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Methylcellulose-Directed Synthesis of Nanocrystalline Zeolite NaA with High CO2 Uptake
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Luleå University of Technology, Sweden.
2014 (English)In: Materials, ISSN 1996-1944, E-ISSN 1996-1944, Vol. 7, no 8, 5507-5519 p.Article in journal (Refereed) Published
Abstract [en]

Zeolite NaA nanocrystals with a narrow particle size distribution were prepared by template-free hydrothermal synthesis in thermo-reversible methylcellulose gels. The effects of the amount of methylcellulose, crystallization time and hydrothermal treatment temperature on the crystallinity and particle size distribution of the zeolite NaA nanocrystals were investigated. We found that the thermogelation of methylcellulose in the alkaline Na2O-SiO2-Al2O3-H2O system played an important role in controlling the particle size. The synthesized zeolite nanocrystals are highly crystalline, as demonstrated by X-ray diffraction (XRD), and scanning electron microscopy (SEM) shows that the nanocrystals can also display a well-defined facetted morphology. Gas adsorption studies on the synthesized nanocrystalline zeolite NaA showed that nanocrystals with a size of 100 nm displayed a high CO2 uptake capacity (4.9 mmol/g at 293 K at 100 kPa) and a relatively rapid uptake rate compared to commercially available, micron-sized particles. Low-cost nanosized zeolite adsorbents with a high and rapid uptake are important for large scale gas separation processes, e.g., carbon capture from flue gas.

Place, publisher, year, edition, pages
2014. Vol. 7, no 8, 5507-5519 p.
Keyword [en]
zeolite NaA, nanocrystals, hydrothermal synthesis, carbon dioxide adsorption
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-107809DOI: 10.3390/ma7085507ISI: 000341210400006OAI: oai:DiVA.org:su-107809DiVA: diva2:752591
Note

AuthorCount:4;

Available from: 2014-10-05 Created: 2014-09-29 Last updated: 2017-12-05Bibliographically approved
In thesis
1. Processing and performance of zeolites for efficient carbon dioxide separation
Open this publication in new window or tab >>Processing and performance of zeolites for efficient carbon dioxide separation
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

We have structured zeolites from powders of zeolite 13X and 4A into hierarchically porous monoliths for efficient carbon dioxide capture by tailoring the pore dimensions to facilitate rapid gas uptake and release. Freeze-casting was used for the first time to shape adsorbents into a lamellar structure. Lamellar walls with thicknesses and spacing in the range of 10 µm were found to be the best combination between rapid gas transport and a short diffusion distance in the zeolite-containing walls for rapid carbon dioxide uptake and release.

Compressive strength measurements of the freeze-cast zeolite-based monoliths showed that monoliths with small pores, thin walls and a lot of interconnectivity between the walls were stronger than monoliths with large pores and thick walls. Image analysis of the structures together with modelling of the deformation behavior suggests that the failure mechanism of freeze-cast monoliths is dominated by buckling.

Binder-free zeolite Y and ZSM-5 -based monoliths were produced by pulsed current processing (PCP) into strong, hierarchically porous monoliths with minimal loss of crystallinity. Ranges for the maximum PCP processing temperatures for the zeolites with different aluminium contents were identified by powder x-ray diffraction (PXRD) with full-profile fitting analysis.

Matching the thermal expansion behavior of the supports with the zeolite film is important to minimize the risk of thermally induced cracking of zeolite membranes. Zeolite supports with a macroporous structure was prepared by PCP and the thermal expansion coefficient was determined by PXRD and compared to traditional alumina substrates. It was found that the slightly negative thermal expansion coefficient of the zeolite supports matched the thermal expansion of the zeolite films very well, whereas the alumina support would induce large stresses upon fluctuating temperatures.

Methylcellulose-directed synthesis of zeolite 4A produced nano-sized crystals with a narrow size distribution, which could be tuned by adjusting the methylcellulose content. The crystallinity of the synthesized 4A was controlled by PXRD and found to be very high, and the gas uptake capability performed well in comparison with available micron-sized zeolites.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2015. 69 p.
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-114160 (URN)978-91-7649-107-2 (ISBN)
Public defence
2015-03-27, Magnéli Hall, Arrhenius Laboratory, Svante Arrhenius Väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Funder
Berzelii Centre EXSELENT
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 2: Submitted.

Available from: 2015-03-05 Created: 2015-02-23 Last updated: 2015-12-02Bibliographically approved

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