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Grape, E. S., Xu, H., Cheung, O., Calmels, M., Zhao, J., Dejoie, C., . . . Inge, A. K. (2020). A Breathing Metal-Organic Framework Based on Flexible Inorganic Building Units. Crystal Growth & Design, 20(1), 320-329
Open this publication in new window or tab >>A Breathing Metal-Organic Framework Based on Flexible Inorganic Building Units
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2020 (English)In: Crystal Growth & Design, ISSN 1528-7483, E-ISSN 1528-7505, Vol. 20, no 1, p. 320-329Article in journal (Refereed) Published
Abstract [en]

Five novel bismuth carboxylate coordination polymers were synthesized from biphenyl-3,4′,5-tricarboxylic acid (H3BPT) and [1,1′:4′,1′′]terphenyl-3,3′′,5,5′′-tetracarboxylic acid (H4TPTC). One of the phases, [Bi(BPT)]·2MeOH (denoted SU-100, as synthesized), is the first example, to the best of our knowledge, of a reversibly flexible bismuth-based metal–organic framework. The material exhibits continuous changes to its unit cell parameters and pore shape depending on the solvent it is immersed in and the dryness of the sample. Typically, in breathing carboxylate-based MOFs, flexibility occurs through tilting of the organic linkers without significantly altering the coordination environment around the cation. In contrast to this, the continuous breathing mechanism in SU-100 involves significant changes to bond angles within the Bi2O12 inorganic building unit (IBU). The flexibility of the IBU of SU-100 reflects the nondiscrete coordination geometry of the bismuth cation. A disproportionate increase in the solvent accessible void volume was observed when compared to the expansion of the unit cell volume of SU-100. Additionally, activated SU-100 (SU-100-HT) exhibits a large increase in unit cell volume, yet has the smallest void volume of all the studied samples.

National Category
Materials Chemistry
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-400206 (URN)10.1021/acs.cgd.9b01266 (DOI)
Available from: 2019-12-19 Created: 2019-12-19 Last updated: 2020-01-29Bibliographically approved
Sun, R., Tai, C.-W., Strømme, M. & Cheung, O. (2020). The Effects of Additives on the Porosity and Stability of Amorphous Calcium Carbonate. Microporous and Mesoporous Materials, 292, Article ID 109736.
Open this publication in new window or tab >>The Effects of Additives on the Porosity and Stability of Amorphous Calcium Carbonate
2020 (English)In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 292, article id 109736Article in journal (Refereed) Published
Abstract [en]

Amorphous calcium carbonate (ACC) stabilized by various carboxylic additives was synthesized by incorporating the additives into an ACC suspension in methanol. The additives studied included polyacrylic acid, citric acid, adipic acid, 6-aminocaproic acid, 4-aminobutyric acid and hexanoic acid. The stabilized ACC samples (ACC-additives) exhibited similar characteristics to ACC alone. They appeared X-ray amorphous, contained characteristic infrared bands and had the same nanoparticle aggregated microstructure as ACC. The porosity of the ACC-additives was, however, markedly improved, with Brunauer-Emmett-Teller (BET) surface areas of up to ~640 m2/g. The BET surface area of ACC-citric acid was close to double that of a highly porous ACC sample. The structure and amount of the additive had a noticeable effect on the porosity of the ACC-additives. When the additive was adsorbed onto the surface of the ACC nanoparticles, their growth was restricted. The restricted growth reduced the size of the ACC nanoparticles, which increased the BET surface area of ACC. Finally, the long-term stability study revealed that the stability of all the ACC-additives was markedly enhanced when stored in ambient or semi-airtight conditions (in a closed falcon tube). In particular, ACC stabilized with adipic acid (ACC-AA-267) had excellent stability, remaining in an amorphous phase for more than one year under ambient conditions and retaining ~87% porosity for 48 weeks under semi-airtight conditions. The extremely high porosity and excellent long-term stability make these ACC-additives promising candidates for applications where porosity and stability are critical, such as those involving adsorption, bone regeneration or drug delivery.

Keywords
Amorphous calcium carbonate, Additives, Porosity, Stability
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-391170 (URN)10.1016/j.micromeso.2019.109736 (DOI)000498292200020 ()
Funder
Swedish Research Council, 2014-3929Swedish Research Council Formas, 2018-00651ÅForsk (Ångpanneföreningen's Foundation for Research and Development), 19-549Knut and Alice Wallenberg Foundation
Available from: 2019-08-20 Created: 2019-08-20 Last updated: 2019-12-18Bibliographically approved
Vall, M., Strömme, M. & Cheung, O. (2019). Amine-Modified Mesoporous Magnesium Carbonate as an Effective Adsorbent for Azo Dyes. ACS Omega, 4, 2973-2979
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
Åhlén, M., Cheung, O. & Strömme, M. (2019). Amorphous Mesoporous Magnesium Carbonate as a Functional Support for UV-Blocking Semiconductor Nanoparticles for Cosmetic Applications. ACS Omega, 4(2), 4429-4436
Open this publication in new window or tab >>Amorphous Mesoporous Magnesium Carbonate as a Functional Support for UV-Blocking Semiconductor Nanoparticles for Cosmetic Applications
2019 (English)In: ACS Omega, ISSN 2470-1343, Vol. 4, no 2, p. 4429-4436Article in journal (Refereed) Published
Abstract [en]

Highly porous amorphous mesoporous magnesium carbonate (MMC) with a Brunauer–Emmett–Teller (BET) surface area over 600 m2·g–1 was evaluated as a micrometer-sized support for TiO2 and ZnO semiconductor nanoparticles. The resulting MMC-TiO2-ZnO contained 25 wt % TiO2 and 25 wt % ZnO incorporated into an MMC structure without blocking the pores as revealed by nitrogen sorption isotherms, scanning electron microscopy, and transmission electron microscopy. In vitro ultraviolet (UV) light-blocking experiments showed that the MMC-TiO2-ZnO had comparable UV-blocking ability as a TiO2 and ZnO nanoparticle mixture containing the same amount of semiconductor particles without a support. Amaranth dye degradation studies revealed that MMC was able to diminish the catalytic activity of TiO2 and ZnO nanoparticles, possibly due to the presence of free carbonate ions in MMC as well as in the dye solution. In summary, this paper demonstrated for the first time that micrometer-sized particles of the recently emerged MMC materials can be used as a support for sun-blocking semiconductor nanoparticles without compromising their UV blocking ability and with significantly lowered photocatalytic activity. When used in a formulation as a support for semiconductor nanoparticles, MMC may also reduce the risk of nanoparticle exposure, and the high porosity of MMC-TiO2-ZnO may be utilized for the delivery of therapeutic agents to the skin.

National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-379180 (URN)10.1021/acsomega.8b03498 (DOI)000460237300215 ()
Funder
Swedish Research Council, 2014-3929
Available from: 2019-03-13 Created: 2019-03-13 Last updated: 2019-03-25Bibliographically approved
Vall, M., Hultberg, J., Strömme, M. & Cheung, O. (2019). Carbon dioxide adsorption on mesoporous magnesium carbonate. Paper presented at 10th International Conference on Applied Energy (ICAE), Hong Kong, August 22-25, 2018. Energy Procedia, 158, 4671-4676
Open this publication in new window or tab >>Carbon dioxide adsorption on mesoporous magnesium carbonate
2019 (English)In: Energy Procedia, ISSN 1876-6102, E-ISSN 1876-6102, Vol. 158, p. 4671-4676Article in journal (Refereed) Published
Abstract [en]

Mesoporous magnesium carbonate (MMC) was synthesized and tested for its ability to separate CO2 from N2. The pure gas CO2 uptake of MMC was around 1.5 mmol/g at 101 kPa, 0 °C. The N2 uptake under the same conditions was less than 0.1 mmol/g. Al(NO3)3, Al2O3, K2CO3 and KNO3 were introduced into the porous structure of MMC as additives. All of the additives tested increased the CO2 uptake of MMC and increased its selectivity towards CO2. The incorporation of 5 wt.% K2CO3 increased the CO2 uptake of MMC up to over 3.2 mmol/g. The ideally adsorbed solution theory was used to calculate the CO2 selectivity of MMC and MMC with additives for a hypothetical gas mixture that contained 15% CO2: 85% N2. The CO2 selectivity at 101 kPa (0 °C) was around 60. MMC with 5 wt.% K2CO3 had a CO2 selectivity of over 150 under the same conditions. Vacuum swing cyclic CO2 adsorption/desorption showed that the CO2 uptake on MMC with 5 wt.% K2CO3 decreased after each cycle. Heat regeneration (up to 250 °C, for 10 minutes) could recover most of the lost CO2 capacity after each cycle. Heat regeneration indicatively improved the cyclic performance of this adsorbent. MMC with 5 wt.% K2CO3 was the best performing adsorbent in this study and can potentially be further developed into a good CO2 adsorbent for temperature swing adsorption (TSA) processes.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Carbon Capture, Storage, Gas separation, Adsorbent, Magnesium carbonate
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-379696 (URN)10.1016/j.egypro.2019.01.738 (DOI)000471031705006 ()
Conference
10th International Conference on Applied Energy (ICAE), Hong Kong, August 22-25, 2018
Note

Part of special issue: Innovative Solutions for Energy Transitions

Available from: 2019-03-19 Created: 2019-03-19 Last updated: 2019-08-05Bibliographically approved
Vall, M., Ferraz, N., Cheung, O., Strömme, M. & Zardán Gómez de la Torre, T. (2019). 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. Molecules, 24(9), Article ID 1820.
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: 2020-02-14Bibliographically approved
Sun, R., Tai, C.-W., Strömme, M. & Cheung, O. (2019). Hierarchical Porous Carbon Synthesized from Novel Porous Amorphous Calcium or Magnesium Citrate with Enhanced SF6 Uptake and SF6/N2 Selectivity. ACS Applied Nano Materials, 2(2), 778-789
Open this publication in new window or tab >>Hierarchical Porous Carbon Synthesized from Novel Porous Amorphous Calcium or Magnesium Citrate with Enhanced SF6 Uptake and SF6/N2 Selectivity
2019 (English)In: ACS Applied Nano Materials, ISSN 2574-0970, Vol. 2, no 2, p. 778-789Article in journal (Refereed) Published
Abstract [en]

The emission of greenhouse gases such as CO2and SF6 is believed to contribute significantly toward globalwarming. One way to reduce their release is by adsorption atpoint sources using a suitable adsorbent. In this work we presentthe synthesis of two hierarchical porous carbon materials(referred to as PC-CaCit and PC-MgCit) with a high uptake ofSF6 (5.23 mmol/g, 0 °C, 100 kPa) and a reasonable uptake ofCO2 (>3 mmol/g). PC-CaCit and PC-MgCit were obtained bypyrolysis of the most porous calcium citrate and magnesiumcitrate ever reported, which were synthesized by us. TheLangmuir specific surface area of PC-CaCit and PC-MgCit wasover 2000 m2/g (BET surface area also close to 2000 m2/g). Wecharacterized PC-CaCit and PC-MgCit using a range of advanced characterization techniques including N2 adsorption, highresolutionelectron microscopy, powder X-ray diffraction, and X-ray photoelectron spectroscopy. PC-CaCit and PC-MgCit alsoshowed a SF6-over-N2 selectivity of ∼33 at 0 °C (100 kPa), good cyclic performance, and moderately low heat of adsorption.The porous carbons synthesized in this work are good candidate adsorbents for greenhouse gases.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
Keywords
porous carbon, SF6 adsorption, CO2 adsorption, amorphous calcium citrate, amorphous magnesium citrate
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-381054 (URN)10.1021/acsanm.8b02005 (DOI)000469409900019 ()
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation
Available from: 2019-04-03 Created: 2019-04-03 Last updated: 2019-08-21Bibliographically approved
Sun, R., Åhlén, M., Tai, C.-W., Bajnóczi, E. G., de Kleijne, F., Ferraz, N., . . . Cheung, O. (2019). Highly Porous Amorphous Calcium Phosphate for Drug Delivery and Bio-Medical Applications. Nanomaterials, 10(1)
Open this publication in new window or tab >>Highly Porous Amorphous Calcium Phosphate for Drug Delivery and Bio-Medical Applications
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2019 (English)In: Nanomaterials, ISSN 2079-4991, Vol. 10, no 1Article in journal (Refereed) Published
Abstract [en]

Amorphous calcium phosphate (ACP) has shown significant effects on the biomineralization and promising applications in bio-medicine. However, the limited stability and porosity of ACP material restrict its practical applications. A storage stable highly porous ACP with Brunauer&ndash;Emmett&ndash;Teller surface area of over 400 m2/g was synthesized by introducing phosphoric acid to a methanol suspension containing amorphous calcium carbonate nanoparticles. Electron microscopy revealed that the porous ACP was constructed with aggregated ACP nanoparticles with dimensions of several nanometers. Large angle X-ray scattering revealed a short-range atomic order of &lt;20 &Aring; in the ACP nanoparticles. The synthesized ACP demonstrated long-term stability and did not crystallize even after storage for over 14 months in air. The stability of the ACP in water and an &alpha;-MEM cell culture medium were also examined. The stability of ACP could be tuned by adjusting its chemical composition. The ACP synthesized in this work was cytocompatible and acted as drug carriers for the bisphosphonate drug alendronate (AL) in vitro. AL-loaded ACP released 25% of the loaded AL in the first 22 days. These properties make ACP a promising candidate material for potential application in biomedical fields such as drug delivery and bone healing.

National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-401158 (URN)10.3390/nano10010020 (DOI)
Available from: 2020-01-07 Created: 2020-01-07 Last updated: 2020-02-04Bibliographically approved
Liu, J., Zhao, G., Cheung, O., Jia, L., Sun, Z. & Zhang, S. (2019). Highly Porous Metalloporphyrin Covalent Ionic Frameworks with Well-Defined Cooperative Functional Groups as Excellent Catalysts for CO2 Cycloaddition. Chemistry - A European Journal, 25(38), 9052-9059
Open this publication in new window or tab >>Highly Porous Metalloporphyrin Covalent Ionic Frameworks with Well-Defined Cooperative Functional Groups as Excellent Catalysts for CO2 Cycloaddition
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2019 (English)In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 25, no 38, p. 9052-9059Article in journal (Refereed) Published
Abstract [en]

The development of multifunctional heterogeneous catalysts with high porosity and remarkable catalytic activity still remains a challenge. Herein, four highly porous metalloporphyrin covalent ionic frameworks (CIFs) were synthesized by coupling 5,10,15,20-tetrakis(4-nitrophenyl)porphyrin (TNPP) with 3,8-diamino-6-phenylphenanithridine (NPPN) or 5,5 '-diamino-2,2 '-bipyridine (NBPy) followed by ionization with bromoethane (C2H5Br) or dibromoethane (C2H4Br2) and then metalization with Zn or Co. The resulting CIFs showed high efficiency in catalyzing the cycloaddition of propylene oxide (PO) with CO2 to form propylene carbonate (PC). All of the Zn-containing CIF catalysts were able to catalyze the cycloaddition reaction with a PC yield greater than 97 %. The TNPP/NBPy (CIF2) catalyst ionized with C2H4Br2 and metalized with Zn (Zn-CIF2-C2H4) exhibited the highest catalytic activity among the synthesized catalysts. The high catalytic performance of Zn-CIF2-C2H4 is related to its high porosity (577 m(2) g(-1)), high Br:metal ratio (1:3.89), and excellent synergistic action between the Lewis acidic Zn sites and the nucleophilic Br- ions. Zn-CIF2-C2H4 is sufficiently stable that greater than 94 % PC yield could be obtained even after six cycles. In addition, Zn-CIF2-C2H4 could catalyze the cycloaddition of several other epoxides with CO2. These highly porous materials are promising multifunctional and efficient catalysts for industrially relevant reactions.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2019
Keywords
carbon dioxide, covalent ionic frameworks, cycloaddition, heterogeneous catalysis, porphyrins
National Category
Organic Chemistry
Identifiers
urn:nbn:se:uu:diva-394169 (URN)10.1002/chem.201900992 (DOI)000484146600019 ()30997700 (PubMedID)
Available from: 2019-10-08 Created: 2019-10-08 Last updated: 2019-10-08Bibliographically approved
Vall, M., Hultberg, J., Strømme, M. & Cheung, O. (2019). Inorganic carbonate composites as potential high temperature CO2 sorbents with enhanced cycle stability. RSC Advances, 9(35), 20273-20280
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
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-4072-4324

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