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Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols.
Chemosphere. 2020 Oct; 256:127104.C

Abstract

Iron(III)-tetraamidomacrocyclic ligand (FeIII-TAML) activators have drawn great attentions due to the high reactivity to degrade organic pollutants. However, previous studies showed that the reactivity and stability of FeIII-TAML were both strongly pH-dependent, which dramatically decrease at lower pH levels. Herein, FeIII-TAML/DODMA (dimethyldioctadecylammonium chloride) microspheres with diameters ranging from 100 to 2000 nm were synthesized via a surfactant-assisted self-assembly technique. The newly synthesized FeIII-TAML/DODMA composite exhibits superior reactivity compared to free FeIII-TAML as indicated by the degradation of bisphenols (i.e., bisphenol A and its analogues) over a wide pH range (i.e., pH 4.5-10.0). Based on the adsorption results and quantitative structure-activity relationship (QSAR) models, the enhanced reactivity of FeIII-TAML/DODMA is mainly ascribed to the hydrophobic sorption of bisphenols. Moreover, the enhanced ionization of the axial water molecule associated with FeIII-TAML could further enhance the reactivity of synthesized microcomposites, which was confirmed by the results of infrared and Raman spectra. Furthermore, FeIII-TAML/DODMA shows distinct acid-resistance as explained by the protection of the hydrophobic alkyl chains of DODMA. This novel method would provide a simple and effective strategy to expand the application of FeIII-TAML in a wide pH range and render FeIII-TAML/DODMA microstructure as a potential catalyst for treatment of bisphenol compounds.

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Publisher Full Text (DOI)

Authors+Show Affiliations

Wang C
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, PR China.
Xian Z
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, PR China.
Ding Y
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, PR China.
Jin X
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, PR China; Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, 210008, PR China.
Gu C
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, PR China. Electronic address: chenggu@nju.edu.cn.

MeSH

Benzhydryl CompoundsCatalysisFerric CompoundsHydrogen PeroxideIronLigandsModels, ChemicalOxidation-ReductionPhenols

Pub Type(s)

Journal Article

Language

eng

PubMed ID

32470734

Citation

Wang, Chao, et al. "Self-assembly of FeIII-TAML-based Microstructures for Rapid Degradation of Bisphenols." Chemosphere, vol. 256, 2020, p. 127104.
Wang C, Xian Z, Ding Y, et al. Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols. Chemosphere. 2020;256:127104.
Wang, C., Xian, Z., Ding, Y., Jin, X., & Gu, C. (2020). Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols. Chemosphere, 256, 127104. https://doi.org/10.1016/j.chemosphere.2020.127104
Wang C, et al. Self-assembly of FeIII-TAML-based Microstructures for Rapid Degradation of Bisphenols. Chemosphere. 2020;256:127104. PubMed PMID: 32470734.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols. AU - Wang,Chao, AU - Xian,Zeyu, AU - Ding,Yunhao, AU - Jin,Xin, AU - Gu,Cheng, Y1 - 2020/05/24/ PY - 2020/01/13/received PY - 2020/05/14/revised PY - 2020/05/15/accepted PY - 2020/5/30/pubmed PY - 2020/7/24/medline PY - 2020/5/30/entrez KW - Bisphenols KW - Catalytic oxidation KW - Iron(III)-Tetraamidomacrocyclic ligand activator KW - Ordered microspheres KW - Surfactant-assisted self-assembly SP - 127104 EP - 127104 JF - Chemosphere JO - Chemosphere VL - 256 N2 - Iron(III)-tetraamidomacrocyclic ligand (FeIII-TAML) activators have drawn great attentions due to the high reactivity to degrade organic pollutants. However, previous studies showed that the reactivity and stability of FeIII-TAML were both strongly pH-dependent, which dramatically decrease at lower pH levels. Herein, FeIII-TAML/DODMA (dimethyldioctadecylammonium chloride) microspheres with diameters ranging from 100 to 2000 nm were synthesized via a surfactant-assisted self-assembly technique. The newly synthesized FeIII-TAML/DODMA composite exhibits superior reactivity compared to free FeIII-TAML as indicated by the degradation of bisphenols (i.e., bisphenol A and its analogues) over a wide pH range (i.e., pH 4.5-10.0). Based on the adsorption results and quantitative structure-activity relationship (QSAR) models, the enhanced reactivity of FeIII-TAML/DODMA is mainly ascribed to the hydrophobic sorption of bisphenols. Moreover, the enhanced ionization of the axial water molecule associated with FeIII-TAML could further enhance the reactivity of synthesized microcomposites, which was confirmed by the results of infrared and Raman spectra. Furthermore, FeIII-TAML/DODMA shows distinct acid-resistance as explained by the protection of the hydrophobic alkyl chains of DODMA. This novel method would provide a simple and effective strategy to expand the application of FeIII-TAML in a wide pH range and render FeIII-TAML/DODMA microstructure as a potential catalyst for treatment of bisphenol compounds. SN - 1879-1298 UR - https://www.unboundmedicine.com/medline/citation/32470734/Self_assembly_of_FeIII_TAML_based_microstructures_for_rapid_degradation_of_bisphenols_ DB - PRIME DP - Unbound Medicine ER -