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采用磁组装 mZVI/DSA 阳极提升复杂水基质的过氧-混凝处理效果:ClO 自由基的重要性。

Upgrading the peroxi-coagulation treatment of complex water matrices using a magnetically assembled mZVI/DSA anode: Insights into the importance of ClO radical.

机构信息

Tianjin Key Laboratory of Clean Energy and Pollution Control, School of Energy and Environment Engineering, Hebei University of Technology, Tianjin, 300401, China.

School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin, 300130, China.

出版信息

Chemosphere. 2022 Sep;303(Pt 1):134948. doi: 10.1016/j.chemosphere.2022.134948. Epub 2022 May 13.

Abstract

The electrochemical technologies for water treatment have flourished over the last decades. However, it is still challenging to treat the actual complex water effluents by a single electrochemical process, often requiring coupling of technologies. In this study, an upgraded peroxi-coagulation (PC) process with a magnetically assembled mZVI/DSA anode has been devised for the first time. COD, NH-N and total phosphorous were simultaneously and effectively removed from livestock wastewater. The advantages, influence of key parameters and evolution of electrogenerated species were systematically investigated to fully understand this novel PC process. The fluorescent substances in livestock wastewater could also be almost removed under optimal conditions (300 mA, 0.2 g ZVI particles and pH 6.8). The interaction between OH and active chlorine yielded ClO with a high steady-state concentration of 6.85 × 10 M, which did not cause COD removal but accelerated the oxidation of NH-N. The Mulliken population suggested that OH and NH-N had similar electron-donor behavior, whereas ClO acted as an electron-withdrawing species. Besides, although the energy barrier for the reaction between OH and NH-N (17.0 kcal/mol) was lower than that with ClO (18.8 kcal/mol), considering the tunneling in the H abstraction reaction, the Skodje-Truhlar method adopted for calculations evidenced a 17-fold faster NH-N oxidation rate with ClO. In summary, this work describes an advantageous single electrochemical process for the effective treatment of a complex water matrix.

摘要

电化学水处理技术在过去几十年中得到了蓬勃发展。然而,通过单一电化学工艺处理实际复杂水废水仍然具有挑战性,通常需要多种技术的结合。在这项研究中,首次设计了一种带有磁组装 mZVI/DSA 阳极的升级过的过氧-凝聚(PC)工艺,用于同时有效地从牲畜废水中去除 COD、NH-N 和总磷。系统地研究了优势、关键参数的影响和电生成物质的演变,以充分理解这种新的 PC 工艺。在最佳条件下(300 mA、0.2 g ZVI 颗粒和 pH 6.8),牲畜废水中的荧光物质也几乎可以被去除。OH 和活性氯之间的相互作用产生了 ClO,其稳态浓度高达 6.85×10 M,这不会导致 COD 去除,但会加速 NH-N 的氧化。Mulliken 种群表明,OH 和 NH-N 具有相似的电子供体行为,而 ClO 则充当电子受体物质。此外,尽管 OH 和 NH-N 之间的反应(17.0 kcal/mol)的能垒低于与 ClO 的反应(18.8 kcal/mol),但考虑到 H 提取反应中的隧道效应,用于计算的 Skodje-Truhlar 方法表明,ClO 使 NH-N 氧化速率快 17 倍。总之,这项工作描述了一种有利的单一电化学工艺,可有效处理复杂的水基质。

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