| 1. |
- Baird, Ross, et al.
(författare)
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High Temperature CO2 Capture Performance and Kinetic Analysis of Novel Potassium Stannate
- 2023
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Ingår i: International Journal of Molecular Sciences. - : MDPI. - 1661-6596 .- 1422-0067. ; 24:3
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Tidskriftsartikel (refereegranskat)abstract
- For the first time, the use of stannate-based sorbents was investigated as high temperature CO2 sorption to evaluate their potential to contribute towards reducing carbon emissions. The sorption capacity and kinetics of commercial tin oxide, sodium, potassium and calcium stannates and lab synthesised potassium stannates were tested using thermogravimetric analysis. Commercial K2SnO3 was found to possess the largest CO2 uptake capacity (2.77 mmol CO2/g or 12.2 wt%) at 700 °C, which is among the highest for potassium sorbents, but the CO2 desorption was not successful. On the contrary, the in-house synthesised K-stannate (K-B) using facile solid-state synthesis outperformed the other sorbents, resulting in a CO2 uptake of 7.3 wt% after 5 min, an adsorption rate (0.016 mg/s) one order of magnitude higher than the other stannates, and stability after 40 cycles. The XRD and XPS analyses showed that K-B contains a mixture of K2SnO3 (76%) and K4SnO4 (21%), while the Scherrer crystal sizes confirmed good resistance to sintering for the potassium stannates. Among the apparent kinetic model tested, the pseudo-second order model was the most suitable to predict the CO2 sorption process of K-B, indicating that chemical adsorption is dominant, while film-diffusion resistance and intra-particle diffusion resistance governed the sorption process in K-B. In summary, this work shows that solid-state synthesised potassium stannate could be an effective sorbent for high temperature separation, and additional work is required to further elucidate its potential.
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| 2. |
- Chang, Ribooga, et al.
(författare)
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Deciphering the existence of hexagonal sodium zirconate CO2 sorbent
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Sodium zirconate (sodium zirconium oxide; Na2ZrO3) is amongst the most investigated carbon dioxide (CO2) sorbent. Na2ZrO3 is renowned for its high capture capacity and cyclic stability. It can effectively capture CO2 at temperatures that are found in industrial processes such as the manufacture of steel or cement. Na2ZrO3 is reported to adopt monoclinic, hexagonal, and cubic structures since it was first discussed in the 1960s. Researchers relied on the differences in the relative intensities between two peaks (2θ ~ 16.2 and 38.7 °) in the powder X-ray diffraction (PXRD) pattern to determine the phase of this compound. It is also widely believed that the CO2 capture performance of Na2ZrO3 is related to the crystal structure, yet the crystal structure of hexagonal Na2ZrO3 has remained elusive. With the use of 3D electron diffraction (3D ED), X-ray photoelectron spectroscopy (XPS), and PXRD, we show that the hexagonal Na2ZrO3 does not exist. The so-called hexagonal Na2ZrO3 is Na2ZrO3 with three different types of disorder. Furthermore, the two PXRD peaks (2θ ~ 16.2 and 38.7 °) cannot be used to distinguish the different phases of Na2ZrO3, as the changes in the PXRD pattern are related to the extent of structure disorder. Finally, we also show that the CO2 capture properties of Na2ZrO3 are related to the Na+ site occupancy between different Na2ZrO3 samples, and not differences in crystal structures. The findings from our work shows that the current literature discussion on the structure of Na2ZrO3 is misleading. In order to further develop Na2ZrO3 as well as other mixed-metal oxides for applications, their structures, as well as any disorder, needs be understood using the methods shown in this study.
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| 3. |
- Chang, Ribooga
(författare)
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Design and Optimization of CO2 sorbents for Point Source Emissions and Direct Air Capture
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This thesis presents a comprehensive study on the design and optimization of CO2 sorbents, targeting two distinct applications: CO2 capture from point source emissions and Direct Air Capture (DAC). The research first introduces Na2HfO3 as a potential CO2 sorbent for point source emissions, using the molten salt effects of Na2CO3 and the thermal stability of HfO2. This combination results in a CO2 sorbent with impressive thermal and cyclic stability, through various optimization steps to enhance CO2 capture performance and efficiency. The study then shows into the structural disorder in Na2ZrO3, a chemically similar CO2 sorbent. This investigation fills a knowledge gap, offering new insights into the sorbent's behavior in CO2 capture. For DAC applications, the thesis explores the design of inorganic anion pillared metal-organic frameworks, focusing on the adjustment of M5+−F− bond lengths in inorganic anion pillars within M5+OFFIVE-1-Ni samples. These structural modifications impact the CO2 capture properties, particularly in terms of capacity and kinetics, demonstrating the potential of structural tuning in enhancing sorbent effectiveness. The synthesized samples exhibit good cyclic and water stability, suggesting their potential for practical DAC applications.
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| 4. |
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| 5. |
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| 6. |
- Chang, Ribooga, et al.
(författare)
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Structural tuning of fluorinated hybrid ultramicroporous materials (HUMs) for low-concentration CO2 capture
- 2024
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Hybrid ultramicroprous materials (HUMs) with a number of different variations of the inorganic pillars as well as surface functional groups have been tested as CO2 sorbent for low-concentration CO2 capture. Specifically well-known HUM NbOFFIVE-1-Ni (NbOFFIVE=(NbOF5)2-, 1=pyz, Ni=nickel(II)) like HUMs were synthesized in this study by replaces Nb with V and Ta. Replacing the metal center from Nb to V or Ta showed that the CO2 adsorption isotherm, in particular at low partial pressures, adopted different shapes and gradient. This study shows that the CO2 adsorption properties at low partial pressures on HUMs can be affected by the metal present in the inorganic pillars.
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| 7. |
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| 8. |
- Chang, Ribooga, et al.
(författare)
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Synthesis and characterization of sodium hafnium oxide (Na2HfO3) and its high-temperature CO2 sorption properties
- 2023
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 11:14, s. 7617-7628
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Tidskriftsartikel (refereegranskat)abstract
- The CO2 sorption properties of sodium hafnium oxide (Na2HfO3) were investigated in this study. Na2HfO3 was synthesized by solid-state synthesis using Na2CO3 and HfO2 as starting materials. The solid-state synthesized Na2HfO3 appeared structurally similar to other mixed metal oxides such as Na2ZrO3, but stacking disorder appeared to be common in Na2HfO3. The synthesis conditions, including the Na : Hf ratio (between 0.5 and 1.5 : 1), synthesis temperature, time and heating rate, were investigated to optimize CO2 sorption properties of Na2HfO3. The Na2HfO3 sorbent showed comparable CO2 uptake capacity, reaction rate and excellent cycling stability compared to other metal oxide sorbents. Na2HfO3 with Na : Hf = 1 : 1 and 1.25 : 1 showed the highest CO2 uptake among all Na2HfO3 samples obtained, with a CO2 uptake capacity of around 15 wt% (at 650–800 °C). The CO2 uptake rate of NHO-1 and NHO-1.25 was fast with over 80% of the equilibrium uptake reached within 250 s. Na2HfO3 remained stable even after 100 cycles with less than 3% difference in the CO2 uptake capacity between the 1st and 100th cycles. We performed kinetic analysis on the CO2 sorption data and found that the Avrami–Erofeev model fitted the kinetic data best among the kinetic models used. Apart from sorbent optimization, we showed that 3D-printing of Na2HfO3 : HfO2 mixtures can be used to produce structured Na2HfO3 sorbents with a slightly improved CO2 uptake rate and the same CO2 uptake capacity as the powder-based solid-state synthesized Na2HfO3 sorbent.
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| 9. |
- Chang, Ribooga, et al.
(författare)
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Synthesis and characterization of sodium hafnium oxide (Na2HfO3) and its high-temperature CO2 sorption properties
- 2023
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 11:14, s. 7617-7628
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Tidskriftsartikel (refereegranskat)abstract
- The CO2 sorption properties of sodium hafnium oxide (Na2HfO3) were investigated in this study. Na2HfO3 was synthesized by solid-state synthesis using Na2CO3 and HfO2 as starting materials. The solid-state synthesized Na2HfO3 appeared structurally similar to other mixed metal oxides such as Na2ZrO3, but stacking disorder appeared to be common in Na2HfO3. The synthesis conditions, including the Na : Hf ratio (between 0.5 and 1.5 : 1), synthesis temperature, time and heating rate, were investigated to optimize CO2 sorption properties of Na2HfO3. The Na2HfO3 sorbent showed comparable CO2 uptake capacity, reaction rate and excellent cycling stability compared to other metal oxide sorbents. Na2HfO3 with Na : Hf = 1 : 1 and 1.25 : 1 showed the highest CO2 uptake among all Na2HfO3 samples obtained, with a CO2 uptake capacity of around 15 wt% (at 650–800 °C). The CO2 uptake rate of NHO-1 and NHO-1.25 was fast with over 80% of the equilibrium uptake reached within 250 s. Na2HfO3 remained stable even after 100 cycles with less than 3% difference in the CO2 uptake capacity between the 1st and 100th cycles. We performed kinetic analysis on the CO2 sorption data and found that the Avrami–Erofeev model fitted the kinetic data best among the kinetic models used. Apart from sorbent optimization, we showed that 3D-printing of Na2HfO3 : HfO2 mixtures can be used to produce structured Na2HfO3 sorbents with a slightly improved CO2 uptake rate and the same CO2 uptake capacity as the powder-based solid-state synthesized Na2HfO3 sorbent.
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| 10. |
- Chang, Ribooga, et al.
(författare)
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Synthetic solid oxide sorbents for CO2 capture : state-of-the art and future perspectives
- 2022
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 10:4, s. 1682-1705
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Forskningsöversikt (refereegranskat)abstract
- Carbon capture is an important and effective approach to control the emission of CO2 from point sources such as fossil fuel power plants, industrial furnaces and cement plants into the atmosphere. For an efficient CO2 capture operation, many aspects of the CO2 capture steps need to be carefully considered. Currently the most mature CO2 capture technology is liquid amine scrubbing. Alternatively, solid sorbents can be used to effectively capture CO2 while alleviating the disadvantages associated with liquid amine sorbents. In this review, we critically assess solid metal oxide CO2 sorbents, especially oxides of group 1 (Li, Na and K) and group 2 (Mg, Ca, Sr and Ba) metals, for capturing CO2 at moderate to high temperatures. In particular, we focus on the recent advances in developing synthetic metal oxide sorbents, and the correlation between the design, synthetic approaches and their cyclic CO2 capture performance, which are characterised by CO2 uptake capacity, rate of carbonation and cyclic stability. The state-of-the-art, challenges, opportunities and future research directions for these metal oxide sorbents are discussed. By devoting more research effort to address the issues identified, there can be great potential to utilise Group 1 and 2 metal oxides as cost-effective, highly efficient sorbents for CO2 capture in a variety of carbon capture applications.
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