{"title":"Adsorption behavior and mechanism of NH2-MIL-101(Cr)@COFs@SA composite adsorbent for tetracycline removal","authors":"","doi":"10.1016/j.polymer.2024.127631","DOIUrl":null,"url":null,"abstract":"<div><p>Herein, we employed a rational approach to develop a hydrogel composite material by encapsulating NH<sub>2</sub>-MIL-101(Cr)/covalent organic frameworks (COFs) in sodium alginate (SA) to effectively capture of tetracycline (TC). Experimental tests and various characterizations (including Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron spectroscopy (SEM), Brunauer-Emmett-Teller (BET), and X-ray photoelectron spectroscopy (XPS)) confirmed that the NH<sub>2</sub>-MIL-101(Cr)@COFs@SA composite exhibited a more robust, multilayer pore structure with abundant active functional groups. Under conditions of 298 K and pH = 7, the NH<sub>2</sub>-MIL-101(Cr)@COFs@SA adsorbent demonstrated remarkable TC adsorption capability, achieving a removal rate of 96.38 % in 120 min and a q<sub>max</sub> of 252.6 mg/g at 298 K by Langmuir model. Kinetic analysis indicated that the interaction between TC and NH<sub>2</sub>-MIL-101(Cr)@COFs@SA follows a pseudo-second-order model, suggesting that chemisoption governs the process. The Langmuir model and thermodynamic analysis suggested that TC adsorption follows a monolayer sorption pattern and is spontaneous and exothermic. Even in the presence of other ions, NH<sub>2</sub>-MIL-101(Cr)@COFs@SA maintained high efficiency for TC adsorption, demonstrating superior selectivity. NH<sub>2</sub>-MIL-101(Cr)@COFs@SA demonstrated remarkable recyclability, with only a minimal reduction in the removal efficiency (85.5 % and 142 mg/g) after 10 cycles of adsorption and regeneration. Various analytical techniques, including FTIR spectroscopy, SEM, EDX, XPS, and density functional theory (DFT) calculations of adsorption energy were used to elucidate the TC adsorption mechanisms by NH<sub>2</sub>-MIL-101(Cr)@COFs@SA. The adsorption process primarily involved π-π stacking, hydrogen bonding, electrostatic interactions, and complexation.</p></div>","PeriodicalId":405,"journal":{"name":"Polymer","volume":null,"pages":null},"PeriodicalIF":4.1000,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Polymer","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0032386124009674","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
引用次数: 0
Abstract
Herein, we employed a rational approach to develop a hydrogel composite material by encapsulating NH2-MIL-101(Cr)/covalent organic frameworks (COFs) in sodium alginate (SA) to effectively capture of tetracycline (TC). Experimental tests and various characterizations (including Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron spectroscopy (SEM), Brunauer-Emmett-Teller (BET), and X-ray photoelectron spectroscopy (XPS)) confirmed that the NH2-MIL-101(Cr)@COFs@SA composite exhibited a more robust, multilayer pore structure with abundant active functional groups. Under conditions of 298 K and pH = 7, the NH2-MIL-101(Cr)@COFs@SA adsorbent demonstrated remarkable TC adsorption capability, achieving a removal rate of 96.38 % in 120 min and a qmax of 252.6 mg/g at 298 K by Langmuir model. Kinetic analysis indicated that the interaction between TC and NH2-MIL-101(Cr)@COFs@SA follows a pseudo-second-order model, suggesting that chemisoption governs the process. The Langmuir model and thermodynamic analysis suggested that TC adsorption follows a monolayer sorption pattern and is spontaneous and exothermic. Even in the presence of other ions, NH2-MIL-101(Cr)@COFs@SA maintained high efficiency for TC adsorption, demonstrating superior selectivity. NH2-MIL-101(Cr)@COFs@SA demonstrated remarkable recyclability, with only a minimal reduction in the removal efficiency (85.5 % and 142 mg/g) after 10 cycles of adsorption and regeneration. Various analytical techniques, including FTIR spectroscopy, SEM, EDX, XPS, and density functional theory (DFT) calculations of adsorption energy were used to elucidate the TC adsorption mechanisms by NH2-MIL-101(Cr)@COFs@SA. The adsorption process primarily involved π-π stacking, hydrogen bonding, electrostatic interactions, and complexation.
期刊介绍:
Polymer is an interdisciplinary journal dedicated to publishing innovative and significant advances in Polymer Physics, Chemistry and Technology. We welcome submissions on polymer hybrids, nanocomposites, characterisation and self-assembly. Polymer also publishes work on the technological application of polymers in energy and optoelectronics.
The main scope is covered but not limited to the following core areas:
Polymer Materials
Nanocomposites and hybrid nanomaterials
Polymer blends, films, fibres, networks and porous materials
Physical Characterization
Characterisation, modelling and simulation* of molecular and materials properties in bulk, solution, and thin films
Polymer Engineering
Advanced multiscale processing methods
Polymer Synthesis, Modification and Self-assembly
Including designer polymer architectures, mechanisms and kinetics, and supramolecular polymerization
Technological Applications
Polymers for energy generation and storage
Polymer membranes for separation technology
Polymers for opto- and microelectronics.