Abstract
Extra-large-pore aluminogermanosilicate zeolite IRR with interconnected 18 × 12 × 12-ring channels was prepared within a wide range of Si/Ge and Al/(Si+Ge) ratio by using a new simple and commercial alkyl-immidazolium as template. The physicochemical properties of IRR zeolite were further characterized by the combination of several techniques, including XRD, SEM, NMR, TGA, ICP, N2 physisorption, NH3-TPD etc. The results revealed that aluminum could be mostly incorporated in the framework with an obviously higher content as a result of the relatively smaller organic template used in this approach. The detemplated IRR by calcination at 550 °C in air presented excellent microporosity with the presence of 18-ring extra-large-pore opening, and considerable amount of acid sites with strong acidity. Finally, for the first time the catalytic performance of IRR zeolite, in comparison with large-pore Beta (12 × 12 × 12-ring) and extra-large-pore NUD-1 (18 × 12 × 12-ring) zeolites, were evaluated for acetalization reaction of aldehydes with triethyl ortoformate. The results showed that the catalytic activity of these three zeolites for aldehydes with different molecular size, that is heptanal and diphenylacetaldehyde, were in diametrically opposite order. IRR exhibited the highest catalytic conversion on bulky substrate diphenylacetaldehyde because its much more open channel system better facilitated the diffusion of reactants into the structure interior, where active acidic sites were located.
Similar content being viewed by others
References
J. Jiang, J. Yu, A. Corma, Angew Chem. Int. Ed. 49, 3120–3145 (2010)
J. Wen, J. Zhang, J. Jiang, Chem. J. Chinese U 42, 101–116 (2021)
M. Moliner, M. Diazcabanas, V. Fornes, C. Martinez, A. Corma, J. Catal. 254, 101–109 (2008)
IZA Structure Commission Website: www.iza-structure.org/databases
Y. Wei, Z. Tian, H. Gies, R. Xu, H. Ma, R. Pei, W. Zhang, Y. Xu, L. Wang, K. Li, B. Wang, G. Wen, L. Lin, Angew Chem. Int. Ed. 49, 5367–5370 (2010)
T. Willhammar, A.W. Burton, Y. Yun, J. Sun, M. Afeworki, K.G. Strohmaier, H. Vroman, X. Zou, J. Am. Chem. Soc. 136, 13570–13573 (2014)
Y. Yun, M. Hernandez, W. Wan, X. Zou, J.L. Jorda, A. Cantin, F. Rey, A. Corma, Chem. Commun. 51, 7602–7605 (2015)
J. Jiang, Y. Yun, X. Zou, J.L. Jorda, A. Corma, Chem. Sci. 6, 480–485 (2015)
A. Corma, M.J. Diaz-Cabanas, J. Jiang, M. Afeworki, D.L. Dorset, S.L. Soled, K.G. Strohmaier, Proc. Natl. Acad. Sci. U. S. A. 107, 13997–14002 (2010)
J. Sun, C. Bonneau, A. Cantin, A. Corma, M.J. Diaz-Cabanas, M. Moliner, D. Zhang, M. Li, X. Zou, Nature. 458, 1154–1157 (2009)
J. Jiang, J.L. Jorda, J. Yu, L.A. Baumes, E. Mugnaioli, M.J. Diaz-Cabanas, U. Kolb, A. Corma, Science. 333, 1131–1134 (2011)
Q. Lin, Z. Gao, C. Lin, S. Zhang, J. Chen, Z. Li, X. Liu, W. Fan, J. Li, X. Chen, M.A. Camblor, F. Chen, Science. 374, 1605–1608 (2021)
J. Jiang, J.L. Jorda, M.J. Diaz-Cabanas, J. Yu, A. Corma, Angew Chem. Int. Ed. 49, 4986–4988 (2010)
K. Qian, Y. Wang, Z. Liang, J. Li, RSC Adv. 5, 63209–63214 (2015)
R. Bai, Q. Sun, N. Wang, Y. Zou, G. Guo, S. Iborra, A. Corma, J. Yu, Chem. Mater. 28, 6455–6458 (2016)
M. Wang, L. Zhang, K. Guo, Y. Lin, X. Meng, P. Huang, Y. Wei, R. Zhang, Chem. Asian J. 14, 621–626 (2019)
X. Hou, Z. Yao, H. Li, M. Wang, Y. Wei, L. Zhang, Y. Liang, J. Qiao, J. Jia, R. Zhang, Microporous Mesoporous Mater. 348, 112340 (2023)
P.S. Petkov, H.A. Aleksandrov, V. Valtchev, G.N. Vayssilov, Chem. Mater. 24, 2509–2518 (2012)
G.V. Gibbs, M.B. Boisen, F.C. Hill, O. Tamada, R.T. Downs, Phys. Chem. Miner. 25, 574–584 (1998)
Y. Lin, L. Zhang, K. Guo, M. Wang, Y. Wei, Chem. Eur. J. 24, 2410–2417 (2018)
M.J. Climent, A. Corma, A. Velty, M. Susarte, J. Catal. 196, 345–351 (2000)
M.J. Climent, A. Corma, A. Velty, Appl. Catal. A Gen. 263, 155–161 (2004)
F. Chen, Y. Xu, H. Du, Angew Chem. Int. Ed. 53, 9592–9596 (2014)
Acknowledgements
The authors thank the financial support from Natural Science Foundation of Beijing Municipality (No. 2182048) and Fundamental Research Funds for the Central Universities (No. JD2213 and XK1802-1).
Author information
Authors and Affiliations
Contributions
HL: Investigation, Formal analysis, Data curation. XH: Data curation. LZ: Validation, Methodology. YW: Writing—review & editing, Supervision, Funding acquisition, Conceptualization. YL: Validation, Formal analysis. JQ: Validation, Investigation. HS: Validation, Investigation. XG: Validation, Investigation. JJ: Visualization, Software. RZ: Resources, Funding acquisition.
Corresponding author
Ethics declarations
Conflict of interest
The authors declare no conflict of interest.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Li, H., Hou, X., Zhang, L. et al. Alkyl-imidazolium templating synthesis to extra-large-pore aluminogermanosilicate zeolite IRR with enhanced Al substitution and excellent catalytic performance in bulky molecule acetalization. J Porous Mater 30, 1311–1318 (2023). https://doi.org/10.1007/s10934-023-01422-6
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10934-023-01422-6