Saghir Summaira, Wang Yongqiang, Xiao Zhenggang
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, 200 Xiaolingwei Street, Nanjing, 210094, People's Republic of China.
J Clean Prod. 2023 Aug 15;414:137654. doi: 10.1016/j.jclepro.2023.137654. Epub 2023 May 30.
The current outbreak of the coronavirus (COVID-19) pandemic has significantly increased the global usage of antiviral drugs (AVDs), leading to higher concentrations of antibiotics in water pollution. To address this current issue, a new kind of adsorbent named isostructural zeolitic tetrazolate imidazolate frameworks (ZTIFs) were synthesized by combining imidazole and tetrazolates into one self-assembly approach by adjusting pores and stability of frameworks. The incorporation of imidazole ligand progressively increased the stability of frameworks. Furthermore, increasing the content of tetrazolate ligand greatly improved the adsorption performance due to N-rich sites by increasing the pore size. The obtained adsorbent composite exhibits macroporous structure up to 53.05 nm with excellent structural stability. Owing to their macropores and highly exposed active sites, the synthesized ZTIFs exhibit the maximum adsorption capacity for oseltamivir (OT) and ritonavir (RT) of 585.2 mg/g and 435.8 mg/g, respectively. Moreover, the adsorption uptake and saturation process were rapid compared to simple MOF. Within 20 min, both pollutants achieved equilibrium. The adsorption isotherms were best interpreted by Pseudo second order kinetics. The adsorption of AVDs on ZTIFs was spontaneous, exothermic, and thermodynamically feasible. The DFT calculations and characterization results after adsorption demonstrate that π-π interaction, pore filling, surface complexation, and electrostatic interaction were the primary features of the adsorption mechanism. The prepared ZTIFs composite exhibits high chemical, mechanical and thermal stability and can be recycled multiple times without destroying its morphology and structure. The adsorbent regeneration for several cycles impacted the operational cost and the eco-friendly characteristic of the process.
当前冠状病毒（COVID-19）大流行的爆发显著增加了抗病毒药物（AVD）在全球的使用量，导致水污染中抗生素浓度升高。为解决这一当前问题，通过将咪唑和四唑酸盐以一种自组装方法结合起来，通过调节骨架的孔隙率和稳定性，合成了一种名为同构沸石四唑酸盐咪唑酸盐骨架（ZTIFs）的新型吸附剂。咪唑配体的引入逐渐提高了骨架的稳定性。此外，增加四唑酸盐配体的含量通过增加孔径极大地改善了由于富含氮的位点而产生的吸附性能。所获得的吸附剂复合材料呈现出高达53.05 nm的大孔结构，具有优异的结构稳定性。由于其大孔和高度暴露的活性位点，合成的ZTIFs对奥司他韦（OT）和利托那韦（RT）的最大吸附容量分别为585.2 mg/g和435.8 mg/g。此外，与简单的金属有机框架（MOF）相比，吸附摄取和饱和过程很快。在20分钟内，两种污染物都达到了平衡。吸附等温线用伪二级动力学能得到最好的解释。AVD在ZTIFs上的吸附是自发的、放热的，并且在热力学上是可行的。吸附后的密度泛函理论（DFT）计算和表征结果表明，π-π相互作用、孔填充、表面络合和静电相互作用是吸附机制的主要特征。制备的ZTIFs复合材料表现出高化学、机械和热稳定性，并且可以多次循环使用而不破坏其形态和结构。吸附剂的多次循环再生影响了运行成本和该过程的生态友好特性。
