Eshghi Fazlolah, Mehrabadi Zohreh, Farsadrooh Majid, Hayati Payam, Javadian Hamedreza, Karimi Mehdi, Karimi-Maleh Hassan, Rostamnia Sadegh, Karaman Ceren, Aghababaei Fatemeh
Department of Chemistry, College of Sciences, Shiraz University, Shiraz, Iran.
Department of Chemistry, Firoozabad Branch, Islamic Azad University, Firoozabad, Iran.
Environ Res. 2023 Apr 1;222:115321. doi: 10.1016/j.envres.2023.115321. Epub 2023 Jan 22.
The first ultrasonic synthesis of [Cu(L)(SCN)] (L = 1-methylimidazole) nanocomplex was carried out under ultrasonic irradiation, and its photocatalytic performance for the degradation of remdesivir (RS) under sunlight irradiation was comprehensively investigated for the first time in this study. The physicochemical properties of the synthesized photocatalyst were examined by Fourier-transform infrared (FT-IR), field emission scanning electron microscopy (FE-SEM), diffuse reflectance spectroscopy (DRS), and thermogravimetric analysis (TGA) techniques. The band gap of the synthesized [Cu(L)(SCN)] nanocomplex was determined to be 2.60 eV by the diffuse reflectance spectroscopy method using Kubelka-Munk formula. The photocatalytic performance of nanocomplex was examined for the removal of remdesivir under sunlight from water for which the results indicated that an amount of 0.5 gL of the [Cu(L)(SCN)] nanocomplex was sufficient to remove more than 96% remdesivir from its 2 mg L concentration within 20 min, at pH = 6. The kinetic data showed that the photodegradation onto the [Cu(L)(SCN)] nanocomplex has a high correlation (0.98) with the pseudo-second-order kinetic model. The decrease in chemical oxygen demand (COD) (from 70.5 mg L to 36.4 mg L) under optimal conditions clearly confirmed the mineralization of the RS drug. The values of ΔS° (-0.131 kJ mol K) and ΔH° (-49.750 kJ mol) were negative, indicating that the adsorption process was spontaneous and more favorable in lower temperatures. Moreover, the RS structure in the open shell state and the high HOMO and LUMO gaps based on the M06/6-31 + G (d) level of theory may be a confirmation of this fact. In addition, the Hirshfeld surface analysis (HSA) of the crystal packing of the prepared complex was discussed in detail to evaluate the interactions between the crystal packings. The results of this study confirm that the [Cu(L)(SCN)] nanocomplex can be successfully used for the photodegradation of pharmaceutical contaminants.
首次在超声辐照下进行了[Cu(L)(SCN)]（L = 1-甲基咪唑）纳米复合物的超声合成，并在本研究中首次全面研究了其在阳光照射下对瑞德西韦（RS）降解的光催化性能。通过傅里叶变换红外光谱（FT-IR）、场发射扫描电子显微镜（FE-SEM）、漫反射光谱（DRS）和热重分析（TGA）技术对合成的光催化剂的物理化学性质进行了研究。使用Kubelka-Munk公式通过漫反射光谱法测定合成的[Cu(L)(SCN)]纳米复合物的带隙为2.60 eV。研究了纳米复合物在阳光下从水中去除瑞德西韦的光催化性能，结果表明，在pH = 6时，0.5 g/L的[Cu(L)(SCN)]纳米复合物足以在20分钟内从2 mg/L浓度的溶液中去除超过96%的瑞德西韦。动力学数据表明，[Cu(L)(SCN)]纳米复合物上的光降解与准二级动力学模型具有高度相关性（0.98）。最佳条件下化学需氧量（COD）的降低（从70.5 mg/L降至36.4 mg/L）清楚地证实了RS药物的矿化。ΔS°（-0.131 kJ mol K）和ΔH°（-49.750 kJ mol）的值为负，表明吸附过程是自发的，并且在较低温度下更有利。此外，基于M06/6-31 + G(d)理论水平的开壳态RS结构以及较高的HOMO和LUMO间隙可能证实了这一事实。此外，详细讨论了制备的复合物晶体堆积的Hirshfeld表面分析（HSA），以评估晶体堆积之间的相互作用。本研究结果证实，[Cu(L)(SCN)]纳米复合物可成功用于光降解药物污染物。
