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Laminated Adsorbents with Very Rapid CO2 Uptake by Freeze-Casting of Zeolites
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).
2013 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 5, no 7, 2669-2676 p.Article in journal (Refereed) Published
Abstract [en]

Structured zeolite 13X monoliths with a laminated structure and hierarchical macro-/microporosity were prepared by freeze-casting aqueous suspensions of zeolite 13X powder, bentonite, and polyethylene glycol. Colloidally stable suspensions with a low viscosity at both room temperature and near freezing could be prepared at alkaline conditions where both the zeolite 13X powder and bentonite carry a negative surface charge. Slow directional freezing of the suspensions led to the formation of well-defined and thin lamellar pores and pore walls while fast freezing resulted in more cylindrical pores. The wall thickness, which varied between 8 and 35 mu m, increased with increasing solids loading of the suspension. Thermal treatment at 1053 K of the freeze-cast bodies containing between 9 and 17 wt % bentonite resulted in mechanically stable zeolite 13X monoliths. The monoliths displayed a carbon dioxide uptake capacity of 4-5 mmol/g and an uptake kinetics characterized by a very fast initial uptake where more than 50% of the maximum uptake was reached within 15 s. Freeze-cast laminated zeolite monoliths could be used to improve the volumetric efficiency and reduce the cycle time, of importance in, for example, biogas upgrading and CO2 separation from flue gas.

Place, publisher, year, edition, pages
2013. Vol. 5, no 7, 2669-2676 p.
Keyword [en]
freeze-casting, zeolite 13X, shaping, structured, laminate, adsorbent, hierarchical, carbon dioxide, CCS, gas separation, uptake kinetics
National Category
Nano Technology Materials Engineering
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-90187DOI: 10.1021/am400122rISI: 000317549100051OAI: oai:DiVA.org:su-90187DiVA: diva2:623823
Note

AuthorCount:4;

Available from: 2013-05-28 Created: 2013-05-28 Last updated: 2017-12-06Bibliographically 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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