-O-" of SO and cyclic adjustment reaction of ClO) 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.

摘要

新型体系由复合氧化剂(过硫酸盐/亚氯酸盐,SO/ClO)和固定相激活剂(零价铁泡沫,Fe)组成,在超声(US)场的驱动下,即使在低温(≈289 K)下也能有效地处理三苯甲烷衍生物。通过对亚系统的比较,依次分析了 US 在 SO、ClO 和 Fe 中的作用。US 使多组分体系的反应级数趋于 1(导致去序反应),并在 ClO 共同激活 SO 的过程中通过超声研磨拓宽了 Fe 的 pH 激活范围。US 和 Fe 受流体涡旋在激活 SO/ClO 时的影响。Fe 对 US 泡-水界面温度的影响较小,但 ClO 的加入会降低其温度。上述 US 反应区的分配容量在反应过程中增加。US 和 ClO 可以富集各种降解中间产物。通过相应的检测手段,自由基(基于 ClO 的自由基、硫酸根自由基(SO)和羟基自由基(OH))和非自由基(ClO 和来自 SO 的“-O-O-”下的离子 Fe 的 O=Fe 以及 ClO 的循环调整反应)过程的声化学诱导的贡献同样重要。特别是,通过自行开发的实时和在线高分辨率质谱进一步证实了由于 US 作用,不同自由基的链转移。这些发现扩展了超声过硫酸盐体系的应用,并提高了对激活机制的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/03fd/8455865/7f78966a1065/gr9.jpg

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