Mali, Gregor

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orcid::0000-0002-9012-2495
  • Mali, Gregor (9)
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Author's Bibliography

Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid

Pavlović, Jelena; Popova, M.; Mihalyi, R. M.; Mazaj, Matjaz; Mali, Gregor; Kovač, Janez; Lazarova, H.; Rajić, Nevenka

(Elsevier B.V., 2019)

TY  - JOUR
AU  - Pavlović, Jelena
AU  - Popova, M.
AU  - Mihalyi, R. M.
AU  - Mazaj, Matjaz
AU  - Mali, Gregor
AU  - Kovač, Janez
AU  - Lazarova, H.
AU  - Rajić, Nevenka
PY  - 2019
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/4157
AB  - Catalysts based on natural zeolite - clinoptilolite loaded with either SnO2 (TOHCLI) or sulfated SnO2 (STOHCLI) were prepared and tested in the esterification of levulinic acid (LA) with octanol or ethanol. The Sn content in TOHCLI and STOHCLI varied from 4.5 to 12.3 wt.%. The catalysts were characterized by powder X-ray diffraction method, scanning electron microscopy coupled with energy dispersive X-ray spectroscopy, thermal analysis, X-ray photoelectron spectroscopy, NZ physisorption at - 196 degrees C, (27)A1 and Si-29 MAS NMR solid state spectroscopy and FTIR spectroscopy for analysis of acidic centers. A high conversion rate of LA into octyl- (OLA) or ethyl levulinate (ELA) was obtained for both TOHCLI and STOHCLI. TOHCLI showed a high activity in the conversion of LA into OLA (55%) and a moderate activity in the conversion to ELA (22%). STOHCLI led to a total conversion of LA to OLA and ELA due to the presence of a high amount of Bronsted and Lewis acid sites in the catalysts. The catalytic activity decreased to 86% for OLA and to 66% for ELA after next five cycles. Lower catalytic activity in the repeated cycles during ELA formation was explained by pore blockage due to coke formation.
PB  - Elsevier B.V.
T2  - Microporous and Mesoporous Materials
T1  - Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid
EP  - 18
SP  - 10
VL  - 279
DO  - 10.1016/j.micromeso.2018.12.009
ER  - 
@article{
author = "Pavlović, Jelena and Popova, M. and Mihalyi, R. M. and Mazaj, Matjaz and Mali, Gregor and Kovač, Janez and Lazarova, H. and Rajić, Nevenka",
year = "2019",
abstract = "Catalysts based on natural zeolite - clinoptilolite loaded with either SnO2 (TOHCLI) or sulfated SnO2 (STOHCLI) were prepared and tested in the esterification of levulinic acid (LA) with octanol or ethanol. The Sn content in TOHCLI and STOHCLI varied from 4.5 to 12.3 wt.%. The catalysts were characterized by powder X-ray diffraction method, scanning electron microscopy coupled with energy dispersive X-ray spectroscopy, thermal analysis, X-ray photoelectron spectroscopy, NZ physisorption at - 196 degrees C, (27)A1 and Si-29 MAS NMR solid state spectroscopy and FTIR spectroscopy for analysis of acidic centers. A high conversion rate of LA into octyl- (OLA) or ethyl levulinate (ELA) was obtained for both TOHCLI and STOHCLI. TOHCLI showed a high activity in the conversion of LA into OLA (55%) and a moderate activity in the conversion to ELA (22%). STOHCLI led to a total conversion of LA to OLA and ELA due to the presence of a high amount of Bronsted and Lewis acid sites in the catalysts. The catalytic activity decreased to 86% for OLA and to 66% for ELA after next five cycles. Lower catalytic activity in the repeated cycles during ELA formation was explained by pore blockage due to coke formation.",
publisher = "Elsevier B.V.",
journal = "Microporous and Mesoporous Materials",
title = "Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid",
pages = "18-10",
volume = "279",
doi = "10.1016/j.micromeso.2018.12.009"
}
Pavlović, J., Popova, M., Mihalyi, R. M., Mazaj, M., Mali, G., Kovač, J., Lazarova, H.,& Rajić, N.. (2019). Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid. in Microporous and Mesoporous Materials
Elsevier B.V.., 279, 10-18.
https://doi.org/10.1016/j.micromeso.2018.12.009
Pavlović J, Popova M, Mihalyi RM, Mazaj M, Mali G, Kovač J, Lazarova H, Rajić N. Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid. in Microporous and Mesoporous Materials. 2019;279:10-18.
doi:10.1016/j.micromeso.2018.12.009 .
Pavlović, Jelena, Popova, M., Mihalyi, R. M., Mazaj, Matjaz, Mali, Gregor, Kovač, Janez, Lazarova, H., Rajić, Nevenka, "Catalytic activity of SnO2- and SO4 /SnO2-containing clinoptilolite in the esterification of levulinic acid" in Microporous and Mesoporous Materials, 279 (2019):10-18,
https://doi.org/10.1016/j.micromeso.2018.12.009 . .
1
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Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid

Pavlović, Jelena; Popova, M.; Mihalyi, R. M.; Mazaj, Matjaz; Mali, Gregor; Kovač, Janez; Lazarova, H.; Rajić, Nevenka

(Elsevier B.V., 2019)

TY  - JOUR
AU  - Pavlović, Jelena
AU  - Popova, M.
AU  - Mihalyi, R. M.
AU  - Mazaj, Matjaz
AU  - Mali, Gregor
AU  - Kovač, Janez
AU  - Lazarova, H.
AU  - Rajić, Nevenka
PY  - 2019
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5042
AB  - Catalysts based on natural zeolite – clinoptilolite loaded with either SnO2 (TOHCLI) or sulfated SnO2 (STOHCLI) were prepared and tested in the esterification of levulinic acid (LA) with octanol or ethanol. The Sn content in TOHCLI and STOHCLI varied from 4.5 to 12.3 wt.%. The catalysts were characterized by powder X-ray diffraction method, scanning electron microscopy coupled with energy dispersive X-ray spectroscopy, thermal analysis, X-ray photoelectron spectroscopy, N2 physisorption at −196 °C, 27Al and 29Si MAS NMR solid state spectroscopy and FTIR spectroscopy for analysis of acidic centers. A high conversion rate of LA into octyl- (OLA) or ethyl levulinate (ELA) was obtained for both TOHCLI and STOHCLI. TOHCLI showed a high activity in the conversion of LA into OLA (55%) and a moderate activity in the conversion to ELA (22%). STOHCLI led to a total conversion of LA to OLA and ELA due to the presence of a high amount of Brønsted and Lewis acid sites in the catalysts. The catalytic activity decreased to 86% for OLA and to 66% for ELA after next five cycles. Lower catalytic activity in the repeated cycles during ELA formation was explained by pore blockage due to coke formation.
PB  - Elsevier B.V.
T2  - Microporous and Mesoporous Materials
T1  - Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid
EP  - 18
SP  - 10
VL  - 279
DO  - 10.1016/j.micromeso.2018.12.009
ER  - 
@article{
author = "Pavlović, Jelena and Popova, M. and Mihalyi, R. M. and Mazaj, Matjaz and Mali, Gregor and Kovač, Janez and Lazarova, H. and Rajić, Nevenka",
year = "2019",
abstract = "Catalysts based on natural zeolite – clinoptilolite loaded with either SnO2 (TOHCLI) or sulfated SnO2 (STOHCLI) were prepared and tested in the esterification of levulinic acid (LA) with octanol or ethanol. The Sn content in TOHCLI and STOHCLI varied from 4.5 to 12.3 wt.%. The catalysts were characterized by powder X-ray diffraction method, scanning electron microscopy coupled with energy dispersive X-ray spectroscopy, thermal analysis, X-ray photoelectron spectroscopy, N2 physisorption at −196 °C, 27Al and 29Si MAS NMR solid state spectroscopy and FTIR spectroscopy for analysis of acidic centers. A high conversion rate of LA into octyl- (OLA) or ethyl levulinate (ELA) was obtained for both TOHCLI and STOHCLI. TOHCLI showed a high activity in the conversion of LA into OLA (55%) and a moderate activity in the conversion to ELA (22%). STOHCLI led to a total conversion of LA to OLA and ELA due to the presence of a high amount of Brønsted and Lewis acid sites in the catalysts. The catalytic activity decreased to 86% for OLA and to 66% for ELA after next five cycles. Lower catalytic activity in the repeated cycles during ELA formation was explained by pore blockage due to coke formation.",
publisher = "Elsevier B.V.",
journal = "Microporous and Mesoporous Materials",
title = "Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid",
pages = "18-10",
volume = "279",
doi = "10.1016/j.micromeso.2018.12.009"
}
Pavlović, J., Popova, M., Mihalyi, R. M., Mazaj, M., Mali, G., Kovač, J., Lazarova, H.,& Rajić, N.. (2019). Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid. in Microporous and Mesoporous Materials
Elsevier B.V.., 279, 10-18.
https://doi.org/10.1016/j.micromeso.2018.12.009
Pavlović J, Popova M, Mihalyi RM, Mazaj M, Mali G, Kovač J, Lazarova H, Rajić N. Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid. in Microporous and Mesoporous Materials. 2019;279:10-18.
doi:10.1016/j.micromeso.2018.12.009 .
Pavlović, Jelena, Popova, M., Mihalyi, R. M., Mazaj, Matjaz, Mali, Gregor, Kovač, Janez, Lazarova, H., Rajić, Nevenka, "Catalytic activity of SnO2- and SO4/SnO2-containing clinoptilolite in the esterification of levulinic acid" in Microporous and Mesoporous Materials, 279 (2019):10-18,
https://doi.org/10.1016/j.micromeso.2018.12.009 . .
1
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Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics

Kaplanec, Iva; Recnik, Aleksander; Mali, Gregor; Rajić, Nevenka

(Desalination Publ, Hopkinton, 2017)

TY  - JOUR
AU  - Kaplanec, Iva
AU  - Recnik, Aleksander
AU  - Mali, Gregor
AU  - Rajić, Nevenka
PY  - 2017
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/3581
AB  - Clinoptilolite-rich tuff (Z) enriched with Fe(III) was studied in the removal of phosphate ions present in aqueous medium at pH = 6.5. Fe(III) modification was performed by a simple wet impregnation giving the product (FeZ) with about 18 wt% Fe. Transmission electron microscopy showed the presence of a flaky Fe(III) amorphous precipitate on the clinoptilolite sheets and a preserved clinoptilolite crystallinity. The modification increased the specific surface area from 28.6 to 140.3 m(2) g(-1). FeZ effectively adsorbed phosphate, the removal rate at 298 K varying from 86% to 42.5% (for C-0 = 50 mg dm(-3) and C-0 = 400 mg dm(-3)). The sorption isotherms were in accord with the Langmuir model, giving for the Langmuir constant (R-L) values in the range 0-1 that are characteristic of a favourable adsorption. The data for adsorption kinetics were best described by the pseudo-second-order model suggesting chemisorption as the phosphate sorption mechanism. Intra-particle diffusion was present in the adsorption, but it was not the rate-limiting step. A P-31 static spin-echo mapping nuclear magnetic resonance (NMR) measurement was performed for studying the phosphate-FeZ interaction. The results showed that the phosphate adsorption on FeZ proceeds through electrostatic interactions and covalent bonding, the latter being more pronounced.
PB  - Desalination Publ, Hopkinton
T2  - Desalination and Water Treatment
T1  - Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics
EP  - 240
SP  - 231
VL  - 78
DO  - 10.5004/dwt.2017.20875
ER  - 
@article{
author = "Kaplanec, Iva and Recnik, Aleksander and Mali, Gregor and Rajić, Nevenka",
year = "2017",
abstract = "Clinoptilolite-rich tuff (Z) enriched with Fe(III) was studied in the removal of phosphate ions present in aqueous medium at pH = 6.5. Fe(III) modification was performed by a simple wet impregnation giving the product (FeZ) with about 18 wt% Fe. Transmission electron microscopy showed the presence of a flaky Fe(III) amorphous precipitate on the clinoptilolite sheets and a preserved clinoptilolite crystallinity. The modification increased the specific surface area from 28.6 to 140.3 m(2) g(-1). FeZ effectively adsorbed phosphate, the removal rate at 298 K varying from 86% to 42.5% (for C-0 = 50 mg dm(-3) and C-0 = 400 mg dm(-3)). The sorption isotherms were in accord with the Langmuir model, giving for the Langmuir constant (R-L) values in the range 0-1 that are characteristic of a favourable adsorption. The data for adsorption kinetics were best described by the pseudo-second-order model suggesting chemisorption as the phosphate sorption mechanism. Intra-particle diffusion was present in the adsorption, but it was not the rate-limiting step. A P-31 static spin-echo mapping nuclear magnetic resonance (NMR) measurement was performed for studying the phosphate-FeZ interaction. The results showed that the phosphate adsorption on FeZ proceeds through electrostatic interactions and covalent bonding, the latter being more pronounced.",
publisher = "Desalination Publ, Hopkinton",
journal = "Desalination and Water Treatment",
title = "Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics",
pages = "240-231",
volume = "78",
doi = "10.5004/dwt.2017.20875"
}
Kaplanec, I., Recnik, A., Mali, G.,& Rajić, N.. (2017). Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics. in Desalination and Water Treatment
Desalination Publ, Hopkinton., 78, 231-240.
https://doi.org/10.5004/dwt.2017.20875
Kaplanec I, Recnik A, Mali G, Rajić N. Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics. in Desalination and Water Treatment. 2017;78:231-240.
doi:10.5004/dwt.2017.20875 .
Kaplanec, Iva, Recnik, Aleksander, Mali, Gregor, Rajić, Nevenka, "Study of the iron(III)-modified clinoptilolite in the adsorption of phosphate from aqueous medium: mechanism and kinetics" in Desalination and Water Treatment, 78 (2017):231-240,
https://doi.org/10.5004/dwt.2017.20875 . .
6
1
6

On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3

Rajić, Nevenka; Stojaković, Đorđe; Jevtić, Sanja; Zabukovec-Logar, Nataša; Mali, Gregor; Kaučič, Venčeslav

(Springer, Dordrecht, 2010)

TY  - JOUR
AU  - Rajić, Nevenka
AU  - Stojaković, Đorđe
AU  - Jevtić, Sanja
AU  - Zabukovec-Logar, Nataša
AU  - Mali, Gregor
AU  - Kaučič, Venčeslav
PY  - 2010
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/1638
AB  - An open-framework aluminophosphate analog of the fluorogallophosphate structure-type ULM-3 was obtained by hydrothermal crystallization of an aqueous aluminum phosphate suspension in the presence of 3-methylpropylamine (MAPA) and hydrofluoric acid. The open-framework fluorinated aluminophosphate structure was confirmed by Rietveld analysis and the (27)Al, (31)P, and (19)F MAS NMR spectroscopy. The MAPA, located in the ten-membered ring channels, is doubly protonated to balance the negative charge of the Al(3)P(3)O(12)F(2) (2-) framework. Thermogravimetric analysis data have been used to study kinetics of the thermal decomposition of MAPA. The decomposition was found to be a complex process, its activation energy varied from 177 to 259 kJ mol(-1). The relatively high E values are explained by the fact that the MAPA cations are bound to the anionic framework both by electrostatic forces as well as strong N-HaEuro broken vertical bar O hydrogen bonds. The strength of the interactions is indirectly confirmed by the in situ high temperature X-ray diffraction analysis which shows that the MAPA decomposition leads to a phase transformation of the open-framework structure to the dense trydimite phase.
PB  - Springer, Dordrecht
T2  - Journal of Thermal Analysis and Calorimetry
T1  - On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3
EP  - 924
IS  - 3
SP  - 919
VL  - 101
DO  - 10.1007/s10973-009-0504-7
ER  - 
@article{
author = "Rajić, Nevenka and Stojaković, Đorđe and Jevtić, Sanja and Zabukovec-Logar, Nataša and Mali, Gregor and Kaučič, Venčeslav",
year = "2010",
abstract = "An open-framework aluminophosphate analog of the fluorogallophosphate structure-type ULM-3 was obtained by hydrothermal crystallization of an aqueous aluminum phosphate suspension in the presence of 3-methylpropylamine (MAPA) and hydrofluoric acid. The open-framework fluorinated aluminophosphate structure was confirmed by Rietveld analysis and the (27)Al, (31)P, and (19)F MAS NMR spectroscopy. The MAPA, located in the ten-membered ring channels, is doubly protonated to balance the negative charge of the Al(3)P(3)O(12)F(2) (2-) framework. Thermogravimetric analysis data have been used to study kinetics of the thermal decomposition of MAPA. The decomposition was found to be a complex process, its activation energy varied from 177 to 259 kJ mol(-1). The relatively high E values are explained by the fact that the MAPA cations are bound to the anionic framework both by electrostatic forces as well as strong N-HaEuro broken vertical bar O hydrogen bonds. The strength of the interactions is indirectly confirmed by the in situ high temperature X-ray diffraction analysis which shows that the MAPA decomposition leads to a phase transformation of the open-framework structure to the dense trydimite phase.",
publisher = "Springer, Dordrecht",
journal = "Journal of Thermal Analysis and Calorimetry",
title = "On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3",
pages = "924-919",
number = "3",
volume = "101",
doi = "10.1007/s10973-009-0504-7"
}
Rajić, N., Stojaković, Đ., Jevtić, S., Zabukovec-Logar, N., Mali, G.,& Kaučič, V.. (2010). On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3. in Journal of Thermal Analysis and Calorimetry
Springer, Dordrecht., 101(3), 919-924.
https://doi.org/10.1007/s10973-009-0504-7
Rajić N, Stojaković Đ, Jevtić S, Zabukovec-Logar N, Mali G, Kaučič V. On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3. in Journal of Thermal Analysis and Calorimetry. 2010;101(3):919-924.
doi:10.1007/s10973-009-0504-7 .
Rajić, Nevenka, Stojaković, Đorđe, Jevtić, Sanja, Zabukovec-Logar, Nataša, Mali, Gregor, Kaučič, Venčeslav, "On the thermal degradation of 3-methylaminopropylamine captured inside the aluminum phosphate analog of ULM-3" in Journal of Thermal Analysis and Calorimetry, 101, no. 3 (2010):919-924,
https://doi.org/10.1007/s10973-009-0504-7 . .
1
1

Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine

Zabukovec-Logar, Nataša; Mali, Gregor; Rajić, Nevenka; Jevtić, Sanja; Rangus, Mojca; Golobić, Amalija; Kaučič, Venčeslav

(Academic Press Inc Elsevier Science, San Diego, 2010)

TY  - JOUR
AU  - Zabukovec-Logar, Nataša
AU  - Mali, Gregor
AU  - Rajić, Nevenka
AU  - Jevtić, Sanja
AU  - Rangus, Mojca
AU  - Golobić, Amalija
AU  - Kaučič, Venčeslav
PY  - 2010
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/1699
AB  - A single-crystal X-ray diffraction analysis of an open-framework aluminophosphate ULM-3 Al prepared by 3-methylaminopropylamine (MAPA) as structure-directing agent revealed an orthorhombic Pcab symmetry (a=9.9949(4)angstrom, b=15.8229(7)angstrom, c=18.1963(5)angstrom, R=0.0648, Z=8, unit cell formula (Al24P24O96F16 center dot C32H112N16]). which differs from the Pbc2(1) symmetry of the structural analogue prepared in the presence of 1,4-diaminobutane. The Al-27, P-31, F-19, C-13 and H-1 NMR investigations, which were performed to study in detail MAPA arrangement inside the framework as well as the interactions of MAPA with the aluminophosphate host, confirmed the crystal symmetry and the proposed hydrogen bonding scheme between the template and the framework.
PB  - Academic Press Inc Elsevier Science, San Diego
T2  - Journal of Solid State Chemistry
T1  - Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine
EP  - 1062
IS  - 5
SP  - 1055
VL  - 183
DO  - 10.1016/j.jssc.2010.02.020
ER  - 
@article{
author = "Zabukovec-Logar, Nataša and Mali, Gregor and Rajić, Nevenka and Jevtić, Sanja and Rangus, Mojca and Golobić, Amalija and Kaučič, Venčeslav",
year = "2010",
abstract = "A single-crystal X-ray diffraction analysis of an open-framework aluminophosphate ULM-3 Al prepared by 3-methylaminopropylamine (MAPA) as structure-directing agent revealed an orthorhombic Pcab symmetry (a=9.9949(4)angstrom, b=15.8229(7)angstrom, c=18.1963(5)angstrom, R=0.0648, Z=8, unit cell formula (Al24P24O96F16 center dot C32H112N16]). which differs from the Pbc2(1) symmetry of the structural analogue prepared in the presence of 1,4-diaminobutane. The Al-27, P-31, F-19, C-13 and H-1 NMR investigations, which were performed to study in detail MAPA arrangement inside the framework as well as the interactions of MAPA with the aluminophosphate host, confirmed the crystal symmetry and the proposed hydrogen bonding scheme between the template and the framework.",
publisher = "Academic Press Inc Elsevier Science, San Diego",
journal = "Journal of Solid State Chemistry",
title = "Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine",
pages = "1062-1055",
number = "5",
volume = "183",
doi = "10.1016/j.jssc.2010.02.020"
}
Zabukovec-Logar, N., Mali, G., Rajić, N., Jevtić, S., Rangus, M., Golobić, A.,& Kaučič, V.. (2010). Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine. in Journal of Solid State Chemistry
Academic Press Inc Elsevier Science, San Diego., 183(5), 1055-1062.
https://doi.org/10.1016/j.jssc.2010.02.020
Zabukovec-Logar N, Mali G, Rajić N, Jevtić S, Rangus M, Golobić A, Kaučič V. Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine. in Journal of Solid State Chemistry. 2010;183(5):1055-1062.
doi:10.1016/j.jssc.2010.02.020 .
Zabukovec-Logar, Nataša, Mali, Gregor, Rajić, Nevenka, Jevtić, Sanja, Rangus, Mojca, Golobić, Amalija, Kaučič, Venčeslav, "Structure investigation of fluorinated aluminophosphate ULM-3 Al templated by 3-methylaminopropylamine" in Journal of Solid State Chemistry, 183, no. 5 (2010):1055-1062,
https://doi.org/10.1016/j.jssc.2010.02.020 . .
7
8
9

On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates

Rajić, Nevenka; Zabukovec-Logar, Nataša; Mali, Gregor; Stojaković, Đorđe; Kaučič, Venčeslav

(Croatian Chemical Society, 2006)

TY  - JOUR
AU  - Rajić, Nevenka
AU  - Zabukovec-Logar, Nataša
AU  - Mali, Gregor
AU  - Stojaković, Đorđe
AU  - Kaučič, Venčeslav
PY  - 2006
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/859
AB  - Three dicarboxylic acids (oxalic, malonic and terephthalic) were investigated as possible pillars in the formation of metallophosphates with extended structures in the presence of 1,2-diaminopropane (DAP) as a structure-directing agent. Only the oxalate ion was proven to be a suitable building block in the formation of hybrid networks. The terephthalate ion seems to possess the ability to be structurally involved in lattice formation, although not in networks of the hybrid type. The malonate ion in this system showed no propensity towards lattice formation, i.e., malonic acid merely exits as an intercalated species inside the 2-D zincophosphate structure. Different pillar-functioning ability has been attributed to structural differences of the three dicarboxylate ions.
PB  - Croatian Chemical Society
T2  - Croatica Chemica Acta
T1  - On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates
EP  - 193
IS  - 2
SP  - 187
VL  - 79
UR  - https://hdl.handle.net/21.15107/rcub_technorep_859
ER  - 
@article{
author = "Rajić, Nevenka and Zabukovec-Logar, Nataša and Mali, Gregor and Stojaković, Đorđe and Kaučič, Venčeslav",
year = "2006",
abstract = "Three dicarboxylic acids (oxalic, malonic and terephthalic) were investigated as possible pillars in the formation of metallophosphates with extended structures in the presence of 1,2-diaminopropane (DAP) as a structure-directing agent. Only the oxalate ion was proven to be a suitable building block in the formation of hybrid networks. The terephthalate ion seems to possess the ability to be structurally involved in lattice formation, although not in networks of the hybrid type. The malonate ion in this system showed no propensity towards lattice formation, i.e., malonic acid merely exits as an intercalated species inside the 2-D zincophosphate structure. Different pillar-functioning ability has been attributed to structural differences of the three dicarboxylate ions.",
publisher = "Croatian Chemical Society",
journal = "Croatica Chemica Acta",
title = "On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates",
pages = "193-187",
number = "2",
volume = "79",
url = "https://hdl.handle.net/21.15107/rcub_technorep_859"
}
Rajić, N., Zabukovec-Logar, N., Mali, G., Stojaković, Đ.,& Kaučič, V.. (2006). On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates. in Croatica Chemica Acta
Croatian Chemical Society., 79(2), 187-193.
https://hdl.handle.net/21.15107/rcub_technorep_859
Rajić N, Zabukovec-Logar N, Mali G, Stojaković Đ, Kaučič V. On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates. in Croatica Chemica Acta. 2006;79(2):187-193.
https://hdl.handle.net/21.15107/rcub_technorep_859 .
Rajić, Nevenka, Zabukovec-Logar, Nataša, Mali, Gregor, Stojaković, Đorđe, Kaučič, Venčeslav, "On a possible role of dicarboxylate ions in the formation of open-framework metallophosphates" in Croatica Chemica Acta, 79, no. 2 (2006):187-193,
https://hdl.handle.net/21.15107/rcub_technorep_859 .
2
2

New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate

Rajić, Nevenka; Zabukovec-Logar, Nataša; Mali, Gregor; Kaučič, Venčeslav

(Amer Chemical Soc, Washington, 2003)

TY  - JOUR
AU  - Rajić, Nevenka
AU  - Zabukovec-Logar, Nataša
AU  - Mali, Gregor
AU  - Kaučič, Venčeslav
PY  - 2003
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/563
AB  - A new 3-D alumino(oxalato)phosphate, [H3NCH(CH3)CH2NH3](2)[Al4P6O20(OH)(4)(C2O4)(H2O)], consists of aluminophosphate layers which are pillared by oxalate anions. It contains a hybrid 12-membered channel where guest species, diprotonated 1,2-diaminopropane and water molecules, are found. The layers are composed of AlO6, AlO4, and PO4 polyhedra giving double chains, which are interconnected through Al-O-P-O-Al bridges. Oxalate ions are quadridentately bonded by participating in the coordination of AlO6 and by bridging the aluminophosphate layers. The guest species strongly interact with the alumino(oxalato)phosphate layers which is evidenced by solid-state NMR spectroscopy. Crystal data are: triclinic, space group P (1) over bar, a = 8.611(1) Angstrom, b = 9.096(1) Angstrom, c = 11.371(1) Angstrom, alpha = 104.811(1)degrees, beta = 111.368(1)degrees, and gamma = 94.248(1)degrees, V = 787.9(1) Angstrom(3), and R = 0.041.
PB  - Amer Chemical Soc, Washington
T2  - Chemistry of Materials
T1  - New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate
EP  - 1738
IS  - 8
SP  - 1734
VL  - 15
DO  - 10.1021/cm021343u
ER  - 
@article{
author = "Rajić, Nevenka and Zabukovec-Logar, Nataša and Mali, Gregor and Kaučič, Venčeslav",
year = "2003",
abstract = "A new 3-D alumino(oxalato)phosphate, [H3NCH(CH3)CH2NH3](2)[Al4P6O20(OH)(4)(C2O4)(H2O)], consists of aluminophosphate layers which are pillared by oxalate anions. It contains a hybrid 12-membered channel where guest species, diprotonated 1,2-diaminopropane and water molecules, are found. The layers are composed of AlO6, AlO4, and PO4 polyhedra giving double chains, which are interconnected through Al-O-P-O-Al bridges. Oxalate ions are quadridentately bonded by participating in the coordination of AlO6 and by bridging the aluminophosphate layers. The guest species strongly interact with the alumino(oxalato)phosphate layers which is evidenced by solid-state NMR spectroscopy. Crystal data are: triclinic, space group P (1) over bar, a = 8.611(1) Angstrom, b = 9.096(1) Angstrom, c = 11.371(1) Angstrom, alpha = 104.811(1)degrees, beta = 111.368(1)degrees, and gamma = 94.248(1)degrees, V = 787.9(1) Angstrom(3), and R = 0.041.",
publisher = "Amer Chemical Soc, Washington",
journal = "Chemistry of Materials",
title = "New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate",
pages = "1738-1734",
number = "8",
volume = "15",
doi = "10.1021/cm021343u"
}
Rajić, N., Zabukovec-Logar, N., Mali, G.,& Kaučič, V.. (2003). New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate. in Chemistry of Materials
Amer Chemical Soc, Washington., 15(8), 1734-1738.
https://doi.org/10.1021/cm021343u
Rajić N, Zabukovec-Logar N, Mali G, Kaučič V. New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate. in Chemistry of Materials. 2003;15(8):1734-1738.
doi:10.1021/cm021343u .
Rajić, Nevenka, Zabukovec-Logar, Nataša, Mali, Gregor, Kaučič, Venčeslav, "New inorganic-organic hybrid: Synthesis and structural characterization of an alumino(oxalato)phosphate" in Chemistry of Materials, 15, no. 8 (2003):1734-1738,
https://doi.org/10.1021/cm021343u . .
13
19
17

Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid

Mali, Gregor; Rajić, Nevenka; Zabukovec-Logar, Nataša; Kaučič, Venčeslav

(Amer Chemical Soc, Washington, 2003)

TY  - JOUR
AU  - Mali, Gregor
AU  - Rajić, Nevenka
AU  - Zabukovec-Logar, Nataša
AU  - Kaučič, Venčeslav
PY  - 2003
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/533
AB  - Short-range order within a novel aluminophosphate-oxalate hybrid material with the unit cell formula CH2(NH3)CH(NH3)CH3Al4P6O20(OH)(4)(C2O4)H2O was studied by multinuclear solid-state NMR measurements. The C-13, Al-27, and P-31 MAS NMR spectra showed several resonance lines that could not be predicted by the single-crystal X-ray diffraction analysis. The underlying variety of carbon, aluminum, and phosphorus local environments was due to the nonuniform arrangement of the protonated 1,2-diaminopropane species and water molecules residing within the pores of the open-framework material. H-1-- gt C-13 CPMAS NNIR spectrum evidenced that the diaminopropane species either occupied two different positions or were present as two different isomers, which also gave rise to two slightly different deformations of one (P(3)O-4) of the three crystallographically distinct PO4 tetrahedra. One-dimensional H-1 and P-31 MAS and 2D H-1-- gt P-31 CPMAS spectra revealed that the water molecule, occupying a well-defined position within the pore with about 42% abundance, attracted H(2) from the hydroxyl group attached to the P(3) atom and involved the hydrogen atom into a strong hydrogen bond. The displacement of H(2) due to the interaction with the water molecule was determined by measuring H(2)-P(3) distances using H-1-- gt P-31 variable-contact-time CPMAS NMR experiments. As evidenced by Al-27 MAS and 3QMAS NMR spectra, the deformation of the P(3)O-4 tetrahedra by water and diaminopropane species further affected also local environments of the two proximal crystallographically inequivalent aluminum sites Al(1) and Al(2).
PB  - Amer Chemical Soc, Washington
T2  - Journal of Physical Chemistry B
T1  - Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid
EP  - 1292
IS  - 6
SP  - 1286
VL  - 107
DO  - 10.1021/jp026469t
ER  - 
@article{
author = "Mali, Gregor and Rajić, Nevenka and Zabukovec-Logar, Nataša and Kaučič, Venčeslav",
year = "2003",
abstract = "Short-range order within a novel aluminophosphate-oxalate hybrid material with the unit cell formula CH2(NH3)CH(NH3)CH3Al4P6O20(OH)(4)(C2O4)H2O was studied by multinuclear solid-state NMR measurements. The C-13, Al-27, and P-31 MAS NMR spectra showed several resonance lines that could not be predicted by the single-crystal X-ray diffraction analysis. The underlying variety of carbon, aluminum, and phosphorus local environments was due to the nonuniform arrangement of the protonated 1,2-diaminopropane species and water molecules residing within the pores of the open-framework material. H-1-- gt C-13 CPMAS NNIR spectrum evidenced that the diaminopropane species either occupied two different positions or were present as two different isomers, which also gave rise to two slightly different deformations of one (P(3)O-4) of the three crystallographically distinct PO4 tetrahedra. One-dimensional H-1 and P-31 MAS and 2D H-1-- gt P-31 CPMAS spectra revealed that the water molecule, occupying a well-defined position within the pore with about 42% abundance, attracted H(2) from the hydroxyl group attached to the P(3) atom and involved the hydrogen atom into a strong hydrogen bond. The displacement of H(2) due to the interaction with the water molecule was determined by measuring H(2)-P(3) distances using H-1-- gt P-31 variable-contact-time CPMAS NMR experiments. As evidenced by Al-27 MAS and 3QMAS NMR spectra, the deformation of the P(3)O-4 tetrahedra by water and diaminopropane species further affected also local environments of the two proximal crystallographically inequivalent aluminum sites Al(1) and Al(2).",
publisher = "Amer Chemical Soc, Washington",
journal = "Journal of Physical Chemistry B",
title = "Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid",
pages = "1292-1286",
number = "6",
volume = "107",
doi = "10.1021/jp026469t"
}
Mali, G., Rajić, N., Zabukovec-Logar, N.,& Kaučič, V.. (2003). Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid. in Journal of Physical Chemistry B
Amer Chemical Soc, Washington., 107(6), 1286-1292.
https://doi.org/10.1021/jp026469t
Mali G, Rajić N, Zabukovec-Logar N, Kaučič V. Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid. in Journal of Physical Chemistry B. 2003;107(6):1286-1292.
doi:10.1021/jp026469t .
Mali, Gregor, Rajić, Nevenka, Zabukovec-Logar, Nataša, Kaučič, Venčeslav, "Solid-state NMR study of an open-framework aluminophosphate-oxalate hybrid" in Journal of Physical Chemistry B, 107, no. 6 (2003):1286-1292,
https://doi.org/10.1021/jp026469t . .
9
11
11

NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34

Tuel, Alain; Caldarelli, Stefano; Meden, Anton; McCusker, Lynne B.; Baerlocher, Christian Baerlocher; Ristic, Alenka; Rajić, Nevenka; Mali, Gregor; Kaučič, Venčeslav

(American Chemical Society, 2000)

TY  - JOUR
AU  - Tuel, Alain
AU  - Caldarelli, Stefano
AU  - Meden, Anton
AU  - McCusker, Lynne B.
AU  - Baerlocher, Christian Baerlocher
AU  - Ristic, Alenka
AU  - Rajić, Nevenka
AU  - Mali, Gregor
AU  - Kaučič, Venčeslav
PY  - 2000
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/6400
AB  - The triclinic form of AlPO4-34, a microporous aluminophosphate with the chabazite (CHA) topology, adopts a rhombohedral symmetry upon calcination. The framework structure of this phase remains intact under ambient conditions, but it distorts dramatically, though reversibly, in the presence of water. Following these structural changes in situ by X-ray diffraction revealed that there are actually two stable rehydrated phases, which differ from each other by one water molecule in the channel. Both of these phases have triclinic unit cells that are closely related to that of the calcined rhombohedral phase. The structure of the low-temperature (10 °C), fully rehydrated phase (phase B) was elucidated by combining high-resolution synchrotron powder diffraction with solid-state NMR techniques. Coordination of three of the six Al atoms to water molecules causes the deformation of the framework and the reduction of the symmetry. Rietveld refinement of the structure of phase B in the triclinic space group P1 (a = 9.026, b = 9.338, c = 9.508 Å, α = 95.1°, β = 104.1°, and γ = 96.6°) converged with RF = 0.079 and RWP = 0.176 (Rexp = 0.087). Framework connectivities derived from the structure were used to assign 31P NMR lines as well as part of the 27Al NMR signal.
PB  - American Chemical Society
T2  - The Journal of Physical Chemistry B
T1  - NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34
EP  - 5705
SP  - 5697
VL  - 104
DO  - 10.1021/jp000455a
ER  - 
@article{
author = "Tuel, Alain and Caldarelli, Stefano and Meden, Anton and McCusker, Lynne B. and Baerlocher, Christian Baerlocher and Ristic, Alenka and Rajić, Nevenka and Mali, Gregor and Kaučič, Venčeslav",
year = "2000",
abstract = "The triclinic form of AlPO4-34, a microporous aluminophosphate with the chabazite (CHA) topology, adopts a rhombohedral symmetry upon calcination. The framework structure of this phase remains intact under ambient conditions, but it distorts dramatically, though reversibly, in the presence of water. Following these structural changes in situ by X-ray diffraction revealed that there are actually two stable rehydrated phases, which differ from each other by one water molecule in the channel. Both of these phases have triclinic unit cells that are closely related to that of the calcined rhombohedral phase. The structure of the low-temperature (10 °C), fully rehydrated phase (phase B) was elucidated by combining high-resolution synchrotron powder diffraction with solid-state NMR techniques. Coordination of three of the six Al atoms to water molecules causes the deformation of the framework and the reduction of the symmetry. Rietveld refinement of the structure of phase B in the triclinic space group P1 (a = 9.026, b = 9.338, c = 9.508 Å, α = 95.1°, β = 104.1°, and γ = 96.6°) converged with RF = 0.079 and RWP = 0.176 (Rexp = 0.087). Framework connectivities derived from the structure were used to assign 31P NMR lines as well as part of the 27Al NMR signal.",
publisher = "American Chemical Society",
journal = "The Journal of Physical Chemistry B",
title = "NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34",
pages = "5705-5697",
volume = "104",
doi = "10.1021/jp000455a"
}
Tuel, A., Caldarelli, S., Meden, A., McCusker, L. B., Baerlocher, C. B., Ristic, A., Rajić, N., Mali, G.,& Kaučič, V.. (2000). NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34. in The Journal of Physical Chemistry B
American Chemical Society., 104, 5697-5705.
https://doi.org/10.1021/jp000455a
Tuel A, Caldarelli S, Meden A, McCusker LB, Baerlocher CB, Ristic A, Rajić N, Mali G, Kaučič V. NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34. in The Journal of Physical Chemistry B. 2000;104:5697-5705.
doi:10.1021/jp000455a .
Tuel, Alain, Caldarelli, Stefano, Meden, Anton, McCusker, Lynne B., Baerlocher, Christian Baerlocher, Ristic, Alenka, Rajić, Nevenka, Mali, Gregor, Kaučič, Venčeslav, "NMR Characterization and Rietveld Refinement of the Structure of Rehydrated AlPO4-34" in The Journal of Physical Chemistry B, 104 (2000):5697-5705,
https://doi.org/10.1021/jp000455a . .
3
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89