Sun Xun, Chen Mingming, Lei Jiayu, Liu Xinran, Ke Xin, Liu Wengang, Wang Jingkuan, Gao Xiaodan, Liu Xin, Zhang Yun
Liaoning Key Laboratory of Clean Energy and College of Energy and Environmental, Shenyang Aerospace University, Shenyang, China.
School of Resources and Civil Engineering, Northeastern University, Shenyang, China.
Front Chem. 2022 Dec 13;10:1040435. doi: 10.3389/fchem.2022.1040435. eCollection 2022.
In this study, β-CD@mesoporous SiO nanospheres (β-CD@mSi) were prepared by loading β-cyclodextrin (β-CD) onto mesoporous silica nanospheres through an synthesis. This not only solved the defect of β-CD being easily soluble in water, but also changed the physical structure of the mesoporous silica nanospheres. FTIR and XPS results showed that β-CD was successfully loaded onto mesoporous silica nanospheres (mSi), while enhancing the adsorption effect. β-CD@mSi with a monomer diameter of about 150 nm were prepared. At a temperature of 298k, the removal efficiency of a 100 mg/L solution of rifampicin can reach 90% in 4 h and the adsorption capacity was 275.42 mg g at high concentration. Through the calculation and analysis of adsorption kinetics, adsorption isotherms and adsorption thermodynamics based on the experimental data, the reaction is a spontaneous endothermic reaction dominated by chemical adsorption. The electron transfer pathway, structure-activity relationship and energy between β-CD@mSi and rifampicin were investigated by quantum chemical calculations. The accuracy of the characterization test results to judge the adsorption mechanism was verified, to show the process of rifampicin removal by β-CD@mSi more clearly and convincingly. The simulation results show that π-π interaction plays a major interaction in the reaction process, followed by intermolecular hydrogen bonding and electrostatic interactions.
在本研究中，通过合成法将β-环糊精（β-CD）负载到介孔二氧化硅纳米球上制备了β-CD@介孔SiO纳米球（β-CD@mSi）。这不仅解决了β-CD易溶于水的缺陷，还改变了介孔二氧化硅纳米球的物理结构。傅里叶变换红外光谱（FTIR）和X射线光电子能谱（XPS）结果表明，β-CD成功负载到介孔二氧化硅纳米球（mSi）上，同时增强了吸附效果。制备了单体直径约为150nm的β-CD@mSi。在298K温度下，100mg/L利福平溶液在4小时内的去除效率可达90%，高浓度下吸附容量为275.42mg/g。通过基于实验数据的吸附动力学、吸附等温线和吸附热力学的计算与分析，该反应是一个以化学吸附为主的自发吸热反应。通过量子化学计算研究了β-CD@mSi与利福平之间的电子转移途径、构效关系和能量。验证了表征测试结果判断吸附机理的准确性，更清晰、更有说服力地展示了β-CD@mSi去除利福平的过程。模拟结果表明，π-π相互作用在反应过程中起主要作用，其次是分子间氢键和静电相互作用。
