Yi Chunlin, Song Lihong, Wu Qingfeng, Li Zhaohui, Zhang Weibin, Yin Ke
School of Physics and Optoelectronic Engineering, Yangtze University 1 Nanhuan Road Jingzhou Hubei 434023 China
Department of Geosciences, University of Wisconsin-Parkside 900 Wood Road Kenosha WI 53144 USA
RSC Adv. 2020 May 4;10(29):17228-17234. doi: 10.1039/d0ra02019b. eCollection 2020 Apr 29.
Understanding the effects of natural solid particles on the phototransformation of pharmaceuticals in aqueous environments is very important, but studies on this are still limited. In this study, natural sands were selected as a solid particle model due to their wide distribution in surface waters during the rainy season, and the phototransformation of diphenhydramine (DP) in the presence of the sands was investigated. The kinetic studies showed that the natural sands exhibited significant photocatalytic activity for the DP photodegradation, and the activity varied depending on their sources. Scavenging experiments and electron paramagnetic resonance analysis demonstrated that O ˙ and ˙OH were produced in the irradiated natural sand systems, and O ˙ played a more important role than ˙OH in the photodegradation of DP. The results obtained from HO treatment and deoxygenation experiments verified that the generation of radicals was mainly attributed to the low content of natural organic matter (NOM) in the sands. The possible reaction mechanism was that the NOM in the sands was excited and became triplet-state NOM after irradiation, and then induced the generation of free radicals through an electron transfer mechanism, resulting in DP oxidation. This work indicated that natural sand particles were a key factor affecting the phototransformation of drugs, and should be considered in evaluating their fate in natural waters.
了解天然固体颗粒对水环境中药物光转化的影响非常重要,但对此的研究仍然有限。在本研究中,由于天然砂在雨季地表水广泛分布,因此选择其作为固体颗粒模型,研究了在砂存在下苯海拉明(DP)的光转化。动力学研究表明,天然砂对DP光降解表现出显著的光催化活性,且活性因来源而异。清除实验和电子顺磁共振分析表明,在辐照的天然砂体系中产生了O˙和˙OH,且O˙在DP光降解中比˙OH起更重要的作用。从HO处理和脱氧实验获得的结果证实,自由基的产生主要归因于砂中天然有机物(NOM)含量低。可能的反应机制是,砂中的NOM在辐照后被激发并变成三重态NOM,然后通过电子转移机制诱导自由基的产生,导致DP氧化。这项工作表明,天然砂颗粒是影响药物光转化的关键因素,在评估其在天然水体中的归宿时应予以考虑。