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Inorganic carbonate composites as potential high temperature CO2 sorbents with enhanced cycle stability
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.ORCID iD: 0000-0002-5496-9664
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.ORCID iD: 0000-0002-4072-4324
2019 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 9, no 35, p. 20273-20280Article in journal (Refereed) Published
Abstract [en]

A calcium magnesium carbonate composite (CMC) material containing highly porous amorphous calcium carbonate (HPACC) and mesoporous magnesium carbonate (MMC) was synthesized. CMCs with varying HPACC : MMC mol ratios and high BET surface area (over 490 m2 g−1) were produced. The CMCs retained the morphology shared by HPACC and MMC. All these materials were built up of aggregated nanometer-sized particles. We tested the CO2 uptake properties of the synthesized materials. The CMCs were calcined at 850 °C to obtain the corresponding calcium magnesium oxide composites (CMOs) that contained CaO : MgO at different mol ratios. CMO with CaO : MgO = 3 : 1 (CMO-3) showed comparable CO2 uptake at 650 °C (0.586 g g−1) to CaO sorbents obtained from pure HPACC (0.658 g g−1) and the commercial CaCO3 (0.562 g g−1). Over 23 adsorption–desorption cycles CMOs also showed a lower CO2 uptake capacity loss (35.7%) than CaO from HPACC (51.3%) and commercial CaCO3 (79.7%). Al was introduced to CMO by the addition of Al(NO3)3 in the synthesis of CMC-3 to give ACMO after calcination. The presence of ∼19 mol% of Al(NO3)3 in ACMO-4 significantly enhanced its stability over 23 cycles (capacity loss of 5.2%) when compared with CMO-3 (calcined CMC-3) without adversely affecting the CO2 uptake. After 100 cycles, ACMO-4 still had a CO2 uptake of 0.219 g g−1. Scanning electron microscope images clearly showed that the presence of Mg and Al in CMO hindered the sintering of CaCO3 at high temperatures and therefore, enhanced the cycle stability of the CMO sorbents. We tested the CO2 uptake properties of CMO and ACMO only under ideal laboratory testing environment, but our results indicated that these materials can be further optimized as good CO2 sorbents for various applications.

Place, publisher, year, edition, pages
2019. Vol. 9, no 35, p. 20273-20280
National Category
Nano Technology
Identifiers
URN: urn:nbn:se:uu:diva-381415DOI: 10.1039/C9RA02843AISI: 000474266800042OAI: oai:DiVA.org:uu-381415DiVA, id: diva2:1303316
Funder
Swedish Research Council, 2014-3929Swedish Research Council Formas, 2018-00651Mistra - The Swedish Foundation for Strategic Environmental Research, 2015/31Available from: 2019-04-09 Created: 2019-04-09 Last updated: 2019-09-17Bibliographically approved
In thesis
1. Development of Nanoporous Inorganic Carbonates for Pharmaceutical and Environmental Applications
Open this publication in new window or tab >>Development of Nanoporous Inorganic Carbonates for Pharmaceutical and Environmental Applications
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Mesoporous magnesium carbonate (MMC) is a highly porous, anhydrous material which can be synthesized without the use of templates. This thesis shows how post- and in synthesis modification of MMC can create porous inorganic carbonates suitable for different pharmaceutical and environmental applications. 

Controlled release of IBU was achieved by loading IBU onto amine modified MMC (aMMC). The amine coverage was varied and there was a clear correlation between the release rate of IBU and the amine coverage, the higher the amine coverage the slower the release rate. aMMC was also used to load salicylic acid (SA). SA was then released within 15 minutes in a phosphate buffer (pH 6.8). The cytotoxicity of aMMC was evaluated and it was found non-toxic for human dermal fibroblast cells with particle concentration up to 1000 µg/mL for 48 h of exposure.  aMMC also showed a high adsorption capacity for three different types of anionic azo dyes;  acid red 183, amaranth and reactive black 5. The addition of amine groups to the surface of MMC significantly increased the uptake of the three dyes tested. Composite materials were synthesized by combining the synthesis of MMC and the synthesis of highly porous amorphous calcium carbonate. The calcium magnesium carbonate composite materials were evaluated for their CO2 sorption capacity (at 650 °C) and their CO2 cyclic stability. Addition of Al(NO3)3 to the best performing composite further improved its cyclic stability and the composite maintained a high CO2 uptake over 23 sorption/desorption cycles. Composite materials were also made by adding Al2O3 and SiO2 nanoparticles to the synthesis liquid of MMC.  This resulted in materials with Al2O3 and SiO2 incorporated into the porous MMC structure. The MMC materials with Al2O3 and SiO2 nanoparticles was then impregnated with Ni(NO3)2, calcined and used for catalytic conversion of syngas to natural gas. The material containing Al2O3 nanoparticles performed the best and had a CO conversion of close to 100% at 350°C as well as a high CH4 yield and selectivity.

In this thesis porous inorganic carbonates have been developed and evaluated for their performance in different pharmaceutical and environmental applications.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2019. p. 65
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1801
Keywords
Mesoporous magnesium carbonate, drug delivery, water purification, CO2 capture, catalysis
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-381336 (URN)978-91-513-0638-4 (ISBN)
Public defence
2019-06-03, Polhemssalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:30 (English)
Opponent
Supervisors
Available from: 2019-05-10 Created: 2019-04-10 Last updated: 2019-06-18

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Vall, MariaStrømme, MariaCheung, Ocean

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