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基于 TiO2 的(FeO、SiO、还原氧化石墨烯)磁性可回收光催化剂用于合成废水中的 imazalil 降解。

TiO-based (FeO, SiO, reduced graphene oxide) magnetically recoverable photocatalysts for imazalil degradation in a synthetic wastewater.

机构信息

Grupo FEAM, Unidad Asociada al CSIC (a través del ICCMM de Sevilla), i-UNAT - Universidad de Las Palmas de Gran Canaria, Edificio del Parque Científico Tecnológico de la ULPGC, 35017, Las Palmas, Spain.

Dpto. de Ingeniería de Procesos, Universidad de Las Palmas De Gran Canaria, Campus Universitario de Tafira, 35017, Las Palmas, Spain.

出版信息

Environ Sci Pollut Res Int. 2018 Oct;25(28):27724-27736. doi: 10.1007/s11356-018-1586-1. Epub 2018 Mar 2.

Abstract

Magnetite (FeO), a core-shell material (SiO@FeO), and reduced graphene oxide-FeO (referred as rGO-MN) were used as supports of a specific highly active TiO photocatalyst. Thermal treatments at 200 or 450 °C, different atmospheres (air or N), and TiO:support weight ratios (1.0, 1.5, or 2.0) were investigated. X-ray diffractograms revealed that magnetite is not oxidized to hematite when the core-shell SiO@FeO material-or a N atmosphere (instead of air) in the thermal treatment-was employed to prepare the TiO-based catalysts (the magnetic properties being preserved). The materials treated with N were first tested for degradation of imazalil (a well-known fungicide) in deionized water. The best compromise between the photocatalytic activity, magnetic separation, and Fe leached (1.61 mg L, i.e., below the threshold for water reuse in irrigation) was found for the magnetic catalyst prepared with SiO@FeO, an intermediate TiO:support ratio (1.5), and treated at 200 °C under N atmosphere (i.e., SiO@FeO-EST-1.5-200-N). This material was then tested for the treatment of imazalil in a synthetic wastewater, SW (with a chemical composition simulating an effluent resulting from fruit postharvest activity). This SW has a pH of 4.2 and the experiments were carried out at this natural pH and at neutral conditions (keeping pH at 7 along the reaction). The magnetic catalyst was more active than bare TiO for the treatment of imazalil in SW at natural pH. Since Fe leaching was observed (3.53 mg L), added HO enhanced both imazalil degradation and mineralization. Conveniently, these catalysts can be readily recovered by using a conventional magnetic field, as demonstrated over three consecutive recycling runs. Graphical abstract % Imazalil conversion using different magnetic catalysts and comparison with bare TiO.

摘要

磁铁矿 (FeO)、核壳材料 (SiO@FeO) 和还原氧化石墨烯-FeO(简称 rGO-MN)被用作特定高活性 TiO2 光催化剂的载体。研究了在 200 或 450°C 下进行的热处理、不同气氛(空气或 N2)以及 TiO2:载体重量比(1.0、1.5 或 2.0)。X 射线衍射图表明,当使用核壳 SiO@FeO 材料或 N2 气氛(而不是空气)进行热处理来制备 TiO2 基催化剂时,磁铁矿不会被氧化为赤铁矿(保留其磁性)。用 N2 处理的材料首先用于在去离子水中降解恶咪唑(一种著名的杀菌剂)。在 N2 气氛下、200°C 热处理的 SiO@FeO-EST-1.5-200-N 磁性催化剂表现出最佳的光催化活性、磁性分离和铁浸出(1.61mg/L,即低于灌溉再利用的阈值)之间的平衡。然后,该材料用于处理合成废水 SW(其化学成分模拟水果采后处理活动产生的废水)中的恶咪唑。SW 的 pH 值为 4.2,实验在自然 pH 值和中性条件下(在反应过程中保持 pH 值为 7)进行。在自然 pH 值下,磁性催化剂比 TiO2 更有效地处理 SW 中的恶咪唑。由于观察到铁浸出(3.53mg/L),因此添加 HO 可增强恶咪唑的降解和矿化。方便地是,这些催化剂可以通过使用常规磁场很容易地回收,在三个连续的回收运行中得到了证明。

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