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Development of Nanoporous Inorganic Carbonates for Pharmaceutical and Environmental Applications
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
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 [en]
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: urn:nbn:se:uu:diva-381336ISBN: 978-91-513-0638-4 (print)OAI: oai:DiVA.org:uu-381336DiVA, id: diva2:1303565
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
List of papers
1. Effects of amine modification of mesoporous magnesium carbonate on controlled drug release
Open this publication in new window or tab >>Effects of amine modification of mesoporous magnesium carbonate on controlled drug release
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2017 (English)In: International Journal of Pharmaceutics, ISSN 0378-5173, E-ISSN 1873-3476, Vol. 524, p. 141-147Article in journal (Refereed) Published
Abstract [en]

(3-Aminopropyl)triethoxysilane (APTES) was used to modify the surface of mesoporous magnesium carbonate (MMC). The as-synthesized MMC had an average pore diameter of ∼5 nm, but amine grafting occurred preferentially on the walls of the largest MMC pores. Analysis of ibuprofen (IBU) loading and release showed that IBU remained stable in the amorphous phase in all the MMC and modified MMC samples. The kinetics of IBU release from the modified MMC were assessed and used to evaluate the effects of the different functional groups. The release rate showed that the release of IBU could be controlled by adjusting the amine surface coverage of MMC and also by changing the surface groups. It was concluded that the interaction between the grafted, functional groups in the modified MMC and the OH in the carboxyl groups of IBU was the most important factor for prolonging the release of the drug. These results are expected to lead to investigation of other as yet unexplored applications for MMC, including using it as a plastic additive and for gas separation.

Keywords
ibuprofen, mesoporous, magnesium carbonate, APTES, controlled release, surface functionalization
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-318721 (URN)10.1016/j.ijpharm.2017.03.063 (DOI)000401108500014 ()28359819 (PubMedID)
Funder
Swedish Research Council, 2014-3929Swedish Energy Agency, P38273-1
Available from: 2017-03-28 Created: 2017-03-28 Last updated: 2019-04-10
2. Exploring the use of amine modified mesoporous magnesium carbonate for the delivery of salicylic acid in topical formulations: in vitro cytotoxicity and drug release studies
Open this publication in new window or tab >>Exploring the use of amine modified mesoporous magnesium carbonate for the delivery of salicylic acid in topical formulations: in vitro cytotoxicity and drug release studies
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2019 (English)In: Molecules, ISSN 1420-3049, E-ISSN 1420-3049, Vol. 24, no 9, article id 1820Article in journal (Refereed) Published
Place, publisher, year, edition, pages
MDPI, 2019
Keywords
mesoporous; magnesium carbonate; amine functionalization; cytotoxicity; salicylic acid; drug release
National Category
Nano Technology
Identifiers
urn:nbn:se:uu:diva-381421 (URN)10.3390/molecules24091820 (DOI)
Available from: 2019-04-10 Created: 2019-04-10 Last updated: 2019-05-13
3. Inorganic carbonate composites as potential high temperature CO2 sorbents with enhanced cycle stability
Open this publication in new window or tab >>Inorganic carbonate composites as potential high temperature CO2 sorbents with enhanced cycle stability
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.

National Category
Nano Technology
Identifiers
urn:nbn:se:uu:diva-381415 (URN)10.1039/C9RA02843A (DOI)000474266800042 ()
Funder
Swedish Research Council, 2014-3929Swedish Research Council Formas, 2018-00651Mistra - The Swedish Foundation for Strategic Environmental Research, 2015/31
Available from: 2019-04-09 Created: 2019-04-09 Last updated: 2019-09-17Bibliographically approved
4. Amine-Modified Mesoporous Magnesium Carbonate as an Effective Adsorbent for Azo Dyes
Open this publication in new window or tab >>Amine-Modified Mesoporous Magnesium Carbonate as an Effective Adsorbent for Azo Dyes
2019 (English)In: ACS Omega, Vol. 4, p. 2973-2979Article in journal (Refereed) Published
Abstract [en]

Mesoporous magnesium carbonate (MMC) was evaluated as a potential candidate material for removal of dyes from textile industry wastewater. The adsorption property of MMC was analyzed for three different azo dyes: reactive black 5 (RB5), amaranth (AM), and acid red 183 (AR183). Further, the effect of porosity, amine modification, ionic strength, and pH was evaluated. MMC modified with 3-(aminopropyl)triethoxysilane (aMMC) showed consistently high uptake levels for all of the azo dyes tested; the uptake of RB5, AM, and AR183 was ∼360, ∼143 and ∼170 mg/g, respectively. The results demonstrated the importance of porosity and surface chemistry in the effective adsorption of the azo dye in aqueous systems. The uptake of RB5 and AM on aMMC was not significantly affected by pH (when varied between 4 and 10), although reduced uptake of RB5 and AM was observed at pH values <2 and >12. The addition of NaCl salt at concentrations up to 1000 mM had minimal effect on the high uptake of RB5 on aMMC. The uptake of AM by aMMC was reduced by approximately 20% in the presence of NaCl even at low concentrations. The uptake of AR183 by aMMC varied noticeably by changes in pH and no specific trend was observed. The presence of NaCl also adversely affected the uptake of AR183 on aMMC. The adsorption of the azo dye on aMMC was most likely driven by electrostatic interactions. We show here that aMMC is a potential candidate adsorbent for the effective removal of azo dyes from textile wastewaters.

National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-380594 (URN)10.1021/acsomega.8b03493 (DOI)
Available from: 2019-03-29 Created: 2019-03-29 Last updated: 2019-04-10Bibliographically approved
5. Novel Ni/MgO Catalysts from mesoporous MgCO3 for Highly Efficient CO methanation: Effects of Al and Si Stabilization
Open this publication in new window or tab >>Novel Ni/MgO Catalysts from mesoporous MgCO3 for Highly Efficient CO methanation: Effects of Al and Si Stabilization
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(English)Manuscript (preprint) (Other academic)
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-381403 (URN)
Available from: 2019-04-09 Created: 2019-04-09 Last updated: 2019-04-10

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