Efficient charge transfer in aluminum-cobalt layered double hydroxide derived from Co-ZIF for enhanced catalytic degradation of tetracycline through peroxymonosulfate activation
“…Owing to the extremely high antimicrobial activity of tetracycline (TC) against multifarious types of bacterial infections, it assorted as the second most used antibiotic ( Cao et al, 2020 ). Furthermore, TC is excessively utilized as a food additive to enhance the animals growing rate since it is a cheap medicine and widely produced ( Xiong et al, 2018 ).…”
Section: Antibiotics Removal By Chitosan Composites-based Adsorbentsmentioning
“…Owing to the extremely high antimicrobial activity of tetracycline (TC) against multifarious types of bacterial infections, it assorted as the second most used antibiotic ( Cao et al, 2020 ). Furthermore, TC is excessively utilized as a food additive to enhance the animals growing rate since it is a cheap medicine and widely produced ( Xiong et al, 2018 ).…”
Section: Antibiotics Removal By Chitosan Composites-based Adsorbentsmentioning
“…The results contradict the commonly accepted mechanism that LCo II -OOSO 3aq decomposes intra-molecularly to form LCo III -OH aq + SO 4 * À . [3,4,[8][9][10][11]13,18] The linear dependence of the second and third reactions observed on [HSO 5 À ] points out that more HSO 5…”
Section: Kinetics At [Hso 5 à ] > [Co II L Aq ]mentioning
confidence: 99%
“…The suggested role of the transition metal is to form SO 4 *À radical anions that are the active oxidizing species formed in the system. Commonly it is assumed that the first reaction occurring is reaction (1): [3,4,[8][9][10][11]13,18] Reaction ð1Þ :…”
Advanced oxidation technologies often use peroxymonosulfate in the presence of Co II aq . It is commonly assumed that the reaction of Co(H 2 O) 6 2 + with HSO 5 À yields Co III aq and SO 4 *À . DFT results point out that first Co II (SO 5 )(H 2 O) 2 is formed. The homolysis of Co II (SO 5 )(H 2 O) 2 to yield (H 2 O)Co II (SO 5 )OH * + SO 4 * À , is exothermic but has a large activation energy. However the cobalt is not oxidized in this reaction. Co II (SO 5 )(H 2 O) 2 reacts with a second HSO 5 À to form Co II (SO 5 ) 2 (H 2 O) 2À that decomposes via disproportionation of the monoperoxysulfate ions without oxidation of the central cobalt ion. Surprisingly even in the presence of ligands, L, that stabilize Co III , i. e., pyrophosphate;tri-polyphosphate and ATP, the experimentally observed reaction mechanism involves the formation of LCo II -OOSO 3aq which then reacts with another HSO 5À to form LCo II -(OOSO 3 2À ) 2 . The latter complex decomposes via disproportionation of the monoperoxysulfate ligands followed by oxidation of the central cobalt cation. Alternatively, in the presence of excess Co II L aq , LCo II -OOSO 3aq reacts with Co II L aq to form 2Co III L aq . These results point out that the mechanism of advanced oxidation processes initiated by a mixture of Co(H 2 O) 6 2 + and HSO 5 À must be reconsidered.
“…As a typical anion layer material, Layered double hydroxides (LDHs) are often referred to as hydrotalcite-like compounds, consisting of a body laminate with metal hydroxide and an interlayer region containing compensating anions and solvated molecules (Daud et al 2016). At present, transition metal-based Layered double hydroxides (LDHs) were widely used for PMS activation because of their unique structure and relatively simple synthesis method (Chen et al 2019;Cao et al 2020a). Generally, LDH was mainly prepared by hydrothermal method (Huang et al 2021), precipitation method (Xiao et al 2019) and other traditional methods, but the specific surface area, morphology and structure of the LDH samples obtained by these methods are difficult to accurately control.…”
Metal-organic frameworks (MOFs) have unique properties and stable structures, which have been widely used as templates/precursors to prepare well developed pore structure and high specific surface area materials. In this article, an innovative and facile method of crystal reorganization was designed by using MOFs as sacrificial templates to prepare a layered double hydroxide (LDH) nano-layer sheet structure through a pseudomorphic conversion process under alkaline conditions. The obtained CoMn-LDH and CoFe-LDH catalysts broke the ligand of MOFs and reorganized the structure on the basis of retaining a high specific surface area and a large number of pores, which had higher specific surface area and well developed pore structure compared with LDH catalysts prepared by traditional methods, and thus provide more active sites to activate peroxymonosulfate (PMS). Due to the unique framework structure of MOFs, the MOF-derived CoMn-LDH and CoFe-LDH catalysts could provide more active sites to activate PMS, and achieve a 2,4-dichlorophenol degradation of 99.3% and 99.2% within 20 minutes, respectively. In addition the two LDH catalysts displayed excellent degradation performance for bisphenol A, ciprofloxacin and 2,4-dichlorophenoxyacetic acid (2,4-D). X-ray photoelectron spectroscopy indicated that the valence state transformation of metal elements participated in PMS activation. Electron paramagnetic resonance manifested that sulfate radical () and singlet oxygen (1O2) were the main species for degrading pollutants. In addition, after the three-cycle experiment, the CoMn-LDH and CoFe-LDH catalysts also showed long-term stability with a slight activity decrease in the third cycle. The phytotoxicity assessment determined by the germination of mung beans proved that PMS activation by MOF-derived LDH catalysts can basically eliminate the phytotoxicity of a 2,4-D solution. This research not only developed high-activity LDH catalysts for PMS activation, but also expanded the environmental applications of MOF derivants.
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