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Qatar National Research Fund - NPRP grant (7-665-1-125)

Authors

Publications

Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study

Đorđević, Vesna R.; Sredojević, Dušan; Dostanić, Jasmina; Lončarević, Davor; Ahrenkiel, Scott Phillip; Švrakić, Nenad M.; Brothers, Edward N.; Belić, Milivoj R.; Nedeljković, Jovan

(2019)

TY  - JOUR
AU  - Đorđević, Vesna R.
AU  - Sredojević, Dušan
AU  - Dostanić, Jasmina
AU  - Lončarević, Davor
AU  - Ahrenkiel, Scott Phillip
AU  - Švrakić, Nenad M.
AU  - Brothers, Edward N.
AU  - Belić, Milivoj R.
AU  - Nedeljković, Jovan
PY  - 2019
UR  - https://linkinghub.elsevier.com/retrieve/pii/S1387181118303639
UR  - https://vinar.vin.bg.ac.rs/handle/123456789/7763
AB  - Surface modification of Al2O3 powders, prepared using reproducible sol-gel synthetic route with small colorless organic molecules, induces charge transfer complex formation and the appearance of absorption in the visible spectral region. Comprehensive microstructural characterization involving transmission electron microscopy, X-ray diffraction analysis, and nitrogen adsorption–desorption isotherms, revealed that γ-crystalline alumina powders consist of mesoporous particles in the size range from 0.1 to 0.3 μm, with specific surface area of 54.8 m2/g, and pore radius between 3 and 4 nm. The attachment of catecholate-type of ligands (catechol, caffeic acid, gallic acid, dopamine and 2,3-dihydroxy naphthalene), salicylate-type of ligands (salicylic acid and 5-amino salicylic acid), and ascorbic acid, to the surface such γ-Al2O3 particles leads to the formation of colored powders and activates their absorption in visible-light spectral region. To the best of our knowledge, similar transformation of an insulator (Al2O3), with the band gap energy of 8.7 eV, into a semiconductor-like hybrid material with tunable optical properties has not been reported in the literature before. The density functional theory (DFT) calculations with periodic boundary conditions were performed in order to estimate the energy gaps of various inorganic/organic hybrids. The calculated values compare well with the experimental data. The good agreement between the calculated and experimentally determined band gaps was found, thus demonstrating predictive ability of the theory when proper model is used.
T2  - Microporous and Mesoporous Materials
T1  - Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study
VL  - 273
SP  - 41
EP  - 49
DO  - 10.1016/j.micromeso.2018.06.053
ER  - 
@article{
author = "Đorđević, Vesna R. and Sredojević, Dušan and Dostanić, Jasmina and Lončarević, Davor and Ahrenkiel, Scott Phillip and Švrakić, Nenad M. and Brothers, Edward N. and Belić, Milivoj R. and Nedeljković, Jovan",
year = "2019",
abstract = "Surface modification of Al2O3 powders, prepared using reproducible sol-gel synthetic route with small colorless organic molecules, induces charge transfer complex formation and the appearance of absorption in the visible spectral region. Comprehensive microstructural characterization involving transmission electron microscopy, X-ray diffraction analysis, and nitrogen adsorption–desorption isotherms, revealed that γ-crystalline alumina powders consist of mesoporous particles in the size range from 0.1 to 0.3 μm, with specific surface area of 54.8 m2/g, and pore radius between 3 and 4 nm. The attachment of catecholate-type of ligands (catechol, caffeic acid, gallic acid, dopamine and 2,3-dihydroxy naphthalene), salicylate-type of ligands (salicylic acid and 5-amino salicylic acid), and ascorbic acid, to the surface such γ-Al2O3 particles leads to the formation of colored powders and activates their absorption in visible-light spectral region. To the best of our knowledge, similar transformation of an insulator (Al2O3), with the band gap energy of 8.7 eV, into a semiconductor-like hybrid material with tunable optical properties has not been reported in the literature before. The density functional theory (DFT) calculations with periodic boundary conditions were performed in order to estimate the energy gaps of various inorganic/organic hybrids. The calculated values compare well with the experimental data. The good agreement between the calculated and experimentally determined band gaps was found, thus demonstrating predictive ability of the theory when proper model is used.",
journal = "Microporous and Mesoporous Materials",
title = "Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study",
volume = "273",
pages = "41-49",
doi = "10.1016/j.micromeso.2018.06.053"
}
Đorđević, V. R., Sredojević, D., Dostanić, J., Lončarević, D., Ahrenkiel, S. P., Švrakić, N. M., Brothers, E. N., Belić, M. R.,& Nedeljković, J.. (2019). Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study. in Microporous and Mesoporous Materials, 273, 41-49.
https://doi.org/10.1016/j.micromeso.2018.06.053
Đorđević VR, Sredojević D, Dostanić J, Lončarević D, Ahrenkiel SP, Švrakić NM, Brothers EN, Belić MR, Nedeljković J. Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study. in Microporous and Mesoporous Materials. 2019;273:41-49.
doi:10.1016/j.micromeso.2018.06.053 .
Đorđević, Vesna R., Sredojević, Dušan, Dostanić, Jasmina, Lončarević, Davor, Ahrenkiel, Scott Phillip, Švrakić, Nenad M., Brothers, Edward N., Belić, Milivoj R., Nedeljković, Jovan, "Visible light absorption of surface-modified Al2O3 powders: A comparative DFT and experimental study" in Microporous and Mesoporous Materials, 273 (2019):41-49,
https://doi.org/10.1016/j.micromeso.2018.06.053 . .
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Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework

Sredojević, Dušan; Moncho, Salvador; Raju, Rajesh Kumar; Belić, Milivoj R.; Brothers, Edward N.

(2018)

TY  - JOUR
AU  - Sredojević, Dušan
AU  - Moncho, Salvador
AU  - Raju, Rajesh Kumar
AU  - Belić, Milivoj R.
AU  - Brothers, Edward N.
PY  - 2018
UR  - https://vinar.vin.bg.ac.rs/handle/123456789/7901
AB  - We performed density functional theory computations to study the structural and electronic properties as the basis of ethylene addition activity for [Ni(XC)4]n (X = Se, S)-extended lattices. We demonstrated that the mechanism of ethylene cycloaddition to a periodic [Ni(SeC)4]n two-dimensional (2D) network is analogous to that previously described for [Ni(SC)4]n 2D sheets and similar to the metal bis(dithiolene) molecular complexes [M(S2C2R2)2] (M = Ni, Pd, Pt, Co, Cu). These nanosheet materials avoid decomposition upon olefin addition, which is one of the main limitations of the molecular metal bis(dithiolene) complexes, as we find the decomposition processes to be thermodynamically unfavorable. Our calculations also suggest that the preferred conformation of the [Ni(SeC)4]n bilayer lattice is parallel displaced, with the Se atoms positioned above the Ni atoms, which is different from the eclipsed conformation found for [Ni(SC)4]n. We also managed to optimize an adduct of [Ni(SC)4]n in the bilayer form, which exceed the ethylene coverage of molecular complexes. We calculate that the preferred three-dimensional geometry of the stacked sheets is eclipsed because of strong van der Waals interactions. Such an arrangement of the sheets indicates that these materials should be highly porous, pointing to the high capacity for olefin bindings. Indeed, a few moderately stable ethylene adducts have been located. Owing to their unique structures and chemical reactivity, these newly predicted materials can be potentially developed as electrocatalysts for olefin purification. © 2018 American Chemical Society.
T2  - The Journal of Physical Chemistry C
T1  - Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework
VL  - 122
IS  - 39
SP  - 22424
EP  - 22434
DO  - 10.1021/acs.jpcc.8b05707
ER  - 
@article{
author = "Sredojević, Dušan and Moncho, Salvador and Raju, Rajesh Kumar and Belić, Milivoj R. and Brothers, Edward N.",
year = "2018",
abstract = "We performed density functional theory computations to study the structural and electronic properties as the basis of ethylene addition activity for [Ni(XC)4]n (X = Se, S)-extended lattices. We demonstrated that the mechanism of ethylene cycloaddition to a periodic [Ni(SeC)4]n two-dimensional (2D) network is analogous to that previously described for [Ni(SC)4]n 2D sheets and similar to the metal bis(dithiolene) molecular complexes [M(S2C2R2)2] (M = Ni, Pd, Pt, Co, Cu). These nanosheet materials avoid decomposition upon olefin addition, which is one of the main limitations of the molecular metal bis(dithiolene) complexes, as we find the decomposition processes to be thermodynamically unfavorable. Our calculations also suggest that the preferred conformation of the [Ni(SeC)4]n bilayer lattice is parallel displaced, with the Se atoms positioned above the Ni atoms, which is different from the eclipsed conformation found for [Ni(SC)4]n. We also managed to optimize an adduct of [Ni(SC)4]n in the bilayer form, which exceed the ethylene coverage of molecular complexes. We calculate that the preferred three-dimensional geometry of the stacked sheets is eclipsed because of strong van der Waals interactions. Such an arrangement of the sheets indicates that these materials should be highly porous, pointing to the high capacity for olefin bindings. Indeed, a few moderately stable ethylene adducts have been located. Owing to their unique structures and chemical reactivity, these newly predicted materials can be potentially developed as electrocatalysts for olefin purification. © 2018 American Chemical Society.",
journal = "The Journal of Physical Chemistry C",
title = "Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework",
volume = "122",
number = "39",
pages = "22424-22434",
doi = "10.1021/acs.jpcc.8b05707"
}
Sredojević, D., Moncho, S., Raju, R. K., Belić, M. R.,& Brothers, E. N.. (2018). Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework. in The Journal of Physical Chemistry C, 122(39), 22424-22434.
https://doi.org/10.1021/acs.jpcc.8b05707
Sredojević D, Moncho S, Raju RK, Belić MR, Brothers EN. Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework. in The Journal of Physical Chemistry C. 2018;122(39):22424-22434.
doi:10.1021/acs.jpcc.8b05707 .
Sredojević, Dušan, Moncho, Salvador, Raju, Rajesh Kumar, Belić, Milivoj R., Brothers, Edward N., "Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework" in The Journal of Physical Chemistry C, 122, no. 39 (2018):22424-22434,
https://doi.org/10.1021/acs.jpcc.8b05707 . .
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Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework

Sredojević, Dušan; Moncho, Salvador; Raju, Rajesh Kumar; Belić, Milivoj R.; Brothers, Edward N.

(2018)

TY  - DATA
AU  - Sredojević, Dušan
AU  - Moncho, Salvador
AU  - Raju, Rajesh Kumar
AU  - Belić, Milivoj R.
AU  - Brothers, Edward N.
PY  - 2018
UR  - https://vinar.vin.bg.ac.rs/handle/123456789/7902
UR  - https://figshare.com/articles/journal_contribution/Reversible_Olefin_Addition_to_Extended_Lattices_of_a_Nickel_Selenium_Framework/7123238
AB  - We performed density functional theory computations to study the structural and electronic properties as the basis of ethylene addition activity for [Ni(XC)4]n (X = Se, S)-extended lattices. We demonstrated that the mechanism of ethylene cycloaddition to a periodic [Ni(SeC)4]n two-dimensional (2D) network is analogous to that previously described for [Ni(SC)4]n 2D sheets and similar to the metal bis(dithiolene) molecular complexes [M(S2C2R2)2] (M = Ni, Pd, Pt, Co, Cu). These nanosheet materials avoid decomposition upon olefin addition, which is one of the main limitations of the molecular metal bis(dithiolene) complexes, as we find the decomposition processes to be thermodynamically unfavorable. Our calculations also suggest that the preferred conformation of the [Ni(SeC)4]n bilayer lattice is parallel displaced, with the Se atoms positioned above the Ni atoms, which is different from the eclipsed conformation found for [Ni(SC)4]n. We also managed to optimize an adduct of [Ni(SC)4]n in the bilayer form, which exceed the ethylene coverage of molecular complexes. We calculate that the preferred three-dimensional geometry of the stacked sheets is eclipsed because of strong van der Waals interactions. Such an arrangement of the sheets indicates that these materials should be highly porous, pointing to the high capacity for olefin bindings. Indeed, a few moderately stable ethylene adducts have been located. Owing to their unique structures and chemical reactivity, these newly predicted materials can be potentially developed as electrocatalysts for olefin purification. © 2018 American Chemical Society.
T2  - The Journal of Physical Chemistry C
T1  - Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework
VL  - 122
IS  - 39
SP  - 22424
EP  - 22434
DO  - 10.1021/acs.jpcc.8b05707
ER  - 
@misc{
author = "Sredojević, Dušan and Moncho, Salvador and Raju, Rajesh Kumar and Belić, Milivoj R. and Brothers, Edward N.",
year = "2018",
abstract = "We performed density functional theory computations to study the structural and electronic properties as the basis of ethylene addition activity for [Ni(XC)4]n (X = Se, S)-extended lattices. We demonstrated that the mechanism of ethylene cycloaddition to a periodic [Ni(SeC)4]n two-dimensional (2D) network is analogous to that previously described for [Ni(SC)4]n 2D sheets and similar to the metal bis(dithiolene) molecular complexes [M(S2C2R2)2] (M = Ni, Pd, Pt, Co, Cu). These nanosheet materials avoid decomposition upon olefin addition, which is one of the main limitations of the molecular metal bis(dithiolene) complexes, as we find the decomposition processes to be thermodynamically unfavorable. Our calculations also suggest that the preferred conformation of the [Ni(SeC)4]n bilayer lattice is parallel displaced, with the Se atoms positioned above the Ni atoms, which is different from the eclipsed conformation found for [Ni(SC)4]n. We also managed to optimize an adduct of [Ni(SC)4]n in the bilayer form, which exceed the ethylene coverage of molecular complexes. We calculate that the preferred three-dimensional geometry of the stacked sheets is eclipsed because of strong van der Waals interactions. Such an arrangement of the sheets indicates that these materials should be highly porous, pointing to the high capacity for olefin bindings. Indeed, a few moderately stable ethylene adducts have been located. Owing to their unique structures and chemical reactivity, these newly predicted materials can be potentially developed as electrocatalysts for olefin purification. © 2018 American Chemical Society.",
journal = "The Journal of Physical Chemistry C",
title = "Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework",
volume = "122",
number = "39",
pages = "22424-22434",
doi = "10.1021/acs.jpcc.8b05707"
}
Sredojević, D., Moncho, S., Raju, R. K., Belić, M. R.,& Brothers, E. N.. (2018). Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework. in The Journal of Physical Chemistry C, 122(39), 22424-22434.
https://doi.org/10.1021/acs.jpcc.8b05707
Sredojević D, Moncho S, Raju RK, Belić MR, Brothers EN. Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework. in The Journal of Physical Chemistry C. 2018;122(39):22424-22434.
doi:10.1021/acs.jpcc.8b05707 .
Sredojević, Dušan, Moncho, Salvador, Raju, Rajesh Kumar, Belić, Milivoj R., Brothers, Edward N., "Supporting information for: Reversible Olefin Addition to Extended Lattices of a Nickel–Selenium Framework" in The Journal of Physical Chemistry C, 122, no. 39 (2018):22424-22434,
https://doi.org/10.1021/acs.jpcc.8b05707 . .
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