Unveiling the elusive role of tetraethyl orthosilicate hydrolysis in ionic-liquid-templated zeolite synthesis

X. Li; T. H. Li; W. Zhou; Y. P. Li; P. H.L. Sit; Z. Wu; O. J. Curnow; K. C.W. Wu; J. Choi; A. C.K. Yip

doi:10.1016/j.mtchem.2021.100658

Unveiling the elusive role of tetraethyl orthosilicate hydrolysis in ionic-liquid-templated zeolite synthesis

X. Li, T. H. Li, W. Zhou, Y. P. Li, P. H.L. Sit, Z. Wu, O. J. Curnow, K. C.W. Wu, J. Choi, A. C.K. Yip

Department of Chemical and Biological Engineering

Research output: Contribution to journal › Article › peer-review

3 Citations (Scopus)

Abstract

Despite previous reports showing that crystallization kinetics affects zeolite phase selectivity because zeolites are metastable species in their synthesis solution rather than thermodynamic end points, the critical kinetics-controlling parameter is yet to be determined. This work elucidated the effect of tetraethyl orthosilicate (TEOS) hydrolysis before hydrothermal treatment on the final zeolite phase selectivity in the ionic liquid-templated synthesis of 10-membered ring zeolites (MFI- or TON-type zeolites). The results showed that the dissolved silica concentration in the synthesis solution, which is controlled by varying the TEOS hydrolysis temperature and addition rate, induced heterogeneous nuclear growth. Specifically, in 1-butyl-3-methylimidazolium ([BMIM]Br)-directed syntheses, the high and low concentrations of dissolved silica species led to MFI and TON zeolite formation, respectively. The experimental results are supported by silica polymerization modeling using the Reaction Ensemble Monte Carlo method and theoretical calculations on composite building unit formation. The results are valuable for understanding the nucleation mechanism in zeolite crystallization.

Original language	English
Article number	100658
Journal	Materials Today Chemistry
Volume	23
DOIs	https://doi.org/10.1016/j.mtchem.2021.100658
Publication status	Published - 2022 Mar

Keywords

Ionic liquids
MFI
TEOS·hydrolysis
TON
Zeolites

ASJC Scopus subject areas

Catalysis
Electronic, Optical and Magnetic Materials
Biomaterials
Polymers and Plastics
Colloid and Surface Chemistry
Materials Chemistry

Access to Document

10.1016/j.mtchem.2021.100658

Cite this

@article{fb08bcde7b074e3aa3a2751cb34decc2,

title = "Unveiling the elusive role of tetraethyl orthosilicate hydrolysis in ionic-liquid-templated zeolite synthesis",

abstract = "Despite previous reports showing that crystallization kinetics affects zeolite phase selectivity because zeolites are metastable species in their synthesis solution rather than thermodynamic end points, the critical kinetics-controlling parameter is yet to be determined. This work elucidated the effect of tetraethyl orthosilicate (TEOS) hydrolysis before hydrothermal treatment on the final zeolite phase selectivity in the ionic liquid-templated synthesis of 10-membered ring zeolites (MFI- or TON-type zeolites). The results showed that the dissolved silica concentration in the synthesis solution, which is controlled by varying the TEOS hydrolysis temperature and addition rate, induced heterogeneous nuclear growth. Specifically, in 1-butyl-3-methylimidazolium ([BMIM]Br)-directed syntheses, the high and low concentrations of dissolved silica species led to MFI and TON zeolite formation, respectively. The experimental results are supported by silica polymerization modeling using the Reaction Ensemble Monte Carlo method and theoretical calculations on composite building unit formation. The results are valuable for understanding the nucleation mechanism in zeolite crystallization.",

keywords = "Ionic liquids, MFI, TEOS·hydrolysis, TON, Zeolites",

author = "X. Li and Li, {T. H.} and W. Zhou and Li, {Y. P.} and Sit, {P. H.L.} and Z. Wu and Curnow, {O. J.} and Wu, {K. C.W.} and J. Choi and Yip, {A. C.K.}",

note = "Funding Information: The authors would like to thank the China Scholarship Council for supporting this work through the doctoral scholarship to Xuemin Li. The authors also acknowledge financial support from the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT ( 2018M3D3A1A01018004 ) and the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant ( UOCX1905 ). Publisher Copyright: {\textcopyright} 2021 Elsevier Ltd",

year = "2022",

month = mar,

doi = "10.1016/j.mtchem.2021.100658",

language = "English",

volume = "23",

journal = "Materials Today Chemistry",

issn = "2468-5194",

publisher = "Elsevier Limited",

}

TY - JOUR

T1 - Unveiling the elusive role of tetraethyl orthosilicate hydrolysis in ionic-liquid-templated zeolite synthesis

AU - Li, X.

AU - Li, T. H.

AU - Zhou, W.

AU - Li, Y. P.

AU - Sit, P. H.L.

AU - Wu, Z.

AU - Curnow, O. J.

AU - Wu, K. C.W.

AU - Choi, J.

AU - Yip, A. C.K.

N1 - Funding Information: The authors would like to thank the China Scholarship Council for supporting this work through the doctoral scholarship to Xuemin Li. The authors also acknowledge financial support from the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT ( 2018M3D3A1A01018004 ) and the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant ( UOCX1905 ). Publisher Copyright: © 2021 Elsevier Ltd

PY - 2022/3

Y1 - 2022/3

N2 - Despite previous reports showing that crystallization kinetics affects zeolite phase selectivity because zeolites are metastable species in their synthesis solution rather than thermodynamic end points, the critical kinetics-controlling parameter is yet to be determined. This work elucidated the effect of tetraethyl orthosilicate (TEOS) hydrolysis before hydrothermal treatment on the final zeolite phase selectivity in the ionic liquid-templated synthesis of 10-membered ring zeolites (MFI- or TON-type zeolites). The results showed that the dissolved silica concentration in the synthesis solution, which is controlled by varying the TEOS hydrolysis temperature and addition rate, induced heterogeneous nuclear growth. Specifically, in 1-butyl-3-methylimidazolium ([BMIM]Br)-directed syntheses, the high and low concentrations of dissolved silica species led to MFI and TON zeolite formation, respectively. The experimental results are supported by silica polymerization modeling using the Reaction Ensemble Monte Carlo method and theoretical calculations on composite building unit formation. The results are valuable for understanding the nucleation mechanism in zeolite crystallization.

AB - Despite previous reports showing that crystallization kinetics affects zeolite phase selectivity because zeolites are metastable species in their synthesis solution rather than thermodynamic end points, the critical kinetics-controlling parameter is yet to be determined. This work elucidated the effect of tetraethyl orthosilicate (TEOS) hydrolysis before hydrothermal treatment on the final zeolite phase selectivity in the ionic liquid-templated synthesis of 10-membered ring zeolites (MFI- or TON-type zeolites). The results showed that the dissolved silica concentration in the synthesis solution, which is controlled by varying the TEOS hydrolysis temperature and addition rate, induced heterogeneous nuclear growth. Specifically, in 1-butyl-3-methylimidazolium ([BMIM]Br)-directed syntheses, the high and low concentrations of dissolved silica species led to MFI and TON zeolite formation, respectively. The experimental results are supported by silica polymerization modeling using the Reaction Ensemble Monte Carlo method and theoretical calculations on composite building unit formation. The results are valuable for understanding the nucleation mechanism in zeolite crystallization.

KW - Ionic liquids

KW - MFI

KW - TEOS·hydrolysis

KW - TON

KW - Zeolites

UR - http://www.scopus.com/inward/record.url?scp=85119901307&partnerID=8YFLogxK

U2 - 10.1016/j.mtchem.2021.100658

DO - 10.1016/j.mtchem.2021.100658

M3 - Article

AN - SCOPUS:85119901307

SN - 2468-5194

VL - 23

JO - Materials Today Chemistry

JF - Materials Today Chemistry

M1 - 100658

ER -

Unveiling the elusive role of tetraethyl orthosilicate hydrolysis in ionic-liquid-templated zeolite synthesis

Abstract

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this