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采用 CuFeO/海泡石催化剂催化臭氧化法有效矿化喹啉和生物处理焦化废水:效率和机制。

Effective mineralization of quinoline and bio-treated coking wastewater by catalytic ozonation using CuFeO/Sepiolite catalyst: Efficiency and mechanism.

机构信息

School of Chemical and Environmental Engineering, China University of Mining and Technology (Beijing), Beijing, 100083, PR China.

出版信息

Chemosphere. 2019 Jul;227:647-656. doi: 10.1016/j.chemosphere.2019.04.040. Epub 2019 Apr 11.

Abstract

In this study, CuFeO nanocomposite loaded on natural sepiolite (CuFeO/SEP) was prepared by the citrate sol-gel method. CuFeO/SEP was characterized by X-ray diffraction, Brunauer-Emmett-Teller adsorption analysis, scanning electron microscopy, and energy dispersive spectroscopy. The CuFeO/SEP composite was stable and showed an excellent catalytic activity for ozonation. The efficiency of quinoline mineralization in the catalytic ozonation with CuFeO/SEP was 90.3%, and this value was 5.4 times higher than that of the uncatalyzed ozonation (16.8%). The quinoline mineralization followed a pseudo first-order kinetics with all the catalysts. The rate constant for the mineralization of quinoline by ozonation in the presence of CuFeO/SEP was 0.0885 min, which was 16.7 times higher than that in ozone alone (0.0053 min). Radical scavenging tests revealed that hydroxyl radical (OH) and superoxide radical (O) were the reactive oxygen species (ROS) in the quinoline degradation. In the presence of CuFeO/SEP, ozone and hydrogen peroxide were rapidly converted into the ROS. Although neutral and alkaline pH were more beneficial for the quinoline mineralization, CuFeO/SEP exhibited significant catalytic activity even under acidic conditions. Meanwhile, five-cycle successive tests suggested that CuFeO/SEP was recyclable and hence, stable. Furthermore, the feasibility of the catalytic ozonation for the treatment of biologically treated coking wastewater was evaluated. The catalytic ozonation resulted in 57.81% total organic carbon removal efficiency at 60 min, which was 2.9 times higher than that in the uncatalyzed ozonation (19.99%).

摘要

在这项研究中,通过柠檬酸溶胶-凝胶法制备了负载在天然海泡石上的 CuFeO 纳米复合材料(CuFeO/SEP)。采用 X 射线衍射、BET 吸附分析、扫描电子显微镜和能谱对 CuFeO/SEP 进行了表征。CuFeO/SEP 复合材料稳定,对臭氧氧化表现出优异的催化活性。在 CuFeO/SEP 催化臭氧氧化中,喹啉的矿化效率达到 90.3%,比未催化臭氧氧化(16.8%)高 5.4 倍。喹啉矿化遵循准一级动力学,所有催化剂均如此。在 CuFeO/SEP 存在下,臭氧氧化喹啉的矿化速率常数为 0.0885 min,比单独臭氧(0.0053 min)高 16.7 倍。自由基捕获实验表明,在喹啉降解过程中,羟基自由基(OH)和超氧自由基(O)是活性氧物种(ROS)。在 CuFeO/SEP 的存在下,臭氧和过氧化氢迅速转化为 ROS。尽管中性和碱性 pH 更有利于喹啉矿化,但 CuFeO/SEP 即使在酸性条件下也表现出显著的催化活性。同时,五次连续循环测试表明,CuFeO/SEP 可回收且稳定。此外,还评估了催化臭氧氧化处理生物处理焦化废水的可行性。在 60 min 时,催化臭氧氧化的总有机碳去除效率达到 57.81%,比未催化臭氧氧化(19.99%)高 2.9 倍。

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