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镍钛层状双氢氧化物@石墨相氮化碳纳米片:一种新型纳米复合材料,具有高光催化和超声光催化性能,可高效降解抗生素。

Ni-Ti Layered Double Hydroxide@Graphitic Carbon Nitride Nanosheet: A Novel Nanocomposite with High and Ultrafast Sonophotocatalytic Performance for Degradation of Antibiotics.

机构信息

Department of Chemistry, Faculty of Basic Sciences , Tarbiat Modares University , Tehran 14115-175 , Iran.

Department of Chemistry, Faculty of Basic Sciences , Azarbaijan Shahid Madani University , Tabriz , Iran.

出版信息

Inorg Chem. 2019 Feb 4;58(3):1834-1849. doi: 10.1021/acs.inorgchem.8b02575. Epub 2019 Jan 16.

Abstract

Pollution of water resources by antibiotics is a growing environmental concern. In this work, nanocomposites of g-CN@Ni-Ti layered double hydroxides (g-CN@Ni-Ti LDH NCs) with high surface areas were synthesized through an optimized hydrothermal method, in the presence of NHF. Application of various characterization techniques unraveled that the prepared nanocomposites are composed of porous Ni-Ti LDH nanoparticles and hierarchical g-CN nanosheets. Further, these NCs were employed for photocatalytic and sonophotocatalytic removal of amoxicillin (AMX), as a model antibiotic, from aqueous solutions. In addition, sonocatalysis was performed. It was found out that the g-CN@Ni-Ti LDH NCs outperform their pure g-CN and Ni-Ti LDH components in photocatalytic degradation of AMX under visible light irradiation. Also, the following order was determined for efficiency of the three adopted processes: sonocatalysis < photocatalysis < sonophotocatalysis. Furthermore, variation of the sonophotocatalysis conditions specified 500 W light intensity, 9 s on/1 s off ultrasound pulse modem and 1.25 g/L g-CN-20@Ni-Ti LDH as the optimal conditions. In this way, optimization of the highly efficient sonophotocatalytic process resulted in 99.5% AMX degradation within 75 min. Moreover, a TOC analyzer was employed to estimate the rate of AMX degradation over the nanocomposites. In addition, formation of hydroxyl radicals (OH) on the surface of the g-CN-20@Ni-Ti LDH particles was approved using the terephthalic acid probe in photoluminescence (PL) spectroscopy. No significant loss was observed in the sonophotocatalytic activity of the nanocomposites even after five consecutive runs. Also, a plausible mechanism was proposed for the sonophotocatalysis reaction. In general, our findings can be considered as a starting point for synthesis of other g-CN-based NCs and application of the resultant nanocomposites to environmental remediation.

摘要

水资源受抗生素污染是一个日益严重的环境问题。在这项工作中,通过优化的水热法,在 NHF 的存在下,合成了具有高表面积的 g-CN@Ni-Ti 层状双氢氧化物(g-CN@Ni-Ti LDH NCs)纳米复合材料。应用各种表征技术揭示,所制备的纳米复合材料由多孔 Ni-Ti LDH 纳米颗粒和分级 g-CN 纳米片组成。此外,这些 NCs 被用于从水溶液中光催化和超声光催化去除阿莫西林(AMX),作为模型抗生素。此外,还进行了声催化。结果发现,在可见光照射下,g-CN@Ni-Ti LDH NCs 在 AMX 的光催化降解方面优于其纯 g-CN 和 Ni-Ti LDH 组分。此外,采用的三种方法的效率确定为:声催化<光催化<超声光催化。此外,还确定了超声光催化条件的变化,指定了 500 W 光强度、9 s 开/1 s 关超声脉冲调制器和 1.25 g/L g-CN-20@Ni-Ti LDH 为最佳条件。通过这种方式,对高效超声光催化过程进行了优化,使 75 分钟内 AMX 的降解率达到 99.5%。此外,还采用 TOC 分析仪来估计纳米复合材料上 AMX 的降解速率。此外,通过光致发光(PL)光谱中的邻苯二甲酸探针证实了在 g-CN-20@Ni-Ti LDH 颗粒表面形成了羟基自由基(OH)。即使在连续五次运行后,纳米复合材料的超声光催化活性也没有明显损失。此外,还提出了超声光催化反应的合理机制。总的来说,我们的发现可以被认为是合成其他基于 g-CN 的 NCs 和将所得纳米复合材料应用于环境修复的起点。

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