DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups

Alexander Carreño, Eduardo Schott, Ximena Zarate, Juan Manuel Manriquez, Juan C. Vega, Miguel Mardones, Alan H. Cowley, Ivonne Chavez, Juan P. Hinestroza, Ramiro Arratia-Perez

Resultado de la investigación: Contribución a la publicaciónArticle

Resumen

Research in functionalized inorganic supports faces special challenges regarding the inmobilization of organic chains and efficient computational methods for the quantum chemical modeling of coordination compounds. The silylant 3-cloropropyltriethoxysilyl (R1) was anchored over silica gel in anhydrous conditions, in order to react with diethyl Iminodiacetate (DIDA) to obtain modified silica gel (R2), which was hydrolized in basic conditions previously synthesized and characterized by S BET, TGA and FTIR spectroscopy to obtain iminodiacetic acid groups IDA to prepare an modified inorganic support (R3) that is able to get hands on metals from the first transition series such as copper and nickel. The obtained experimental values showed that the functionalized grade of R3 corresponds to 0.1598 mmol of the nitrogen indicated that the adsorbed Cu(II) or Ni(II) have the stoichiometry for both cation of 1:1. Based on this relation, the three different structures were proposed to carry out the computational studies using density functional theory (DFT) in its LDA and PW91 with the TZP slater type basis set. The primary coordination sphere of copper(II) or nickel (II) ion in R3 are optimized, structural parameters are calculated, vibrational bands are assigned and energy gaps of frontier orbital (HOMO-LUMO) have been calculated. The calculated results reproduced the experimental data with good agreement. An energy decomposition analysis (EDA) of the different models proposed here was performed and suggest a 1:1 coordination form.

Idioma originalEnglish
Páginas (desde - hasta)1019-1030
Número de páginas12
PublicaciónChemical Papers
Volumen71
Número de edición6
Identificadores de objetos digitales
EstadoPublished - 1 jun 2017

Huella dactilar

Silica Gel
Nickel
Adsorption
Copper
Silica gel
Density functional theory
Fourier Transform Infrared Spectroscopy
Cations
Spectrum Analysis
Nitrogen
Metals
Ions
Acids
Computational methods
Stoichiometry
Energy gap
Positive ions
Spectroscopy
Decomposition

Keywords

    ASJC Scopus subject areas

    • Chemistry(all)
    • Biochemistry
    • Chemical Engineering(all)
    • Industrial and Manufacturing Engineering
    • Materials Chemistry

    Citar esto

    Carreño, Alexander; Schott, Eduardo; Zarate, Ximena; Manriquez, Juan Manuel; Vega, Juan C.; Mardones, Miguel; Cowley, Alan H.; Chavez, Ivonne; Hinestroza, Juan P.; Arratia-Perez, Ramiro / DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups.

    En: Chemical Papers, Vol. 71, N.º 6, 01.06.2017, p. 1019-1030.

    Resultado de la investigación: Contribución a la publicaciónArticle

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    title = "DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups",
    abstract = "Research in functionalized inorganic supports faces special challenges regarding the inmobilization of organic chains and efficient computational methods for the quantum chemical modeling of coordination compounds. The silylant 3-cloropropyltriethoxysilyl (R1) was anchored over silica gel in anhydrous conditions, in order to react with diethyl Iminodiacetate (DIDA) to obtain modified silica gel (R2), which was hydrolized in basic conditions previously synthesized and characterized by S BET, TGA and FTIR spectroscopy to obtain iminodiacetic acid groups IDA to prepare an modified inorganic support (R3) that is able to get hands on metals from the first transition series such as copper and nickel. The obtained experimental values showed that the functionalized grade of R3 corresponds to 0.1598 mmol of the nitrogen indicated that the adsorbed Cu(II) or Ni(II) have the stoichiometry for both cation of 1:1. Based on this relation, the three different structures were proposed to carry out the computational studies using density functional theory (DFT) in its LDA and PW91 with the TZP slater type basis set. The primary coordination sphere of copper(II) or nickel (II) ion in R3 are optimized, structural parameters are calculated, vibrational bands are assigned and energy gaps of frontier orbital (HOMO-LUMO) have been calculated. The calculated results reproduced the experimental data with good agreement. An energy decomposition analysis (EDA) of the different models proposed here was performed and suggest a 1:1 coordination form.",
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    author = "Alexander Carreño and Eduardo Schott and Ximena Zarate and Manriquez, {Juan Manuel} and Vega, {Juan C.} and Miguel Mardones and Cowley, {Alan H.} and Ivonne Chavez and Hinestroza, {Juan P.} and Ramiro Arratia-Perez",
    year = "2017",
    month = "6",
    doi = "10.1007/s11696-016-0022-6",
    volume = "71",
    pages = "1019--1030",
    journal = "Chemical Papers",
    issn = "0366-6352",
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    Carreño, A, Schott, E, Zarate, X, Manriquez, JM, Vega, JC, Mardones, M, Cowley, AH, Chavez, I, Hinestroza, JP & Arratia-Perez, R 2017, 'DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups' Chemical Papers, vol. 71, n.º 6, pp. 1019-1030. DOI: 10.1007/s11696-016-0022-6

    DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups. / Carreño, Alexander; Schott, Eduardo; Zarate, Ximena; Manriquez, Juan Manuel; Vega, Juan C.; Mardones, Miguel; Cowley, Alan H.; Chavez, Ivonne; Hinestroza, Juan P.; Arratia-Perez, Ramiro.

    En: Chemical Papers, Vol. 71, N.º 6, 01.06.2017, p. 1019-1030.

    Resultado de la investigación: Contribución a la publicaciónArticle

    TY - JOUR

    T1 - DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups

    AU - Carreño,Alexander

    AU - Schott,Eduardo

    AU - Zarate,Ximena

    AU - Manriquez,Juan Manuel

    AU - Vega,Juan C.

    AU - Mardones,Miguel

    AU - Cowley,Alan H.

    AU - Chavez,Ivonne

    AU - Hinestroza,Juan P.

    AU - Arratia-Perez,Ramiro

    PY - 2017/6/1

    Y1 - 2017/6/1

    N2 - Research in functionalized inorganic supports faces special challenges regarding the inmobilization of organic chains and efficient computational methods for the quantum chemical modeling of coordination compounds. The silylant 3-cloropropyltriethoxysilyl (R1) was anchored over silica gel in anhydrous conditions, in order to react with diethyl Iminodiacetate (DIDA) to obtain modified silica gel (R2), which was hydrolized in basic conditions previously synthesized and characterized by S BET, TGA and FTIR spectroscopy to obtain iminodiacetic acid groups IDA to prepare an modified inorganic support (R3) that is able to get hands on metals from the first transition series such as copper and nickel. The obtained experimental values showed that the functionalized grade of R3 corresponds to 0.1598 mmol of the nitrogen indicated that the adsorbed Cu(II) or Ni(II) have the stoichiometry for both cation of 1:1. Based on this relation, the three different structures were proposed to carry out the computational studies using density functional theory (DFT) in its LDA and PW91 with the TZP slater type basis set. The primary coordination sphere of copper(II) or nickel (II) ion in R3 are optimized, structural parameters are calculated, vibrational bands are assigned and energy gaps of frontier orbital (HOMO-LUMO) have been calculated. The calculated results reproduced the experimental data with good agreement. An energy decomposition analysis (EDA) of the different models proposed here was performed and suggest a 1:1 coordination form.

    AB - Research in functionalized inorganic supports faces special challenges regarding the inmobilization of organic chains and efficient computational methods for the quantum chemical modeling of coordination compounds. The silylant 3-cloropropyltriethoxysilyl (R1) was anchored over silica gel in anhydrous conditions, in order to react with diethyl Iminodiacetate (DIDA) to obtain modified silica gel (R2), which was hydrolized in basic conditions previously synthesized and characterized by S BET, TGA and FTIR spectroscopy to obtain iminodiacetic acid groups IDA to prepare an modified inorganic support (R3) that is able to get hands on metals from the first transition series such as copper and nickel. The obtained experimental values showed that the functionalized grade of R3 corresponds to 0.1598 mmol of the nitrogen indicated that the adsorbed Cu(II) or Ni(II) have the stoichiometry for both cation of 1:1. Based on this relation, the three different structures were proposed to carry out the computational studies using density functional theory (DFT) in its LDA and PW91 with the TZP slater type basis set. The primary coordination sphere of copper(II) or nickel (II) ion in R3 are optimized, structural parameters are calculated, vibrational bands are assigned and energy gaps of frontier orbital (HOMO-LUMO) have been calculated. The calculated results reproduced the experimental data with good agreement. An energy decomposition analysis (EDA) of the different models proposed here was performed and suggest a 1:1 coordination form.

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    KW - Morokuma-Ziegler methodology

    KW - Silica gel

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    Carreño A, Schott E, Zarate X, Manriquez JM, Vega JC, Mardones M y otros. DFT studies on coordination models for adsorption essays of Cu(II) and Ni(II) solutions in modified silica gel with iminodiacetic groups. Chemical Papers. 2017 jun 1;71(6):1019-1030. Disponible desde, DOI: 10.1007/s11696-016-0022-6