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焦炭束缚的环境持久性自由基在过氧化物降解菲中的作用。

Role of coke-bounded environmentally persistent free radicals in phenanthrene degradation by hydrogen peroxide.

机构信息

College of Resources and Environment, Northwest A & F University, Yangling, People's Republic of China.

出版信息

Environ Technol. 2020 Jun;41(16):2122-2129. doi: 10.1080/09593330.2018.1556347. Epub 2018 Dec 17.

Abstract

Emission of polycyclic aromatic hydrocarbons (PAHs) is accompanied with the discharge of carbonaceous particles during the coke production. To degrade the adsorbed PAHs, hydrogen peroxide (HO) was applied as an oxidising agent, which might be activated by the inherent environmentally persistent free radicals (EPFRs) on coke particles. The transformation of phenanthrene (PHE), selected as model molecule, was achieved in HO/coke particle system without the addition of additional activating agent. This process consumed the particle-bounded EPFRs, inducing the decreasing of spin density from 1.92 × 10 to 4.4 × 10 spins g in 30 min of reaction time. Electron paramagnetic resonance (EPR) technique coupled with spin-trapping agent 5, 5-dimethyl-1-pyrroline-N-oxide (DMPO) was used to probe the potential formation of reactive oxygen species. A higher capture [[Formula: see text]] concentration was observed with larger decreases in EPFRs concentration, indicating that EPFRs were the main contributor to the formation of [Formula: see text]. The obtained results suggested that the activation of HO by EPFRs on coke particles resulted in the generation of hydroxyl radical ([Formula: see text]), which then back-reacted with adsorbed PHE. The finding of this study shed light on a new remediation technology for toxic carbonaceous byproducts discharged during the coke production.

摘要

在生产焦炭的过程中,多环芳烃(PAHs)的排放伴随着碳质颗粒的排放。为了降解吸附的多环芳烃,过氧化氢(HO)被用作氧化剂,它可能被焦炭颗粒上固有的环境持久性自由基(EPFRs)激活。在没有添加额外的活化剂的情况下,HO/焦炭颗粒体系中实现了菲(PHE)的转化,选择其作为模型分子。这个过程消耗了颗粒结合的 EPFRs,导致自旋密度从反应时间 30 分钟内的 1.92×10 降至 4.4×10 自旋/g。电子顺磁共振(EPR)技术与自旋捕获剂 5,5-二甲基-1-吡咯啉-N-氧化物(DMPO)结合使用,以探测活性氧物质的潜在形成。观察到更高的捕获 [[Formula: see text]]浓度,同时 EPFRs 浓度的较大降低,表明 EPFRs 是 [Formula: see text]形成的主要贡献者。所得结果表明,HO 通过焦炭颗粒上的 EPFRs 被激活,生成羟基自由基([Formula: see text]),然后与吸附的 PHE 发生反向反应。这项研究的结果为解决焦炭生产过程中排放的有毒碳质副产物提供了一种新的修复技术。

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