| 官能化锆基金属有机骨架材料去除水体中四环素性能 |
| Functionalized zirconium metal-organic frameworks for the removal of tetracycline from water |
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| 摘要: 本研究通过预修饰和后修饰2种策略分别合成了官能化锆基金属有机骨架(MOF)材料UiO-66-CHO和UiO-66-CH=C (CN)2，用于去除水中的四环素(TC)。采用粉末X射线衍射、FTIR、1H NMR、热重分析、扫描电子显微镜和N2吸附-脱附等测试手段对合成的MOFs进行了表征。UiO-66-CHO较UiO-66-CH=C (CN)2比表面积大，吸附性能更好。实验数据证实，2种MOFs对TC的吸附符合准二级动力学和Langmuir等温线模型，是单层的化学吸附。在pH=9.0时，UiO-66-CHO和UiO-66-CH=C (CN)2的理论最大吸附量分别为199.28和62.61 mg·g-1，平衡时间为150 min。热力学分析表明，UiO-66-CHO吸附TC是一个自发的吸热过程。UiO-66-CHO在重复5次循环吸附后，对TC去除率仍达75%以上。 |
| 关键词: 四环素 金属有机骨架 UiO-66-CHO 氰基 吸附 |
| 基金项目: 国家自然科学基金青年项目(No.21701137);山西省基础计划青年科学研究项目(No.202303021212297)和忻州市科技局基础研究项目(No.20230510)资助。 |
| Abstract: In this study, UiO-66-CHO and UiO-66-CH=C(CN)2 were synthesized using pre-synthetic and postsynthetic modification methods, for the adsorption of tetracycline (TC) from aqueous solution. The powder X-ray diffraction patterns of these functional MOFs exhibit that they have the same frameworks with UiO-66 and good crystallinity. FTIR and 1H NMR spectroscopy powerfully suggested that the formyl and the cyano were successfully introduced to the frameworks. Compared to UiO-66, UiO-66-CHO and UiO-66-CH=C(CN)2 exhibit slightly diminished thermal stability in the thermogravimetric analysis and the absence of organic linkers. The Brunauer-Emmett-Teller (BET) specific surface area calculated from the N2 adsorption and desorption experiment data shows that all modified materials also preserve porousness. The three materials in the scanning electron microscope showed similar morphology at the microscopic level, and uniform particle size may be favorable for TC adsorption. A series of experiments were conducted on UiO-66-CHO and UiO-66-CH=C(CN)2 for the adsorption of TC in water. For the two functional MOFs, adsorption experiment data confirmed that the adsorption occurs via chemisorption on a monolayer, aligning with the pseudo-second-order kinetic and Langmuir isotherm models. UiO-66-CHO and UiO-66-CH=C (CN)2 exhibited a higher theoretical maximum adsorption capacity of 199.28 and 62.61 mg·g-1 at pH 9.0 than UiO-66 and shorter adsorption equilibrium time of about 150 min. Thermodynamic experiments have shown that the uptake of TC is both endothermic and spontaneous, leading to an increased disorder at the solid-solution interface. It is worth noting that UiO-66-CHO could preserve the 75% removal efficiency in the fifth adsorption cycle. |
| Keywords: tetracycline metal-organic frameworks UiO-66-CHO cyano adsorption |
| 投稿时间：2024-07-31 修订日期：2024-12-20 |
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| 席福贵,李都,闫周瑞,王慧,相俊宇,董智云.官能化锆基金属有机骨架材料去除水体中四环素性能[J].无机化学学报,2025,41(4):683-694. |
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