Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions
Апстракт
Polymer-based, highly porous nanocomposites with functionalized ligands attached to the core structure are extremely efficient in the detection, removal and recovery of metals through the process of sorption. Quantum-chemical models could be helpful for sorption process analyses. The sorption of Cu(II) ions by amino-functionalized chelating macroporous copolymers poly(GMA-co-EGDMA)-amine and sorption selectivity of the subject copolymers, ethylenediamine (en), diethylenetriamine (dien) and triethylenetetramine (trien), were successfully modelled by quantum chemical calculations. Considering the crystal structures from CSD and experimental conditions during the formation of metal complexes, the most frequent mononuclear complexes are those with the tetradentate teta ligand, while binuclear complexes are formed when the metal ion is in large excess. Although the en-copolymer was the most effective functionalized one, higher maximum sorption capacities (Q(max)) were observed for the dien-... and trien-copolymers, due to their abilities to form binuclear complexes. The enthalpy term has the greatest contribution to the total Gibbs energy change of reaction for the formation of mononuclear Cu(II) complexes (Delta G(aq)), while the solvation energy of the reaction has the greatest contribution in the formation of binuclear complexes. The results of the study indicate that small amines with the ability to form binuclear complex are the best choice for functionalization of the considered copolymer.
Кључне речи:
sorption of metal ions / amino-functionalized copolymer / DFT modelling / coordination isomers / CSDИзвор:
Journal of the Serbian Chemical Society, 2019, 84, 12, 1391-1404Издавач:
- Srpsko hemijsko društvo, Beograd
Финансирање / пројекти:
- Електропроводни и редокс-активни полимери и олигомери: синтеза, структура, својства и примена (RS-172043)
- Истраживања интеракција ензима са токсичним и фармаколошки активним молекулима (RS-172023)
- Нове технологије за мониторинг и заштиту животног окружења од штетних хемијских супстанци и радијационог оптерећења (RS-43009)
DOI: 10.2298/JSC190125031S
ISSN: 0352-5139
WoS: 000506674800005
Scopus: 2-s2.0-85079543416
Институција/група
Tehnološko-metalurški fakultetTY - JOUR AU - Suručić, Ljiljana T. AU - Nastasović, Aleksandra AU - Onjia, Antonije AU - Janjić, Goran AU - Rakić, Aleksandra PY - 2019 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/4208 AB - Polymer-based, highly porous nanocomposites with functionalized ligands attached to the core structure are extremely efficient in the detection, removal and recovery of metals through the process of sorption. Quantum-chemical models could be helpful for sorption process analyses. The sorption of Cu(II) ions by amino-functionalized chelating macroporous copolymers poly(GMA-co-EGDMA)-amine and sorption selectivity of the subject copolymers, ethylenediamine (en), diethylenetriamine (dien) and triethylenetetramine (trien), were successfully modelled by quantum chemical calculations. Considering the crystal structures from CSD and experimental conditions during the formation of metal complexes, the most frequent mononuclear complexes are those with the tetradentate teta ligand, while binuclear complexes are formed when the metal ion is in large excess. Although the en-copolymer was the most effective functionalized one, higher maximum sorption capacities (Q(max)) were observed for the dien- and trien-copolymers, due to their abilities to form binuclear complexes. The enthalpy term has the greatest contribution to the total Gibbs energy change of reaction for the formation of mononuclear Cu(II) complexes (Delta G(aq)), while the solvation energy of the reaction has the greatest contribution in the formation of binuclear complexes. The results of the study indicate that small amines with the ability to form binuclear complex are the best choice for functionalization of the considered copolymer. PB - Srpsko hemijsko društvo, Beograd T2 - Journal of the Serbian Chemical Society T1 - Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions EP - 1404 IS - 12 SP - 1391 VL - 84 DO - 10.2298/JSC190125031S ER -
@article{ author = "Suručić, Ljiljana T. and Nastasović, Aleksandra and Onjia, Antonije and Janjić, Goran and Rakić, Aleksandra", year = "2019", abstract = "Polymer-based, highly porous nanocomposites with functionalized ligands attached to the core structure are extremely efficient in the detection, removal and recovery of metals through the process of sorption. Quantum-chemical models could be helpful for sorption process analyses. The sorption of Cu(II) ions by amino-functionalized chelating macroporous copolymers poly(GMA-co-EGDMA)-amine and sorption selectivity of the subject copolymers, ethylenediamine (en), diethylenetriamine (dien) and triethylenetetramine (trien), were successfully modelled by quantum chemical calculations. Considering the crystal structures from CSD and experimental conditions during the formation of metal complexes, the most frequent mononuclear complexes are those with the tetradentate teta ligand, while binuclear complexes are formed when the metal ion is in large excess. Although the en-copolymer was the most effective functionalized one, higher maximum sorption capacities (Q(max)) were observed for the dien- and trien-copolymers, due to their abilities to form binuclear complexes. The enthalpy term has the greatest contribution to the total Gibbs energy change of reaction for the formation of mononuclear Cu(II) complexes (Delta G(aq)), while the solvation energy of the reaction has the greatest contribution in the formation of binuclear complexes. The results of the study indicate that small amines with the ability to form binuclear complex are the best choice for functionalization of the considered copolymer.", publisher = "Srpsko hemijsko društvo, Beograd", journal = "Journal of the Serbian Chemical Society", title = "Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions", pages = "1404-1391", number = "12", volume = "84", doi = "10.2298/JSC190125031S" }
Suručić, L. T., Nastasović, A., Onjia, A., Janjić, G.,& Rakić, A.. (2019). Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions. in Journal of the Serbian Chemical Society Srpsko hemijsko društvo, Beograd., 84(12), 1391-1404. https://doi.org/10.2298/JSC190125031S
Suručić LT, Nastasović A, Onjia A, Janjić G, Rakić A. Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions. in Journal of the Serbian Chemical Society. 2019;84(12):1391-1404. doi:10.2298/JSC190125031S .
Suručić, Ljiljana T., Nastasović, Aleksandra, Onjia, Antonije, Janjić, Goran, Rakić, Aleksandra, "Design of an amino-functionalized chelating macroporous copolymer poly(GMA-co-EGDMA) for the sorption of Cu(II) ions" in Journal of the Serbian Chemical Society, 84, no. 12 (2019):1391-1404, https://doi.org/10.2298/JSC190125031S . .