Department of Process Engineering and Chemical Technology, Faculty of Chemistry, Gdańsk University of Technology, G. Narutowicza 11/12, Gdańsk, 80-233, Poland.
Department of Process Engineering and Chemical Technology, Faculty of Chemistry, Gdańsk University of Technology, G. Narutowicza 11/12, Gdańsk, 80-233, Poland.
Chemosphere. 2022 Dec;308(Pt 1):136191. doi: 10.1016/j.chemosphere.2022.136191. Epub 2022 Aug 26.
In the present study, a hybrid photocatalyst of Zn/Ti layered double hydroxide (LDH) coupled with MXene - TiC was synthesized for the first time and applied in photocatalytic degradation of acetaminophen and ibuprofen, two commonly present in the natural environment and prone to accumulate in the aquatic ecosystem pharmaceuticals. The effect of MXene content (0.5 wt%, 2.5 wt%, and 5 wt%) on the photocatalytic activity of LDH/MXene composite was investigated. The composite of LDH/MXene containing 2.5 wt% of MXene revealed the highest photocatalytic activity in the degradation of acetaminophen (100% within 40 min) and ibuprofen (99.7% within 60 min). Furthermore, an improvement in acetaminophen and ibuprofen mineralization was observed for the composite material. Meanwhile, the introduction of interfering ions (Na, Ca, Mg, Cl, SO) in the model seawater did not affect the removal efficiency of both pharmaceuticals. The photocatalytic experiment performed in the four subsequent cycles, as well as FTIR, TEM, and XPS analyses after the photodegradation process confirmed the excellent stability and reusability of the prepared composite material. In order to evaluate the effect of various reactive oxidizing species (ROS) on the photocatalytic process, the trapping experiment was applied. It was noticed that •O had the main contribution in photocatalytic degradation of acetaminophen, while •OH and h mainly affected the degradation of ibuprofen. Finally, based on the results of Mott Schottky analysis, bandgap calculation, and ROS trapping experiment, the possible mechanism for pharmaceuticals degradation was proposed. This research illustrates the feasibility and novelty of the treatment of pharmaceuticals by LDH/MXene composites, implying that MXene plays a significant role in the electron-hole separation and thus high photocatalytic activity.
在本研究中，首次合成了 Zn/Ti 层状双氢氧化物 (LDH) 与 MXene-TiC 的杂化光催化剂，并将其应用于对乙酰氨基酚和布洛芬这两种常见的环境污染物和易在水生态系统中积累的药物的光催化降解。考察了 MXene 含量（0.5wt%、2.5wt%和 5wt%）对 LDH/MXene 复合材料光催化活性的影响。含 2.5wt%MXene 的 LDH/MXene 复合材料在降解乙酰氨基酚（40min 内达到 100%）和布洛芬（60min 内达到 99.7%）方面表现出最高的光催化活性。此外，复合材料中观察到乙酰氨基酚和布洛芬的矿化程度提高。同时，模型海水中引入干扰离子（Na、Ca、Mg、Cl、SO）并不影响两种药物的去除效率。在随后的四个循环中进行了光催化实验，并在光降解过程后进行了 FTIR、TEM 和 XPS 分析，证实了所制备复合材料的优异稳定性和可重复使用性。为了评估各种活性氧化物种（ROS）对光催化过程的影响，进行了捕获实验。结果表明，•O 在乙酰氨基酚的光催化降解中起主要作用，而•OH 和 h 主要影响布洛芬的降解。最后，基于 Mott-Schottky 分析、能带隙计算和 ROS 捕获实验的结果，提出了药物降解的可能机制。本研究说明了 LDH/MXene 复合材料处理药物的可行性和新颖性，表明 MXene 在电子-空穴分离中起着重要作用，从而具有高的光催化活性。
