Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols
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...
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description | 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.
[Display omitted]
•A SAS method is used to synthesize FeIII-TAML based microsphere.•FeIII-TAML/DODMA shows superior reactivity in degradation of bisphenols.•FeIII-TAML/DODMA exhibits higher efficiency than free FeIII-TAML over a wide pH range.•Intermolecular forces play an important role in the enhanced reactivity of FeIII-TAML/DODMA. |
doi_str_mv | 10.1016/j.chemosphere.2020.127104 |
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[Display omitted]
•A SAS method is used to synthesize FeIII-TAML based microsphere.•FeIII-TAML/DODMA shows superior reactivity in degradation of bisphenols.•FeIII-TAML/DODMA exhibits higher efficiency than free FeIII-TAML over a wide pH range.•Intermolecular forces play an important role in the enhanced reactivity of FeIII-TAML/DODMA.</description><identifier>ISSN: 0045-6535</identifier><identifier>EISSN: 1879-1298</identifier><identifier>DOI: 10.1016/j.chemosphere.2020.127104</identifier><language>eng</language><publisher>Elsevier Ltd</publisher><subject>Bisphenols ; Catalytic oxidation ; Iron(III)-Tetraamidomacrocyclic ligand activator ; Ordered microspheres ; Surfactant-assisted self-assembly</subject><ispartof>Chemosphere (Oxford), 2020-10, Vol.256, p.127104-127104, Article 127104</ispartof><rights>2020 Elsevier Ltd</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1993-7a8a21a9a5e79ac2605f36d2741e8b47c910d4415597266aa3cd04a6755a1a5e3</citedby><cites>FETCH-LOGICAL-c1993-7a8a21a9a5e79ac2605f36d2741e8b47c910d4415597266aa3cd04a6755a1a5e3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.chemosphere.2020.127104$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3548,27922,27923,45993</link.rule.ids></links><search><creatorcontrib>Wang, Chao</creatorcontrib><creatorcontrib>Xian, Zeyu</creatorcontrib><creatorcontrib>Ding, Yunhao</creatorcontrib><creatorcontrib>Jin, Xin</creatorcontrib><creatorcontrib>Gu, Cheng</creatorcontrib><title>Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols</title><title>Chemosphere (Oxford)</title><description>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.
[Display omitted]
•A SAS method is used to synthesize FeIII-TAML based microsphere.•FeIII-TAML/DODMA shows superior reactivity in degradation of bisphenols.•FeIII-TAML/DODMA exhibits higher efficiency than free FeIII-TAML over a wide pH range.•Intermolecular forces play an important role in the enhanced reactivity of FeIII-TAML/DODMA.</description><subject>Bisphenols</subject><subject>Catalytic oxidation</subject><subject>Iron(III)-Tetraamidomacrocyclic ligand activator</subject><subject>Ordered microspheres</subject><subject>Surfactant-assisted self-assembly</subject><issn>0045-6535</issn><issn>1879-1298</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqNkLFOwzAQhi0EEqXwDmFjSbEdO4nHqqJQqYiBdrau9oW6SuJgJ0i8PYnKwMh00un_ft19hNwzumCU5Y-nhTli42N3xIALTvm45wWj4oLMWFmolHFVXpIZpUKmuczkNbmJ8UTpCEs1I_t3rKsUYsTmUH8nvkrWuNls0t3ydZseIKJNGmeCj30YTD8EjEnlQxKgczax-BHAQu98O5EHN53R-jrekqsK6oh3v3NO9uun3eol3b49b1bLbWqYUllaQAmcgQKJhQLDcyqrLLe8EAzLgyiMYtQKwaRUBc9zgMxYKiAvpAQ2QtmcPJx7u-A_B4y9blw0WNfQoh-i5oKWnGZSZGNUnaPTMzFgpbvgGgjfmlE9qdQn_UelnlTqs8qRXZ1ZHH_5chh0NA5bg9YFNL223v2j5Qfh3IIw</recordid><startdate>202010</startdate><enddate>202010</enddate><creator>Wang, Chao</creator><creator>Xian, Zeyu</creator><creator>Ding, Yunhao</creator><creator>Jin, Xin</creator><creator>Gu, Cheng</creator><general>Elsevier Ltd</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>202010</creationdate><title>Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols</title><author>Wang, Chao ; Xian, Zeyu ; Ding, Yunhao ; Jin, Xin ; Gu, Cheng</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1993-7a8a21a9a5e79ac2605f36d2741e8b47c910d4415597266aa3cd04a6755a1a5e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Bisphenols</topic><topic>Catalytic oxidation</topic><topic>Iron(III)-Tetraamidomacrocyclic ligand activator</topic><topic>Ordered microspheres</topic><topic>Surfactant-assisted self-assembly</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Chao</creatorcontrib><creatorcontrib>Xian, Zeyu</creatorcontrib><creatorcontrib>Ding, Yunhao</creatorcontrib><creatorcontrib>Jin, Xin</creatorcontrib><creatorcontrib>Gu, Cheng</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Chemosphere (Oxford)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Chao</au><au>Xian, Zeyu</au><au>Ding, Yunhao</au><au>Jin, Xin</au><au>Gu, Cheng</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols</atitle><jtitle>Chemosphere (Oxford)</jtitle><date>2020-10</date><risdate>2020</risdate><volume>256</volume><spage>127104</spage><epage>127104</epage><pages>127104-127104</pages><artnum>127104</artnum><issn>0045-6535</issn><eissn>1879-1298</eissn><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.
[Display omitted]
•A SAS method is used to synthesize FeIII-TAML based microsphere.•FeIII-TAML/DODMA shows superior reactivity in degradation of bisphenols.•FeIII-TAML/DODMA exhibits higher efficiency than free FeIII-TAML over a wide pH range.•Intermolecular forces play an important role in the enhanced reactivity of FeIII-TAML/DODMA.</abstract><pub>Elsevier Ltd</pub><doi>10.1016/j.chemosphere.2020.127104</doi><tpages>1</tpages></addata></record> |
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subjects | Bisphenols Catalytic oxidation Iron(III)-Tetraamidomacrocyclic ligand activator Ordered microspheres Surfactant-assisted self-assembly |
title | Self-assembly of FeIII-TAML-based microstructures for rapid degradation of bisphenols |
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