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用于水中扑热息痛和四环素超吸附的高介孔碳的两步制备:孔填充和π-π相互作用的重要贡献

Two-stage preparation of highly mesoporous carbon for super-adsorption of paracetamol and tetracycline in water: Important contribution of pore filling and π-π interaction.

作者信息

Ninh Pham Thanh Trung, Ngoc Tuyen Le Thi, Dat Nguyen Duy, Nguyen My Linh, Dong Nguyen Thanh, Chao Huan-Ping, Tran Hai Nguyen

机构信息

Faculty of Chemical & Food Technology, Ho Chi Minh City University of Technology and Education, Thu Duc, Ho Chi Minh, 700000, Viet Nam.

Faculty of Chemical & Food Technology, Ho Chi Minh City University of Technology and Education, Thu Duc, Ho Chi Minh, 700000, Viet Nam.

出版信息

Environ Res. 2023 Feb 1;218:114927. doi: 10.1016/j.envres.2022.114927. Epub 2022 Nov 29.

DOI:10.1016/j.envres.2022.114927
PMID:36460071
Abstract

This study aimed to develop an extremely highly porous activated carbon derived from soybean curd residues (SCB-AC) through two-step pyrolyzing coupled with KOH activating process and then apply it for removing paracetamol (PRC) and tetracycline (TCH) from water. The optimal conditions for chemical activation were 800 °C and the ratio of KOH to material (4/1; wt./wt.). SCB-AC adsorbents (before and after adsorption) were characterized by Brunauer-Emmet-Teller (BET) analyser, Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy, and Raman spectroscopy. Adsorption kinetics, isotherm, and thermodynamics were concluded under batch experiments. The effects of pH (2-10) and NaCl (0-1 M) on adsorption processes were investigated. Reusable properties of laden SCB-AC were evaluated by studying desorption and cycles of adsorption/desorption. Results indicated that SCB-AC exhibited a large specific surface area (3306 m/g) and high total pore volume (2.307 cm/g), with mesoporous volume accounting for 86.9%. Its porosity characteristics (average pore width: 2.725 nm) are very appropriate for adsorbing two pharmaceuticals through pore-filling mechanism. Adsorption processes were less affected by the parameters: pH, NaCl, and water matrixes. The kinetics for adsorbing PRC reached a faster equilibrium than that for TCH. The Langmuir maximum adsorption capacity of SCB-AC (pH 7.0 and 25 °C) was 1235 mg/g (for adsorbing TCH) and 646 mg/g (PRC). Pore filling (confirmed by BET analyser) and π-π interaction (confirmed by FTIR and Raman spectroscopy) were dominant adsorption mechanisms. Those mechanisms were physisorption (ΔH° = 13.71 and -21.04 kJ/mol for adsorbing TCH and PRC, respectively). SCB-AC can serve as an outstanding material for removing pharmaceuticals from water.

摘要

本研究旨在通过两步热解结合KOH活化工艺,制备一种由豆腐渣残渣衍生的超高孔隙率活性炭(SCB - AC),并将其用于去除水中的对乙酰氨基酚(PRC)和四环素(TCH)。化学活化的最佳条件为800℃以及KOH与原料的比例(4/1;重量/重量)。采用布鲁诺尔-埃米特-泰勒(BET)分析仪、傅里叶变换红外光谱(FTIR)、扫描电子显微镜和拉曼光谱对SCB - AC吸附剂(吸附前后)进行表征。在间歇实验中得出吸附动力学、等温线和热力学。研究了pH值(2 - 10)和NaCl(0 - 1 M)对吸附过程的影响。通过研究解吸以及吸附/解吸循环来评估负载SCB - AC的可重复使用性能。结果表明,SCB - AC具有较大的比表面积(3306 m/g)和较高的总孔体积(2.307 cm/g),其中介孔体积占86.9%。其孔隙特征(平均孔径:2.725 nm)非常适合通过孔隙填充机制吸附两种药物。吸附过程受pH值、NaCl和水基质等参数的影响较小。吸附PRC的动力学比吸附TCH达到平衡的速度更快。SCB - AC在pH 7.0和25℃时对TCH的朗缪尔最大吸附容量为1235 mg/g,对PRC为646 mg/g。孔隙填充(由BET分析仪证实)和π-π相互作用(由FTIR和拉曼光谱证实)是主要吸附机制。这些机制均为物理吸附(吸附TCH和PRC时的ΔH°分别为13.71和 - 21.04 kJ/mol)。SCB - AC可作为从水中去除药物的优良材料。

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