| 羧基微孔有机网络材料的合成及其对水中苯并三唑类污染物的快速吸附与去除 |
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| 基金项目:国家自然科学基金资助项目（22174071） |
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| 中文摘要:以富含羧基的反应单体合成了比表面积大、溶剂和热稳定性好的羧基微孔有机网络材料MON-2COOH，开展了其用于快速吸附和去除水中苯并三唑类污染物的研究。通过固体核磁碳谱、N2吸附 - 解吸、傅里叶变换红外光谱、热重分析、扫描电镜和水接触角实验对所合成的MON-2COOH进行了表征。考察了MON-2COOH吸附1H-苯并三唑（BTri）和5-甲苯基三唑（5-TTri）的吸附等温线、吸附动力学和热力学，以及离子强度、pH值和腐殖酸等对吸附的影响。BTri和5-TTri在MON-2COOH上的吸附符合准二级和Langmuir吸附模型。MON-2COOH在10 min内即可实现对BTri和5-TTri（100 mg·L-1）的吸附平衡，最大吸附量分别为251.3、369.0 mg·g-1，优于文献报道的大多吸附剂。MON-2COOH还具有良好的可重复使用性和再生性，并成功用于实际水样中BTri和5-TTri的吸附和去除。机理研究表明π - π、疏水和氢键相互作用在吸附过程中起重要作用。该文为设计和合成高效去除苯并三唑类污染物的吸附剂提供了一种新方法，有望促进功能化MONs材料在环境污染物分析和去除中的应用。 |
| 中文关键词:微孔有机网络 ?苯并三唑 ?吸附 ?去除 ?环境污染物 |
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| Synthesis of a Carboxyl Enriched Microporous Organic Network and Its Application in Rapid Adsorption and Removal of Benzotriazoles in Water |
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| Abstract:A carboxyl enriched microporous organic network（MON-2COOH） with large surface area （720.2 m2·g-1），good solvent and thermal stability（280 ℃） was synthesized with carboxyl-contained monomers for rapid adsorption and efficient removal of benzotriazoles in water．The synthesized MON-2COOH was characterized by solid-state?13C nuclear magnetic spectroscopy，N2 adsorption - desorption，Fourier transform infrared spectroscopy，thermogravimetric analysis，scanning electronic microscopy and water contact angle analysis.The adsorption isotherms，kinetics and thermodynamics，effects of ionic strength，pH and humic acid of MON-2COOH for 1H-benzotriazole （BTri） and 5-tolyltriazole （5-TTri） were also investigatied in detail.The adsorption equilibriums of BTri and 5-TTri （100 mg·L-1） were realized within 10 min on MON-2COOH，showing the extremely fast adsorption kinetics of MON-2COOH for benzotriazoles．The pseudo-second-order kinetics plots showed good linearity for all three initial concentrations of BTri and 5-TTri，and the adsorption capacity values calculated from the pseudo-second-order model were all close to the experimental ones，both suggesting the well-fitting of pseudo-second-order kinetic model for BTri and 5-TTri on MON-2COOH．The good linearity of the Langmuir adsorption plots revealed the good plotting of Langmuir adsorption model and the monolayer adsorption process for BTri and 5-TTri on MON-2COOH．The MON-2COOH gave the large maximum adsorption capacities of 251.3 and 369.0 mg·g-1 for BTri and 5-TTri，respectively，which were larger than many reported adsorbents.The MON-2COOH gave relatively stable adsorption capacity for BTri and 5-TTri in the pH range of 2.0 - 7.0，but decreased adsorption capacity of BTri and 5-TTri from 8.0 to 11.0，which suggested the alkaline condition was unfavorable for the adsorption of BTri and 5-TTri on MON-2COOH.Moreover，the adsorption capacity of BTri and 5-TTri was independent under NaCl concentration lower than 100 mg·g-1 and humic acid concentration less than 40 mg·g-1．The MON-2COOH also owned good reusability and reproducibility．In addition，MON-2COOH was successfully applied to the adsorption and removal of BTri and 5-TTri in real lake and river water samples．The mechanisms studies revealed the important roles of π - π，hydrophobic and hydrogen bonding interaction during the adsorption．This work provided a promising way to design and synthesize efficient adsorbents for benzotriazoles，which may also promote the application of functionalized MONs in environmental contaminants analysis and elimination． |
| Key Words:microporous organic network ?benzotriazoles ?adsorption ?removal ?environmental contaminants |
| 引用本文：崔媛媛，杨成雄.羧基微孔有机网络材料的合成及其对水中苯并三唑类污染物的快速吸附与去除[J].分析测试学报,2022,41(5):692-700. |
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