用于去除水中妥布霉素和氧氟沙星的羧基官能化共价有机聚合物,ACS Applied Nano Materials

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用于去除水中妥布霉素和氧氟沙星的羧基官能化共价有机聚合物
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-12-19 , DOI: 10.1021/acsanm.3c04905
Hengqiang Zhao _{1,

2} , Ran Miao ₁ , Lidan Zhang ₁ , Rongyu Wang ₁ , Wenhua Ji _{1,

2} , Xiaobei Ning _{1,

2} , Yingchao Lv _{1,

2} , Shaojun Zong _{1,

2} , Xiao Wang _{1,

2} , Zhaoyu Qiao ₁

Affiliation

传统污水处理方法效率低下，有效去除亲水污染物对于环境保护具有重要意义。在这项工作中，使用2,2',2''-(苯-1,3,5-三基)三乙腈(BTNA)和2,4,6-三(4)制备了氰基-亚乙烯基连接的共价有机聚合物。 -甲酰基苯基)-1,3,5-三嗪 (TFPT) 作为 Knoevenagel 反应单体。然后将氰基水解以获得羧基官能化的共价有机聚合物(COP-COOH)。TFPT-BTAN-COP-COOH具有良好的比表面积（73.9 m ² g ^–1）和大通道（∼3.82 nm），通过多功能结合位点对妥布霉素和氧氟沙星表现出快速吸附平衡和高吸附能力。具体而言，羧基和碱性基团（例如氨基、哌嗪和二氢吡啶）之间的静电相互作用对于选择性去除妥布霉素和氧氟沙星起着关键作用。利用密度泛函理论计算出TFPT-BTAN-COP-COOH吸附妥布霉素和氧氟沙星的结合能分别为-59.83和-35.63 kcal/mol。对于其他氨基糖苷类和喹诺酮类抗生素，如恩诺沙星、诺氟沙星、新霉素、链霉素等，以TFPT-BTAN-COP-COOH为吸附剂，30 min内去除率可达95%以上。这项工作探索了一种在环境修复过程中消除亲水性有机污染物的有前景的策略。

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Carboxyl-Functionalized Covalent Organic Polymer for Removal of Tobramycin and Ofloxacin from Water

The effective removal of hydrophilic pollutants is of vital significance for environmental protection mainly because of the low efficiency of traditional sewage treatment methods. In this work, the cyano-vinylene-linked covalent organic polymer was prepared using 2,2′,2′′-(benzene-1,3,5-triyl)triacetonitrile (BTNA) and 2,4,6-tris(4-formylphenyl)-1,3,5-triazine (TFPT) as the Knoevenagel reaction monomers. The cyano group was then hydrolyzed to obtain a carboxyl-functionalized covalent organic polymer (COP-COOH). With good surface area (73.9 m² g^–1) and large channel (∼3.82 nm), TFPT-BTAN-COP-COOH showed fast adsorption equilibrium and high adsorption capacity for tobramycin and ofloxacin via multiple-functional binding sites. Specifically, the electrostatic interaction between the carboxyl group and basic groups (e.g., amino, piperazine, and dihydropyridine) plays a critical role for the selective removal of tobramycin and ofloxacin. The binding energies of TFPT-BTAN-COP-COOH adsorbed tobramycin and ofloxacin calculated using the density functional theory are −59.83 and −35.63 kcal/mol, respectively. For other aminoglycoside and quinolone antibiotics, such as enrofloxacin, norfloxacin, neomycin, and streptomycin, the removal rate can reach over 95% within 30 min using TFPT-BTAN-COP-COOH as the adsorbent. This work explored a promising strategy for the elimination of hydrophilic organic pollutants during environmental remediation.

更新日期：2023-12-19

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