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      Photocatalytic Degradation of Tetracycline by a Novel (CMC)/MIL-101(Fe)/β-CDP Composite Hydrogel

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          Abstract

          Herein, we report a novel carboxymethyl cellulose (CMC)/MIL-101 (Fe)/poly(β-cyclodextrin) (β-CDP) hydrogel with high photocatalytic activity. β-CDP can significantly enhance the photoactivity of MIL-101(Fe) in the hydrogel prepared by a simple solvothermal method. The structure and property of this composite hydrogel were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Tetracycline was selected as a model pharmaceutical antibiotic to evaluate the photocatalytic activity of the composite hydrogel under visible light irradiation and darkness, respectively. This composite hydrogel shows excellent activity for degrading pharmaceutical antibiotics under visible light irradiation. The increased photocatalytic activity can be attributed to β-CDP, which acts as a promoter and affords an efficient separation of photogenerated electron-hole pairs of MIL-101(Fe). Moreover, the composite hydrogel is shown to have good water retainability. The hydrogel is inexpensive and shows high photocatalytic activity. Hence, it can be used as an efficient photocatalytic material.

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          Most cited references 26

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          Ultrahigh porosity in metal-organic frameworks.

          Crystalline solids with extended non-interpenetrating three-dimensional crystal structures were synthesized that support well-defined pores with internal diameters of up to 48 angstroms. The Zn4O(CO2)6 unit was joined with either one or two kinds of organic link, 4,4',4''-[benzene-1,3,5-triyl-tris(ethyne-2,1-diyl)]tribenzoate (BTE), 4,4',44''-[benzene-1,3,5-triyl-tris(benzene-4,1-diyl)]tribenzoate (BBC), 4,4',44''-benzene-1,3,5-triyl-tribenzoate (BTB)/2,6-naphthalenedicarboxylate (NDC), and BTE/biphenyl-4,4'-dicarboxylate (BPDC), to give four metal-organic frameworks (MOFs), MOF-180, -200, -205, and -210, respectively. Members of this series of MOFs show exceptional porosities and gas (hydrogen, methane, and carbon dioxide) uptake capacities. For example, MOF-210 has Brunauer-Emmett-Teller and Langmuir surface areas of 6240 and 10,400 square meters per gram, respectively, and a total carbon dioxide storage capacity of 2870 milligrams per gram. The volume-specific internal surface area of MOF-210 (2060 square meters per cubic centimeter) is equivalent to the outer surface of nanoparticles (3-nanometer cubes) and near the ultimate adsorption limit for solid materials.
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            Visible-Light Photoredox Catalysis

            In the last few years, visible-light initiated organic transformations have attracted increasing attention. The development of visible-light-promoted photocatalytic reactions, which enable rapid and efficient synthesis of fine chemicals, is highly desirable from the viewpoint of cost, safety, availability, and environmental friendliness. In this Minireview, recent advances made in this fast developing area of research are discussed.
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              Ultimate biodegradation and elimination of antibiotics in inherent tests.

              The biodegradation and elimination of antibiotics in municipal wastewater treatment plants is of particular concern because sewage is the main exposure route for antibiotics used in human medicine. The inherent biodegradability of 17 antibiotics was determined in a combined test design based on the Zahn-Wellens test (OECD 302 B, 1992) and the CO2-evolution test (OECD 301 B, 1992). CO2 Evolution test (Modified Sturm test). OECD Guideline for the Testing of Chemicals, Paris). Only benzylpenicillin sodium salt (Penicillin G) proved to be ultimately biodegradable, reaching ThCO2 degradation extents of 78-87%. Among the others, only amoxicillin, imipenem and nystatin showed certain ultimate biodegradation in few of the parallel flasks and can be regarded as partially biodegradable with formation of stable metabolites. The DOC-elimination of tetracycline-HCl showed a typical degradation curve starting with 18% and reaching the plateau phase at 80% after 21 days. Nevertheless, the CO2-evolution measured in parallel did not support the data, indicating that the time needed for reaching the adsorption equilibrium was underestimated. Several other antibiotics showed considerable DOC-elimination in the inherent test while only minor incidences of ultimate biodegradation were observed. The combination of CO2-evolution and DOC-elimination is a suitable instrument for assessing the behaviour of chemicals within one test. It enables one to assess both inherent ultimate biodegradability and DOC-elimination by sorption. The applicability of the test is limited to substances with a moderate toxicity.
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                Author and article information

                Contributors
                Journal
                Front Chem
                Front Chem
                Front. Chem.
                Frontiers in Chemistry
                Frontiers Media S.A.
                2296-2646
                12 January 2021
                2020
                : 8
                Affiliations
                School of Forestry and Landscape Architecture, Anhui Agricultural University , Hefei, China
                Author notes

                Edited by: Yinan Wu, Tongji University, China

                Reviewed by: Khaled Mohammad Saoud, Virginia Commonwealth University School of the Arts, Qatar; Cheng-an Tao, National University of Defense Technology, China

                *Correspondence: Shengquan Liu liusq@ 123456ahau.edu.cn

                This article was submitted to Nanoscience, a section of the journal Frontiers in Chemistry

                †These authors have contributed equally to this work

                Article
                10.3389/fchem.2020.593730
                7845018
                33520930
                Copyright © 2021 Zhang, Zhou, Li, Rong, Jiang and Liu.

                This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.

                Page count
                Figures: 9, Tables: 0, Equations: 0, References: 26, Pages: 8, Words: 4015
                Categories
                Chemistry
                Original Research

                photo-catalytic, mil-101(fe), β-cdp, tetracycline, hydrogel

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