Highly porous hybrid metallosilicate materials prepared by
non-hydrolytic sol-gel: Hydrothermal stability and catalytic
properties in ethanol dehydration

J 2020

Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration

STÝSKALÍK, Aleš, Imene KORDOGHLI, Claude POLEUNIS, Arnaud DELCORTE, Carmela APRILE et. al.

Základní údaje

Originální název

Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration

Autoři

STÝSKALÍK, Aleš (203 Česká republika, garant, domácí), Imene KORDOGHLI, Claude POLEUNIS, Arnaud DELCORTE, Carmela APRILE, Luca FUSARO a Damien P. DEBECKER

Vydání

Microporous and Mesoporous Materials, Amsterdam, Elsevier, 2020, 1387-1811

Další údaje

Jazyk

angličtina

Typ výsledku

Článek v odborném periodiku

Obor

10402 Inorganic and nuclear chemistry

Stát vydavatele

Nizozemské království

Utajení

není předmětem státního či obchodního tajemství

Odkazy

URL

Impakt faktor

Impact factor: 5.455

Kód RIV

RIV/00216224:14310/20:00116885

Organizační jednotka

Přírodovědecká fakulta

DOI

http://dx.doi.org/10.1016/j.micromeso.2020.110028

UT WoS

000517854500005

Klíčová slova anglicky

Non-hydrolytic sol-gel; Hybrid metallosilicate; Hydrothermal stability; Heterogeneous catalysis; Ethanol dehydration

Štítky

CF CRYO, CF SAXS, rivok

Příznaky

Mezinárodní význam, Recenzováno

Změněno: 14. 10. 2024 15:30, Ing. Marie Švancarová

Anotace

V originále

Herein, we present novel phenylene- and xylylene-bridged silica and metallosilicate materials prepared by non-hydrolytic sol-gel. The hybrid silica are highly porous, chemically similar to periodic mesoporous organosilica (PMO), but amorphous without any pore ordering. Analogous hybrid metallosilicates are obtained by directly incorporating Al, Nb, or Sn in the hybrid silica framework. Exhibiting open texture, surface acidity and tunable hydrophobicity, these materials are excellent candidates for catalytic alcohol dehydration reactions. The gas-phase hydrothermal and thermal stability of these materials is examined. While the hybrid silica is expectedly stable, a stark decrease in stability is observed for phenylene bridged silsesquioxanes upon metal introduction. The extent of the hydrolytic Si-C(sp(2)) bond cleavage is quantitatively followed by Si-29 MAS NMR, TG analysis, and GC-FID analysis of effluent coming from samples exposed to water vapor. Two important features affecting the hydrothermal and thermal stability are identified: (i) the homogeneity of metal dispersion within the silica matrix, and (ii) the electronegativity of the incorporated metal. The stability of hybrid metallosilicates is significantly improved by replacing the phenylene bridges with xylylene bridges, due to the presence of more stable Si-C(sp(3)) bonds. Interestingly, the latter hybrid metallosilicate proves to be an active catalyst for the dehydration of ethanol to ethylene. Unlike the other hybrid materials presented here, it reaches high ethylene yields without undergoing degradation and deactivation.

Návaznosti

LQ1601, projekt VaV

Název: CEITEC 2020 (Akronym: CEITEC2020)

Investor: Ministerstvo školství, mládeže a tělovýchovy ČR, CEITEC 2020

90043, velká výzkumná infrastruktura

Název: CIISB

Citovat

STÝSKALÍK, Aleš, Imene KORDOGHLI, Claude POLEUNIS, Arnaud DELCORTE, Carmela APRILE, Luca FUSARO a Damien P. DEBECKER. Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration. Microporous and Mesoporous Materials. Amsterdam: Elsevier, 2020, roč. 297, MAY 1 2020, s. 1-13. ISSN 1387-1811. Dostupné z: https://dx.doi.org/10.1016/j.micromeso.2020.110028.

@article{1691036,
   author = {Stýskalík, Aleš and Kordoghli, Imene and Poleunis, Claude and Delcorte, Arnaud and Aprile, Carmela and Fusaro, Luca and Debecker, Damien P.},
   article_location = {Amsterdam},
   article_number = {MAY 1 2020},
   doi = {http://dx.doi.org/10.1016/j.micromeso.2020.110028},
   keywords = {Non-hydrolytic sol-gel; Hybrid metallosilicate; Hydrothermal stability; Heterogeneous catalysis; Ethanol dehydration},
   language = {eng},
   issn = {1387-1811},
   journal = {Microporous and Mesoporous Materials},
   title = {Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration},
   url = {https://doi.org/10.1016/j.micromeso.2020.110028},
   volume = {297},
   year = {2020}
}

TY  - JOUR
ID  - 1691036
AU  - Stýskalík, Aleš - Kordoghli, Imene - Poleunis, Claude - Delcorte, Arnaud - Aprile, Carmela - Fusaro, Luca - Debecker, Damien P.
PY  - 2020
TI  - Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration
JF  - Microporous and Mesoporous Materials
VL  - 297
IS  - MAY 1 2020
SP  - 1-13
EP  - 1-13
PB  - Elsevier
SN  - 13871811
KW  - Non-hydrolytic sol-gel
KW  - Hybrid metallosilicate
KW  - Hydrothermal stability
KW  - Heterogeneous catalysis
KW  - Ethanol dehydration
UR  - https://doi.org/10.1016/j.micromeso.2020.110028
L2  - https://doi.org/10.1016/j.micromeso.2020.110028
N2  - Herein, we present novel phenylene- and xylylene-bridged silica and metallosilicate materials prepared by non-hydrolytic sol-gel. The hybrid silica are highly porous, chemically similar to periodic mesoporous organosilica (PMO), but amorphous without any pore ordering. Analogous hybrid metallosilicates are obtained by directly incorporating Al, Nb, or Sn in the hybrid silica framework. Exhibiting open texture, surface acidity and tunable hydrophobicity, these materials are excellent candidates for catalytic alcohol dehydration reactions. The gas-phase hydrothermal and thermal stability of these materials is examined. While the hybrid silica is expectedly stable, a stark decrease in stability is observed for phenylene bridged silsesquioxanes upon metal introduction. The extent of the hydrolytic Si-C(sp(2)) bond cleavage is quantitatively followed by Si-29 MAS NMR, TG analysis, and GC-FID analysis of effluent coming from samples exposed to water vapor. Two important features affecting the hydrothermal and thermal stability are identified: (i) the homogeneity of metal dispersion within the silica matrix, and (ii) the electronegativity of the incorporated metal. The stability of hybrid metallosilicates is significantly improved by replacing the phenylene bridges with xylylene bridges, due to the presence of more stable Si-C(sp(3)) bonds. Interestingly, the latter hybrid metallosilicate proves to be an active catalyst for the dehydration of ethanol to ethylene. Unlike the other hybrid materials presented here, it reaches high ethylene yields without undergoing degradation and deactivation.
ER  -

STÝSKALÍK, Aleš, Imene KORDOGHLI, Claude POLEUNIS, Arnaud DELCORTE, Carmela APRILE, Luca FUSARO a Damien P. DEBECKER. Highly porous hybrid metallosilicate materials prepared by non-hydrolytic sol-gel: Hydrothermal stability and catalytic properties in ethanol dehydration. \textit{Microporous and Mesoporous Materials}. Amsterdam: Elsevier, 2020, roč.~297, MAY 1 2020, s.~1-13. ISSN~1387-1811. Dostupné z: https://dx.doi.org/10.1016/j.micromeso.2020.110028.

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