Bamiduro, F orcid.org/0000-0002-1914-5731, Guozhao, J, Brown, AP orcid.org/0000-0001-9692-2154 et al. (3 more authors) (2017) Spray-Dried Sodium Zirconate: A Rapid Absorption Powder for CO2 Capture with Enhanced Cyclic Stability. ChemSusChem, 10 (9). pp. 2059-2067. ISSN 1864-5631
Abstract
Improved powders for capturing CO2 at high temperatures are required for H2 production using sorption-enhanced steam reforming. Here, we examine the relationship between particle structure and carbonation rate for two types of Na2ZrO3 powders. Hollow spray-dried microgranules with a wall thickness of 100–300 nm corresponding to the dimensions of the primary acetate-derived particles gave about 75 wt % theoretical CO2 conversion after a process-relevant 5 min exposure to 15 vol % CO2. A conventional powder prepared by solid-state reaction carbonated more slowly, achieving only 50 % conversion owing to a greater proportion of the reaction requiring bulk diffusion through the densely agglomerated particles. The hollow granular structure of the spray-dried powder was retained postcarbonation but chemical segregation resulted in islands of an amorphous Na-rich phase (Na2CO3) within a crystalline ZrO2 particle matrix. Despite this phase separation, the reverse reaction to re-form Na2ZrO3 could be achieved by heating each powder to 900 °C in N2 (no dwell time). This resulted in a very stable multicycle performance in 40 cycle tests using thermogravimetric analysis for both powders. Kinetic analysis of thermogravimetric data showed the carbonation process fits an Avrami–Erofeyev 2 D nucleation and nuclei growth model, consistent with microstructural evidence of a surface-driven transformation. Thus, we demonstrate that spray drying is a viable processing route to enhance the carbon capture performance of Na2ZrO3 powder.
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Copyright, Publisher and Additional Information: | (c) 2017, Wiley. This is the peer reviewed version of the following article: Bamiduro, F , Guozhao, J, Brown, AP et al. (3 more authors) (2017) Spray-Dried Sodium Zirconate: A Rapid Absorption Powder for CO2 Capture with Enhanced Cyclic Stability. ChemSusChem, 10 (9). pp. 2059-2067., which has been published in final form at https://doi.org/10.1002/cssc.201700046. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. | ||||||||||||||||||||||||||||||||||||||
Keywords: | absorption; co2 capture; kinetic analysis; sodium zirconate; spray drying | ||||||||||||||||||||||||||||||||||||||
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Institution: | The University of Leeds | ||||||||||||||||||||||||||||||||||||||
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemical & Process Engineering (Leeds) | ||||||||||||||||||||||||||||||||||||||
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Depositing User: | Symplectic Publications | ||||||||||||||||||||||||||||||||||||||
Date Deposited: | 04 Apr 2017 11:49 | ||||||||||||||||||||||||||||||||||||||
Last Modified: | 03 Apr 2018 00:38 | ||||||||||||||||||||||||||||||||||||||
Published Version: | https://doi.org/10.1002/cssc.201700046 | ||||||||||||||||||||||||||||||||||||||
Status: | Published | ||||||||||||||||||||||||||||||||||||||
Publisher: | Wiley | ||||||||||||||||||||||||||||||||||||||
Identification Number: | https://doi.org/10.1002/cssc.201700046 |