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Synthesis, Porous Structure Analysis, and Application of Sorbents in CO2 Capture

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Porous Materials".

Deadline for manuscript submissions: closed (20 May 2023) | Viewed by 16756

Special Issue Editor

Centro de Quimica Estrutural, Instituto Superior Técnico da Universidade de Lisboa, Lisboa, Portugal
Interests: CO2 capture and use; high/medium temperature CO2 sorbents; calcium looping; natural and synthetic sorbents; in situ CO2 capture; thermochemical energy storage materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The International Energy Agency has consistently highlighted that there is no unique or simple solution to meeting international neutral climate goals; cutting emissions is an urgent priority, but the development and deployment of carbon removal technologies using different CO2 capture materials could play chief and complementary roles in shifting the energy sector toward carbon neutrality or negative emissions. 

This Special Issue, “Synthesis, Porous Structure Analysis, and Application of Sorbents in CO2 capture” will address topics related, but not limited to, advances in the synthesis of sorbents for CO2 capture; manipulation of sorbents porosity; supported and unsupported sorbents; micronized and nanosized sorbents; and stability, activity and regeneration of sorbents under different technologic applications, at low, medium, or high temperature. Additionally, bifunctional sorbent materials for CO2 capture and conversion are welcome.

Original papers or reviews of efficient CO2 capture sorbents synthesized by emerging and innovative techniques will be considered. 

Dr. Paula Teixeira
Guest Editor

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Keywords

  • Synthesis of CO2 sorbents using innovative and emerging techniques
  • Advanced and alternative sorbents for CO2 capture
  • Micronized and nanosized CO2 sorbents
  • Manipulation of sorbents porosity
  • Activity, stability, and regeneration of CO2 sorbents
  • Synthesis of bifunctional sorbents: capture and conversion

Published Papers (10 papers)

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Research

20 pages, 2491 KiB  
Article
Understanding the Role of Mono and Ternary Alkali Metal Salts on CO2 Uptake of MgO Sorbents
by Patrícia Correia, Carla I. C. Pinheiro and Paula Teixeira
Materials 2023, 16(24), 7539; https://doi.org/10.3390/ma16247539 - 06 Dec 2023
Viewed by 840
Abstract
CO2 uptake by MgO-based sorbents at intermediate temperatures is attractive for pre- and post-combustion CO2 capture applications. However, besides the high CO2 uptake potential of these materials (1.1 g CO2 g−1 sorbent), in practice, the realistic CO2 [...] Read more.
CO2 uptake by MgO-based sorbents at intermediate temperatures is attractive for pre- and post-combustion CO2 capture applications. However, besides the high CO2 uptake potential of these materials (1.1 g CO2 g−1 sorbent), in practice, the realistic CO2 capture is far from that of the theorical values. In this work, the sol–gel method was used to synthetize unsupported and supported MgO sorbents (10% Ca or 10% Ce support, mol) that were impregnated with different fractions (15, 25, and 35; % mol) of a NaNO3 single salt or a ternary alkali salt (NaNO3, LiNO3 and KNO3 (18/30/52; % mol)). To understand the role of alkali metal salts (AMSs) in the MgO sorbents’ performance, the working and decomposition temperature ranges of AMS under different atmospheres (CO2 and air) were evaluated. The findings show that the CO2 uptake temperature range and maximum uptake (20–500 °C, CO2 atmosphere) of sorbents are correlated. The cyclic CO2 uptake of the most promising sorbents was tested along five carbonation–calcination cycles. For the first and fifth cycles, respectively, the 15 (Na, K, Li)-MgO sorbents showed the highest carrying capacity, i.e., 460–330 mg CO2 g−1 sorbent, while for the 15 (Na, K, Li)-MgO-Ca sorbents, it was 375–275 mg CO2 g−1. However, after the first cycle, the carbonation occurred faster for the 15 (Na, K, Li)-MgO-Ca sorbents, meaning that it can be a path to overpassing carbonation kinetics limitations of the MgO sorbent, making it viable for industrial applications. Full article
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11 pages, 2448 KiB  
Article
Modelling Selective CO2 Absorption and Validation via Photosynthetic Bacteria and Chemical Adsorbents for Methane Purification in Anaerobic Fermentation Bioreactors
by Yu-Chen Hsu, Shunnian Wu, Juei-Yu Chiu, Hashan N. Thenuwara, Hasanthi L. Senevirathna and Ping Wu
Materials 2023, 16(19), 6533; https://doi.org/10.3390/ma16196533 - 01 Oct 2023
Viewed by 995
Abstract
This study delves into advanced methane purification techniques within anaerobic fermentation bioreactors, focusing on selective CO2 absorption and comparing photosynthetic bacteria (PNSB) with chemical adsorbents. Our investigation demonstrates that MgO-Mg(OH)2 composites exhibit remarkable CO2 selectivity over CH4, substantiated [...] Read more.
This study delves into advanced methane purification techniques within anaerobic fermentation bioreactors, focusing on selective CO2 absorption and comparing photosynthetic bacteria (PNSB) with chemical adsorbents. Our investigation demonstrates that MgO-Mg(OH)2 composites exhibit remarkable CO2 selectivity over CH4, substantiated through rigorous bulk and surface modelling analyses. To address the challenges posed by MgCO3 shell formation on MgO particles, hindering CO2 transport, we advocate for the utilisation of MgO-Mg(OH)2 composites. In on-site experiments, these composites, particularly saturated MgO-Mg(OH)2 solutions (S2), achieved an astonishing 100% CO2 removal rate within a single day while preserving CH4 content. In contrast, solid MgO powder (S3) retained a mere 5% of CH4 over a 10 h period. Although PNSB (S1) exhibited slower CO2 removal, it excelled in nutrient recovery from anaerobic effluent. We introduce a groundbreaking hybrid strategy that leverages S2’s swift CO2 removal and S1 PNSB’s nutrient recovery capabilities, potentially resulting in a drastic reduction in bioreactor processing time, from 10 days when employing S1 to just 1 day with the use of S2. This represents a remarkable efficiency improvement of 1000%. This pioneering strategy has the potential to revolutionise methane purification, enhancing both efficiency and sustainability. Importantly, it can be seamlessly integrated into existing bioreactors through an additional CO2 capture step, offering a promising solution for advancing biogas production and promoting sustainable waste treatment practices. Full article
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12 pages, 2734 KiB  
Article
On the Selectivity of Simultaneous CO2 and N2 Reduction Using TiO2/Carbon Sphere Photocatalysts Prepared by Microwave Treatment and Mounted on Silica Cloth
by Ewelina Kusiak-Nejman, Katarzyna Ćmielewska, Iwona Pełech, Ewa Ekiert, Piotr Staciwa, Daniel Sibera, Agnieszka Wanag, Joanna Kapica-Kozar, Marcin Gano, Urszula Narkiewicz and Antoni W. Morawski
Materials 2023, 16(17), 5810; https://doi.org/10.3390/ma16175810 - 24 Aug 2023
Viewed by 518
Abstract
This paper presents new photocatalysts obtained by treating carbon spheres (CS) and TiO2 in a microwave reactor at a pressure of 20 atm and a temperature of up to 300 °C for 15 min and then depositing TiO2/CS composites on [...] Read more.
This paper presents new photocatalysts obtained by treating carbon spheres (CS) and TiO2 in a microwave reactor at a pressure of 20 atm and a temperature of up to 300 °C for 15 min and then depositing TiO2/CS composites on glass fibre cloths. Such highly CO2-adsorbing photocatalysts showed photoactivity in the simultaneous water-splitting process, generating H2, reducing CO2 to CO and CH4, and reducing N2 to NH3. In addition, calculations of the hydrogen balance involved in all reactions were performed. Adding 1 g of carbon spheres per 1 g of TiO2 maintained the high selectivity of nitrogen fixation at 95.87–99.5%, which was continuously removed from the gas phase into the water as NH4+ ions. Full article
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14 pages, 3850 KiB  
Article
Efficient Synthesis of 2D Mica Nanosheets by Solvothermal and Microwave-Assisted Techniques for CO2 Capture Applications
by P. Vishakha T. Weerasinghe, Shunnian Wu, W. P. Cathie Lee, Ming Lin, Franklin Anariba, Xu Li, Debbie Hwee Leng Seng, Jia Yu Sim and Ping Wu
Materials 2023, 16(7), 2921; https://doi.org/10.3390/ma16072921 - 06 Apr 2023
Cited by 2 | Viewed by 1849
Abstract
Mica, a commonly occurring mineral, has significant potential for various applications due to its unique structure and properties. However, due to its non-Van Der Waals bonded structure, it is difficult to exfoliate mica into ultrathin nanosheets. In this work, we report a rapid [...] Read more.
Mica, a commonly occurring mineral, has significant potential for various applications due to its unique structure and properties. However, due to its non-Van Der Waals bonded structure, it is difficult to exfoliate mica into ultrathin nanosheets. In this work, we report a rapid solvothermal microwave synthesis of 2D mica with short reaction time and energy conservation. The resulting exfoliated 2D mica nanosheets (eMica nanosheets) were characterized by various techniques, and their ability to capture CO2 was tested by thermogravimetric analysis (TGA). Our results showed an 87% increase in CO2 adsorption capacity with eMica nanosheets compared to conventional mica. Further characterization by Fourier-transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS), as well as first-principles calculations, showed that the high specific surface area and deposited K2CO3 layer contribute to the increased CO2 adsorption on the mica nanosheets. These results speak to the potential of high-quality eMica nanosheets and efficient synthesis processes to open new avenues for new physical properties of 2D materials and the development of CO2 capture technologies. Full article
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13 pages, 14432 KiB  
Article
Solvent-Free Coupling Reaction of Carbon Dioxide and Epoxides Catalyzed by Quaternary Ammonium Functionalized Schiff Base Metal Complexes under Mild Conditions
by Qin Wen, Xuexin Yuan, Qiqi Zhou, Hai-Jian Yang, Qingqing Jiang, Juncheng Hu and Cun-Yue Guo
Materials 2023, 16(4), 1646; https://doi.org/10.3390/ma16041646 - 16 Feb 2023
Cited by 1 | Viewed by 1358
Abstract
A series of bifunctional Schiff base metal catalysts (Zn-NPClR, Zn-NPXH, and M-NPClH) with two quaternary ammonium groups were prepared for carbon dioxide (CO2) and epoxide coupling reactions. The effects of the reaction variables on the catalytic activity were systematically investigated, and [...] Read more.
A series of bifunctional Schiff base metal catalysts (Zn-NPClR, Zn-NPXH, and M-NPClH) with two quaternary ammonium groups were prepared for carbon dioxide (CO2) and epoxide coupling reactions. The effects of the reaction variables on the catalytic activity were systematically investigated, and the optimal reaction conditions (120 °C, 1 MPa CO2, 3 h) were screened. The performances of different metal-centered catalysts were evaluated, and Co-NPClH showed excellent activity. This kind of bifunctional catalyst has a wide range of substrate applicability, excellent stability, and can be reused for more than five runs. A relatively high TOF could reach up to 1416 h−1 with Zn-NPClH as catalyst by adjusting reaction factors. In addition, the kinetic study of the coupling reaction catalyzed by three catalysts (Zn, Co, and Ni) was carried out to obtain the activation energy (Ea) for the formation of cyclic carbonates. Finally, a possible mechanism for this cyclization reaction was proposed. Full article
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38 pages, 4931 KiB  
Article
Optimization of CO2 Sorption onto Spent Shale with Diethylenetriamine (DETA) and Ethylenediamine (EDA)
by Asmau Iyabo Balogun, Eswaran Padmanabhan, Firas Ayad Abdulkareem, Haylay Tsegab Gebretsadik, Cecilia Devi Wilfred, Hassan Soleimani, Prasanna Mohan Viswanathan, Boon Siong Wee and Jemilat Yetunde Yusuf
Materials 2022, 15(23), 8293; https://doi.org/10.3390/ma15238293 - 22 Nov 2022
Cited by 1 | Viewed by 1190
Abstract
A novel technique was employed to optimize the CO2 sorption performance of spent shale at elevated pressure–temperature (PT) conditions. Four samples of spent shale prepared from the pyrolysis of oil shale under an anoxic condition were further modified with diethylenetriamine (DETA) and [...] Read more.
A novel technique was employed to optimize the CO2 sorption performance of spent shale at elevated pressure–temperature (PT) conditions. Four samples of spent shale prepared from the pyrolysis of oil shale under an anoxic condition were further modified with diethylenetriamine (DETA) and ethylenediamine (EDA) through the impregnation technique to investigate the variations in their physicochemical characteristics and sorption performance. The textural and structural properties of the DETA- and EDA- modified samples revealed a decrease in the surface area from tens of m2/g to a unit of m2/g due to the amine group dispersing into the available pores, but the pore sizes drastically increased to macropores and led to the creation of micropores. The N–H and C–N bonds of amine noticed on the modified samples exhibit remarkable affinity for CO2 sequestration and are confirmed to be thermally stable at higher temperatures by thermogravimetric (TG) analysis. Furthermore, the maximum sorption capacity of the spent shale increased by about 100% with the DETA modification, and the equilibrium isotherm analyses confirmed the sorption performance to support heterogenous sorption in conjunction with both monolayer and multilayer coverage since they agreed with the Sips, Toth, Langmuir, and Freundlich models. The sorption kinetics confirm that the sorption process is not limited to diffusion, and both physisorption and chemisorption have also occurred. Furthermore, the heat of enthalpy reveals an endothermic reaction observed between the CO2 and amine-modified samples as a result of the chemical bond, which will require more energy to break down. This investigation reveals that optimization of spent shale with amine functional groups can enhance its sorption behavior and the amine-modified spent shale can be a promising sorbent for CO2 sequestration from impure steams of the natural gas. Full article
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18 pages, 5077 KiB  
Article
Synthesis and Characterization of a Crystalline Imine-Based Covalent Organic Framework with Triazine Node and Biphenyl Linker and Its Fluorinated Derivate for CO2/CH4 Separation
by Stefanie Bügel, Malte Hähnel, Tom Kunde, Nader de Sousa Amadeu, Yangyang Sun, Alex Spieß, Thi Hai Yen Beglau, Bernd M. Schmidt and Christoph Janiak
Materials 2022, 15(8), 2807; https://doi.org/10.3390/ma15082807 - 11 Apr 2022
Cited by 9 | Viewed by 3143
Abstract
A catalyst-free Schiff base reaction was applied to synthesize two imine-linked covalent organic frameworks (COFs). The condensation reaction of 1,3,5-tris-(4-aminophenyl)triazine (TAPT) with 4,4′-biphenyldicarboxaldehyde led to the structure of HHU-COF-1 (HHU = Heinrich-Heine University). The fluorinated analog HHU-COF-2 was obtained with 2,2′,3,3′,5,5′,6,6′-octafluoro-4,4′-biphenyldicarboxaldehyde. Solid-state NMR, [...] Read more.
A catalyst-free Schiff base reaction was applied to synthesize two imine-linked covalent organic frameworks (COFs). The condensation reaction of 1,3,5-tris-(4-aminophenyl)triazine (TAPT) with 4,4′-biphenyldicarboxaldehyde led to the structure of HHU-COF-1 (HHU = Heinrich-Heine University). The fluorinated analog HHU-COF-2 was obtained with 2,2′,3,3′,5,5′,6,6′-octafluoro-4,4′-biphenyldicarboxaldehyde. Solid-state NMR, infrared spectroscopy, X-ray photoelectron spectroscopy, and elemental analysis confirmed the successful formation of the two network structures. The crystalline materials are characterized by high Brunauer–Emmett–Teller surface areas of 2352 m2/g for HHU-COF-1 and 1356 m2/g for HHU-COF-2. The products of a larger-scale synthesis were applied to prepare mixed-matrix membranes (MMMs) with the polymer Matrimid. CO2/CH4 permeation tests revealed a moderate increase in CO2 permeability at constant selectivity for HHU-COF-1 as a dispersed phase, whereas application of the fluorinated COF led to a CO2/CH4 selectivity increase from 42 for the pure Matrimid membrane to 51 for 8 wt% of HHU-COF-2 and a permeability increase from 6.8 to 13.0 Barrer for the 24 wt% MMM. Full article
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12 pages, 1848 KiB  
Article
Counter-Intuitive Magneto-Water-Wetting Effect to CO2 Adsorption at Room Temperature Using MgO/Mg(OH)2 Nanocomposites
by Hasanthi L. Senevirathna, P. Vishakha T. Weerasinghe, Xu Li, Ming-Yan Tan, Sang-Sub Kim and Ping Wu
Materials 2022, 15(3), 983; https://doi.org/10.3390/ma15030983 - 27 Jan 2022
Cited by 2 | Viewed by 1673
Abstract
MgO/Mg(OH)2-based materials have been intensively explored for CO2 adsorption due to their high theoretical but low practical CO2 capture efficiency. Our previous study on the effect of H2O wetting on CO2 adsorption in MgO/Mg(OH)2 nanostructures [...] Read more.
MgO/Mg(OH)2-based materials have been intensively explored for CO2 adsorption due to their high theoretical but low practical CO2 capture efficiency. Our previous study on the effect of H2O wetting on CO2 adsorption in MgO/Mg(OH)2 nanostructures found that the presence of H2O molecules significantly increases (decreases) CO2 adsorption on the MgO (Mg(OH)2) surface. Furthermore, the magneto-water-wetting technique is used to improve the CO2 capture efficiency of various nanofluids by increasing the mass transfer efficiency of nanobeads. However, the influence of magneto-wetting to the CO2 adsorption at nanobead surfaces remains unknown. The effect of magneto-water-wetting on CO2 adsorption on MgO/Mg(OH)2 nanocomposites was investigated experimentally in this study. Contrary to popular belief, magneto-water-wetting does not always increase CO2 adsorption; in fact, if Mg(OH)2 dominates in the nanocomposite, it can actually decrease CO2 adsorption. As a result of our structural research, we hypothesized that the creation of a thin H2O layer between nanograins prevents CO2 from flowing through, hence slowing down CO2 adsorption during the carbon-hydration aging process. Finally, the magneto-water-wetting technique can be used to control the carbon-hydration process and uncover both novel insights and discoveries of CO2 capture from air at room temperature to guide the design and development of ferrofluid devices for biomedical and energy applications. Full article
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9 pages, 1380 KiB  
Article
Morphology Design and Fabrication of Bio-Inspired Nano-MgO–Mg(OH)2 via Vapor Steaming to Enable Bulk CO2 Diffusion and Capture
by Hasanthi L. Senevirathna, Shunnian Wu, W. P. Cathie Lee and Ping Wu
Materials 2022, 15(2), 680; https://doi.org/10.3390/ma15020680 - 17 Jan 2022
Cited by 6 | Viewed by 1870
Abstract
The absorption of CO2 on MgO is being studied in depth in order to enhance carbon engineering. Production of carbonate on MgO surfaces, such as MgCO3, for example, has been shown to hinder further carbon lattice transit and lower CO [...] Read more.
The absorption of CO2 on MgO is being studied in depth in order to enhance carbon engineering. Production of carbonate on MgO surfaces, such as MgCO3, for example, has been shown to hinder further carbon lattice transit and lower CO2 collecting efficiency. To avoid the carbonate blocking effect, we mimic the water harvesting nano-surface systems of desert beetles, which use alternate hydrophobic and hydrophilic surface domains to collect liquid water and convey condensed droplets down to their mouths, respectively. We made CO2-philic MgO and CO2-phobic Mg(OH)2 nanocomposites from electrospun nano-MgO by vapor steaming for 2–20 min at 100 °C. The crystal structure, morphology, and surface properties of the produced samples were instrumentally characterized using XRD, SEM, XPS, BET, and TGA. We observed that (1) fiber morphology shifted from hierarchical particle and sheet-like structures to flower-like structures, and (2) CO2 capture capacity shifted by around 25%. As a result, the carbonate production and breakdown processes may be managed and improved using vapor steaming technology. These findings point to a new CO2 absorption technique and technology that might pave the way for more CO2 capture, mineralization, and fuel synthesis options. Full article
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18 pages, 4776 KiB  
Article
Blending Wastes of Marble Powder and Dolomite Sorbents for Calcium-Looping CO2 Capture under Realistic Industrial Calcination Conditions
by Paula Teixeira, Auguste Fernandes, Filipa Ribeiro and Carla I. C. Pinheiro
Materials 2021, 14(16), 4379; https://doi.org/10.3390/ma14164379 - 05 Aug 2021
Cited by 13 | Viewed by 1896
Abstract
The use of wastes of marble powder (WMP) and dolomite as sorbents for CO2 capture is extremely promising to make the Ca-looping (CaL) process a more sustainable and eco-friendly technology. For the downstream utilization of CO2, it is more realistic [...] Read more.
The use of wastes of marble powder (WMP) and dolomite as sorbents for CO2 capture is extremely promising to make the Ca-looping (CaL) process a more sustainable and eco-friendly technology. For the downstream utilization of CO2, it is more realistic to produce a concentrated CO2 stream in the calcination step of the CaL process, so more severe conditions are required in the calciner, such as an atmosphere with high concentration of CO2 (>70%), which implies higher calcination temperatures (>900 °C). In this work, experimental CaL tests were carried out in a fixed bed reactor using natural CaO-based sorbent precursors, such as WMP, dolomite and their blend, under mild (800 °C, N2) and realistic (930 °C, 80% CO2) calcination conditions, and the sorbents CO2 carrying capacity along the cycles was compared. A blend of WMP with dolomite was tested as an approach to improve the CO2 carrying capacity of WMP. As regards the realistic calcination under high CO2 concentration at high temperature, there is a strong synergetic effect of inert MgO grains of calcined dolomite in the blended WMP + dolomite sorbent that leads to an improved stability along the cycles when compared with WMP used separately. Hence, it is a promising approach to tailor cheap waste-based blended sorbents with improved carrying capacity and stability along the cycles under realistic calcination conditions. Full article
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