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一种可重复使用的可见光驱动 N 和 C-N 掺杂 TiO2 磁性纳米复合材料,用于水中和废水中直接红 16 偶氮染料的光降解。

A reusable visible driven N and C-N doped TiO magnetic nanocomposites for photodegradation of direct red 16 azo dye in water and wastewater.

机构信息

Department of Chemical Engineering, Faculty of Engineering, University of Isfahan, Isfahan, Iran.

Environmental Research Center (ERC), Department of Applied Chemistry, Razi University, Kermanshah, Iran.

出版信息

Environ Technol. 2022 Apr;43(9):1269-1284. doi: 10.1080/09593330.2020.1825530. Epub 2020 Oct 2.

Abstract

The visible active N-doped TiO/ZnFeO (urea-TiO/ZnFeO) and CN-codoped TiO/ZnFeO (L-asparagine-TiO/ZnFeO) nanocomposites were successfully synthesized by the sol-gel-hydrothermal method for direct red 16 (DR16) photodegradation. Their properties of the prepared nanocomposites were analysed using XRD, FT-IR, FE-SEM, EDX, DRS and PL tests. The DRS and PL results confirmed a narrow band-gap energy and low recombination rate of photo-produced electron and hole pairs, respectively. The effect of adding various dopant agents (urea and L-asparagine) with different loadings and magnetic nanoparticle (ZnFeO) into TiO sol on the photodegradation of DR16 was also evaluated. As a result, the L-asparagine (2 wt. %)-TiO/ZnFeO is the best photocatalyst compared to the other modified TiO nanocomposites due to its narrow band gap and high quantum efficiency. The catalyst concentration (1-2 g/L), DR16 concentration (25-45 ppm), initial pH (4-10), and irradiation time (30-90 min) as numerical variables were also considered for photocatalytic process analysis and moulding by central composite design (CCD). The increase in the pH and dye concentration reduces the photodegradation efficiency while irradiation time and catalyst concentration effectively improved its photodegradation efficiency. The DR16 was completely removed at 25 ppm of DR16, initial pH of 4 and 1.5 g/L of photocatalyst after 90-min irradiation. The photoactivity test was also repeated four times by reused L-asparagine-TiO/ZnFeO photocatalyst at optimum conditions. The decrease of dye degradation and loss of photocatalyst were not significant which was approved by the good performance and high recovery capability of the prepared nanocomposite.

摘要

采用溶胶-凝胶-水热法成功合成了可见活性 N 掺杂 TiO/ZnFeO(尿素-TiO/ZnFeO)和 CN 共掺杂 TiO/ZnFeO(L-天冬氨酸-TiO/ZnFeO)纳米复合材料,用于直接红 16(DR16)光降解。通过 XRD、FT-IR、FE-SEM、EDX、DRS 和 PL 测试分析了制备的纳米复合材料的性能。DRS 和 PL 结果分别证实了窄带隙能量和光生电子和空穴对的低复合率。还评估了在 TiO 溶胶中添加不同负载量的各种掺杂剂(尿素和 L-天冬氨酸)和磁性纳米颗粒(ZnFeO)对 DR16 光降解的影响。结果表明,与其他改性 TiO 纳米复合材料相比,由于其窄带隙和高光量子效率,L-天冬氨酸(2wt%)-TiO/ZnFeO 是最佳的光催化剂。还考虑了催化剂浓度(1-2g/L)、DR16 浓度(25-45ppm)、初始 pH(4-10)和照射时间(30-90min)作为数值变量,通过中心组合设计(CCD)进行光催化过程分析和建模。pH 值和染料浓度的增加降低了光降解效率,而照射时间和催化剂浓度则有效地提高了其光降解效率。在 90min 照射后,在 25ppm 的 DR16、初始 pH 值为 4 和 1.5g/L 的光催化剂下,DR16 完全被去除。在最佳条件下,还通过重复使用 L-天冬氨酸-TiO/ZnFeO 光催化剂进行了四次光活性测试。染料降解的减少和光催化剂的损失并不明显,这证明了所制备的纳米复合材料具有良好的性能和高回收能力。

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