Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO2 Cycloaddition with Epichlorohydrin

Jose J. Delgado-Marín; Alejandra Rendón-Patiño; Vijay Kumar Velisoju; Gadde Sathish Kumar; Naydu Zambrano; Magnus Rueping; Jorge Gascón; Pedro Castaño; Javier Narciso; Enrique V. Ramos-Fernandez

doi:10.1021/acs.chemmater.2c03374

Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO₂ Cycloaddition with Epichlorohydrin

Jose J. Delgado-Marín, Alejandra Rendón-Patiño, Vijay Kumar Velisoju, Gadde Sathish Kumar, Naydu Zambrano, Magnus Rueping, Jorge Gascón, Pedro Castaño, Javier Narciso, Enrique V. Ramos-Fernandez^*

^*Corresponding author for this work

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

15 Scopus citations

Abstract

Zeolitic imidazolate frameworks (ZIFs) have been profusely used as catalysts for inserting CO₂ into organic epoxides (i.e., epichlorohydrin) through cycloaddition. Here, we demonstrate that these materials suffer from irreversible degradation by leaching. To prove this, we performed the reactions and analyzed the final reaction mixtures by elemental analysis and the resulting materials by different microscopies. We found that the difference in catalytic activity between three ZIF-67 and one ZIF-L catalysts was related to the rate at which the materials degraded. Particularly, the {100} facet leaches faster than the others, regardless of the material used. The catalytic activity strongly depended on the amount of leached elements in the liquid phase since these species are extremely active. Our work points to the instability of these materials under relevant reaction conditions and the necessity of additional treatments to improve their stability.

Original language	English (US)
Pages (from-to)	692-699
Number of pages	8
Journal	Chemistry of Materials
Volume	35
Issue number	2
DOIs	https://doi.org/10.1021/acs.chemmater.2c03374
State	Published - Jan 24 2023

Bibliographical note

Funding Information:
The authors acknowledge financial support by Ministerio de Ciencia e Innovación (PID2020-116998RB-I00), Ministerio de Educación y Formación Profesional (PRX21/00407), Conselleria de Innovacion, Universidades, Ciencia y Sociedad Digital (CIPROM/2021/022 and MFA/2022/057), and the King Abdullah University of Science and Technology (KAUST). This study forms part of the Advanced Materials Program and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and by Generalitat Valenciana

Publisher Copyright:
© 2023 American Chemical Society.

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering
Materials Chemistry

Access to Document

10.1021/acs.chemmater.2c03374

Cite this

Delgado-Marín, J. J., Rendón-Patiño, A., Velisoju, V. K., Kumar, G. S., Zambrano, N., Rueping, M., Gascón, J., Castaño, P., Narciso, J., & Ramos-Fernandez, E. V. (2023). Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO₂ Cycloaddition with Epichlorohydrin. Chemistry of Materials, 35(2), 692-699. https://doi.org/10.1021/acs.chemmater.2c03374

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title = "Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO2 Cycloaddition with Epichlorohydrin",

abstract = "Zeolitic imidazolate frameworks (ZIFs) have been profusely used as catalysts for inserting CO2 into organic epoxides (i.e., epichlorohydrin) through cycloaddition. Here, we demonstrate that these materials suffer from irreversible degradation by leaching. To prove this, we performed the reactions and analyzed the final reaction mixtures by elemental analysis and the resulting materials by different microscopies. We found that the difference in catalytic activity between three ZIF-67 and one ZIF-L catalysts was related to the rate at which the materials degraded. Particularly, the {100} facet leaches faster than the others, regardless of the material used. The catalytic activity strongly depended on the amount of leached elements in the liquid phase since these species are extremely active. Our work points to the instability of these materials under relevant reaction conditions and the necessity of additional treatments to improve their stability.",

author = "Delgado-Mar{\'i}n, {Jose J.} and Alejandra Rend{\'o}n-Pati{\~n}o and Velisoju, {Vijay Kumar} and Kumar, {Gadde Sathish} and Naydu Zambrano and Magnus Rueping and Jorge Gasc{\'o}n and Pedro Casta{\~n}o and Javier Narciso and Ramos-Fernandez, {Enrique V.}",

note = "Funding Information: The authors acknowledge financial support by Ministerio de Ciencia e Innovaci{\'o}n (PID2020-116998RB-I00), Ministerio de Educaci{\'o}n y Formaci{\'o}n Profesional (PRX21/00407), Conselleria de Innovacion, Universidades, Ciencia y Sociedad Digital (CIPROM/2021/022 and MFA/2022/057), and the King Abdullah University of Science and Technology (KAUST). This study forms part of the Advanced Materials Program and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and by Generalitat Valenciana Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

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Delgado-Marín, JJ, Rendón-Patiño, A , Velisoju, VK, Kumar, GS, Zambrano, N, Rueping, M , Gascón, J , Castaño, P, Narciso, J & Ramos-Fernandez, EV 2023, 'Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO₂ Cycloaddition with Epichlorohydrin', Chemistry of Materials, vol. 35, no. 2, pp. 692-699. https://doi.org/10.1021/acs.chemmater.2c03374

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T1 - Leaching in Specific Facets of ZIF-67 and ZIF-L Zeolitic Imidazolate Frameworks During the CO2 Cycloaddition with Epichlorohydrin

AU - Delgado-Marín, Jose J.

AU - Rendón-Patiño, Alejandra

AU - Velisoju, Vijay Kumar

AU - Kumar, Gadde Sathish

AU - Zambrano, Naydu

AU - Rueping, Magnus

AU - Gascón, Jorge

AU - Castaño, Pedro

AU - Narciso, Javier

AU - Ramos-Fernandez, Enrique V.

N1 - Funding Information: The authors acknowledge financial support by Ministerio de Ciencia e Innovación (PID2020-116998RB-I00), Ministerio de Educación y Formación Profesional (PRX21/00407), Conselleria de Innovacion, Universidades, Ciencia y Sociedad Digital (CIPROM/2021/022 and MFA/2022/057), and the King Abdullah University of Science and Technology (KAUST). This study forms part of the Advanced Materials Program and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and by Generalitat Valenciana Publisher Copyright: © 2023 American Chemical Society.

PY - 2023/1/24

Y1 - 2023/1/24

N2 - Zeolitic imidazolate frameworks (ZIFs) have been profusely used as catalysts for inserting CO2 into organic epoxides (i.e., epichlorohydrin) through cycloaddition. Here, we demonstrate that these materials suffer from irreversible degradation by leaching. To prove this, we performed the reactions and analyzed the final reaction mixtures by elemental analysis and the resulting materials by different microscopies. We found that the difference in catalytic activity between three ZIF-67 and one ZIF-L catalysts was related to the rate at which the materials degraded. Particularly, the {100} facet leaches faster than the others, regardless of the material used. The catalytic activity strongly depended on the amount of leached elements in the liquid phase since these species are extremely active. Our work points to the instability of these materials under relevant reaction conditions and the necessity of additional treatments to improve their stability.

AB - Zeolitic imidazolate frameworks (ZIFs) have been profusely used as catalysts for inserting CO2 into organic epoxides (i.e., epichlorohydrin) through cycloaddition. Here, we demonstrate that these materials suffer from irreversible degradation by leaching. To prove this, we performed the reactions and analyzed the final reaction mixtures by elemental analysis and the resulting materials by different microscopies. We found that the difference in catalytic activity between three ZIF-67 and one ZIF-L catalysts was related to the rate at which the materials degraded. Particularly, the {100} facet leaches faster than the others, regardless of the material used. The catalytic activity strongly depended on the amount of leached elements in the liquid phase since these species are extremely active. Our work points to the instability of these materials under relevant reaction conditions and the necessity of additional treatments to improve their stability.

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