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天然针铁矿催化臭氧化降解水溶液中的 N, N-二甲基乙酰胺(DMAC):动力学、性能、生物毒性和机制。

Natural mackinawite catalytic ozonation for N, N-dimethylacetamide (DMAC) degradation in aqueous solution: Kinetic, performance, biotoxicity and mechanism.

机构信息

Department of Environmental Science and Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.

Haitian Water Group Co., Ltd, Chengdu 610065, China.

出版信息

Chemosphere. 2018 Nov;210:831-842. doi: 10.1016/j.chemosphere.2018.07.072. Epub 2018 Jul 17.

Abstract

To enhance the degradation of N, N-dimethylacetamide (DMAC) in aqueous solution, the natural mackinawite (NM) is introduced for catalytic ozonation in this study as it is an environmentally friendly catalyst with low cost and easy availability. The properties of the NM were initially characterized via scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), Fourier Transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Then, impact factors including NM dosage, ozone gas concentration and initial pH were investigated and the optimal conditions (i.e., NM dosage = 3.5 g/L, ozone gas concentration = 300 L/min, initial pH = 6.8) were obtained in NM/O3 process. Besides, the superiority of the NM/O process was confirmed by the experiments that the degradation efficiency of DMAC in the NM/O process (i.e., 95.4%) was much higher than that in the zero-valent iron (ZVI)/O process (i.e., 46.1%) and the synthetic FeS/O process (i.e., 68.6%). Furthermore, the intermediate and possible degradation pathway of DMAC were proposed, and the biological toxicity of the intermediate was subsequently evaluated by the activated sludge. Finally, the mechanism of the NM/O3 process was proposed in this study based on control experiment and radical scavenging experiment. The extraordinary efficiency for DMAC degradation was found to be mainly caused by HO of the reactive oxygen species (ROS) (i.e., HO, O and HO) generated in the NM/O process. Therefore, this study confirmed that NM was a high efficient catalyst for degradation the toxic and refractory pollutants in catalytic ozonation system.

摘要

为了增强 N,N-二甲基乙酰胺(DMAC)在水溶液中的降解,本研究引入了天然磁黄铁矿(NM)进行催化臭氧化,因为它是一种具有成本低、易得的环保型催化剂。NM 的性质通过扫描电子显微镜(SEM)、能量色散 X 射线光谱(EDS)、X 射线衍射(XRD)、傅里叶变换红外光谱(FTIR)和 X 射线光电子能谱(XPS)进行了初步表征。然后,考察了影响因素,包括 NM 用量、臭氧气体浓度和初始 pH 值,并在 NM/O3 工艺中获得了最佳条件(即 NM 用量为 3.5g/L、臭氧气体浓度为 300L/min、初始 pH 值为 6.8)。此外,NM/O 工艺的优越性通过实验得到了证实,即在 NM/O 工艺中 DMAC 的降解效率(即 95.4%)远高于零价铁(ZVI)/O 工艺(即 46.1%)和合成 FeS/O 工艺(即 68.6%)。此外,提出了 DMAC 的中间产物和可能的降解途径,并随后通过活性污泥评价了中间产物的生物毒性。最后,根据对照实验和自由基清除实验,提出了 NM/O3 工艺的机理。在 NM/O 工艺中,发现 HO 等活性氧物种(ROS)中的 HO(即 HO、O 和 HO)产生的非凡的 DMAC 降解效率是主要原因。因此,本研究证实 NM 是一种高效的催化剂,可用于催化臭氧化系统中降解有毒和难降解污染物。

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