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MnO 活化过硫酸盐过程与电解耦联的机制和效率。

The mechanism and efficiency of MnO activated persulfate process coupled with electrolysis.

机构信息

Department of Environmental Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, China; Shenzhen Research Institute of Wuhan University, Shenzhen 518057, China.

Department of Environmental Engineering, Hubei Environmental Remediation Material Engineering Technology Research Center, Wuhan University, Wuhan 430079, China.

出版信息

Sci Total Environ. 2017 Dec 31;609:644-654. doi: 10.1016/j.scitotenv.2017.07.151. Epub 2017 Jul 28.

Abstract

Pure three-dimensional manganese oxides (MnO) were successfully synthesized by a simple one-step hydrothermal process. The obtained particles were characterized via XRD, BET, SEM, XPS and FTIR techniques. To enhance the efficiency of heterogeneous catalytic process, a facile and effective electrochemical method was introduced. The degradation of C. I. Acid Orange 7 (AO7) as the target pollutant in aqueous solution by an oxidation system involving MnO activated peroxydisulfate (PDS) coupled with electrochemical method is reported herein. Influences of some key reaction parameters such as initial pH (pH), current density, initial AO7 concentration, dosage of MnO and anions (Cl, NO, HCO and HPO) were investigated. The cyclic voltammetry (CV) was performed to investigate the charge transfer process occurred at the surface of catalyst. LC-MS/MS analysis was applied to identify degradation intermediates and a plausible degradation mechanism is proposed accordingly. Activated sludge inhibition tests were carried out to evaluate the change of toxicity of the dye solution in the oxidation process. The inorganic by-products such as NO, NO, and NH along with AO7 degradation were also identified. The stability of MnO catalyst was evaluated by recycling experiments and the electrical energy consumption was also investigated. Radical quenching tests with several scavengers (methanol, tert-butyl alcohol, 1,4-benzoquinone and phenol) were performed to clarify the dominating reactive species participating in this oxidation process and the underlying mechanisms involving the generation of radical from the proposed electro-assisted heterogeneous activated PDS system were identified.

摘要

通过简单的一步水热法成功合成了纯三维锰氧化物 (MnO)。通过 XRD、BET、SEM、XPS 和 FTIR 技术对获得的颗粒进行了表征。为了提高多相催化过程的效率,引入了一种简单有效的电化学方法。本文报道了在氧化体系中通过 MnO 激活过二硫酸盐 (PDS) 与电化学方法相结合,以 C.I. 酸性橙 7 (AO7) 为目标污染物在水溶液中的降解。研究了一些关键反应参数的影响,如初始 pH 值 (pH)、电流密度、初始 AO7 浓度、MnO 的用量和阴离子 (Cl、NO、HCO 和 HPO)。进行了循环伏安法 (CV) 以研究催化剂表面发生的电荷转移过程。LC-MS/MS 分析用于鉴定降解中间体,并提出相应的可能降解机制。进行了活性污泥抑制试验以评估氧化过程中染料溶液毒性的变化。还鉴定了 NO、NO 和 NH 等无机副产物以及 AO7 的降解。通过回收实验评估了 MnO 催化剂的稳定性,并研究了电能消耗。通过几种猝灭剂(甲醇、叔丁醇、1,4-苯醌和苯酚)进行了自由基猝灭试验,以阐明参与该氧化过程的主要反应性物质,并确定了从所提出的电辅助多相活化 PDS 系统中生成自由基的潜在机制。

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