Adsorbents For Carbon Dioxide Capture Research Articles

Oxidation-stable amine-containing adsorbents for carbon dioxide capture

Amine-containing solids have been investigated as promising adsorbents for CO2 capture, but the low oxidative stability of amines has been the biggest hurdle for their practical applications. Here, we developed an extra-stable adsorbent by combining two strategies. First, poly(ethyleneimine) (PEI) was functionalized with 1,2-epoxybutane, which generates tethered 2-hydroxybutyl groups. Second, chelators were pre-supported onto a silica support to poison p.p.m.-level metal impurities (Fe and Cu) that catalyse amine oxidation. The combination of these strategies led to remarkable synergy, and the resultant adsorbent showed a minor loss of CO2 working capacity (8.5%) even after 30 days aging in O2-containing flue gas at 110 °C. This corresponds to a ~50 times slower deactivation rate than a conventional PEI/silica, which shows a complete loss of CO2 uptake capacity after the same treatment. The unprecedentedly high oxidative stability may represent an important breakthrough for the commercial implementation of these adsorbents.

Preparation and Properties of A Hyperbranch-Structured Polyamine adsorbent for Carbon Dioxide Capture

A fibrous adsorbent with amino-terminated hyperbranch structure (PP-AM-HBP-NH2) was prepared by grafting hyperbranched polyamine (HBP-NH2) onto the acrylamide-modified polypropylene (PP) fibers. The grafting of AM on PP fibers provided the active sites for introducing HBP-NH2 onto the PP fibers. This kind of “grafting to” procedure to synthesize hyperbranch-structured fiber could overcome the disadvantages of stepwise growth procedure, avoiding the complicated synthesis process and the requirement of strict experimental conditions. The grafted HBP-NH2 was three-dimensional dentritic architecture and had a large number of pores existing within the grafted polymers, which is favorable for CO2 molecules to diffuse into the HBP-NH2. Therefore, the as-prepared PP-AM-HBP-NH2 fibers showed a high adsorption capacity (5.64 mmol/g) for CO2 in the presence of water at 25 °C, and the utilization efficiency of alkyl amino groups could reach 88.2%, demonstrating that the hyperbranched structure of adsorbents can greatly promote adsorption capacity and efficiency. This could be attributed to better swelling properties and lower mass transfer resistance to CO2 of the hyperbranched adsorbent. PP-AM-HBP-NH2 also showed excellent regeneration performance, and it could maintain the same adsorption capacity for CO2 after 15 recycle numbers as the fresh adsorbent.

Simple template-free synthesis of high surface area mesoporous ceria and its new use as a potential adsorbent for carbon dioxide capture

The development of an efficient technique for carbon dioxide (CO2) capture from a variety of large stationary sources is in important global issue. If we are to achieve an energy-efficient and effectively higher CO2 capture process based on an adsorption approach, we need new adsorbent materials realistic enough to provide higher CO2 loading on a volumetric basis. For this reason we have focused on the practical use of high surface area mesoporous ceria as a new application in the field of CO2 capture. In this regard, we demonstrate the simple and inexpensive template-free synthesis of mesoporous ceria with a high surface area up to 200m2g−1, and characterize it as an effective CO2 adsorbent for the first time. The mesoporous ceria is prepared based on sol–gel chemistry, where the product is simply precipitated by the self-assembly of ceria nanoparticles within a short reaction period at room temperature under highly alkaline conditions with optimized chemical compositions. The results of CO2 adsorption–desorption measurement at 298K show that the obtained ceria with an enhanced surface area exhibits a noticeably higher CO2 adsorption capacity per volume than commercially available non-porous ceria, activated carbon and zeolite 13X over a wide pressure range with robust stability as well as regenerability. This work enables us to prepare promising new materials for the CO2 capture process based on an easy-to-handle synthesis system, and this effective material will have a broad applicability to the efficient CO2 separation from variety of industrial emission sources. The features of the obtained mesoporous ceria are reported and discussed.

Oxidative Stability of Amino Polymer–Alumina Hybrid Adsorbents for Carbon Dioxide Capture

Amine/oxide hybrid carbon dioxide adsorbents prepared via impregnation of low molecular weight polymeric amines into porous oxide supports are among the most promising solid adsorbents developed for postcombustion CO2 capture or CO2 extraction from ambient air. The oxidative stability of adsorbents prepared by impregnation of poly(ethylenimine) (PEI) or poly(allylamine) (PAA) into mesoporous γ-alumina under humid oxidation conditions is evaluated in this work. The PEI-based adsorbents, which contain primary, secondary, and tertiary amines, are shown to degrade drastically at elevated temperatures (110 °C) and in high oxygen concentrations (21%, akin to air), with these effects reduced by both reductions in temperature (70 °C) and oxygen concentration (5%, akin to flue gas). The oxidation behavior of PEI-based adsorbents supported on alumina is qualitatively similar to past work on silica-supported PEI adsorbents. In contrast, the alumina-supported PAA adsorbents that contain only primary amines show signi...

Development of solid adsorbent for carbon dioxide capture from flue gas

The adsorption of carbon dioxide (CO2) from simulated flue gas using newly developed solid adsorbents has been studied in the present work. Adsorptive capture of CO2 from flue gas streams is a promising technology for greenhouse gas mitigation. The success of CO2 capture using solid sorbents is greatly dependent on the development of a low cost, regenerable sorbent with high CO2 adsorption capacity. Solid sorbent is expected to offer the benefits over the liquid amines used in the typical absorption process, with the added advantages that solids do not give corrosion problems like liquid amines. In the present study, alkali-impregnated meso-porous solid sorbents have been developed and their performances for CO2 capture from simulated flue gas were evaluated by using a fixed bed reactor. The effect of various process parameters like temperature, CO2 concentration and loading of active component has been studied. The adsorbent with 20wt% Na2CO3 loading have shown the best CO2 adsorption capacity among the studied adsorbents and the adsorption capacity lies in the range of 0.35–0.39mmol/g of adsorbent at a temperature of about 55°C and atmospheric pressure.

Carbon nanotube modified carbon composite monoliths as superior adsorbents for carbon dioxide capture

Carbon composite monoliths were prepared from a commercial phenolic resin mixed with just 1 wt% of carbon nanotubes (CNTs) followed by carbonization and physical activation with CO2. The products possess a hierarchical macroporous–microporous structure and superior CO2 adsorption properties. In particular, they show the top-ranked CO2 capacity (52 mg CO2 per g adsorbent at 25 °C and 114 mmHg) under low CO2 partial pressures, which is of more relevance for flue gas applications. This matches or exceeds those of carbons produced by complex chemical activation and functionalization. Our study demonstrates an effective way to create narrow micropores through structural modification of carbon composites by CNTs.

MgO-modified mesoporous silicas impregnated by potassium carbonate for carbon dioxide adsorption

Mesoporous adsorbents for carbon dioxide capture were prepared by introducing of magnesium oxide and potassium carbonate into SBA-15, SBA-16 silicas and MCM-48-like-silica. In order to avoid destruction of silica supports, a novel procedure based on the precipitation of magnesium acetate on the silica surface was developed. Subsequent in situ chemical conversion of magnesium acetate provided magnesium oxalate, while final magnesium oxide was formed by calcination. To introduce potassium carbonate, silica modified with MgO was impregnated with potassium oxalate followed by its conversion to carbonate. All prepared mesoporous adsorbents preserved characteristic features of mesoporous molecular sieve.The comparison of carbon dioxide isotherms obtained on prepared samples reveals that their adsorption properties are decisively influenced by the type of mesoporous structure. Modified sample of SBA-15 silica has shown the most steep adsorption isotherm and higher CO2 adsorption capacity than adsorption capacity of samples prepared from SBA-16 and MCM-48-ls silicas.

Stability Effects on CO2 Adsorption for the DOBDC Series of Metal–Organic Frameworks

Metal-organic frameworks with unsaturated metal centers in their crystal structures, such as Ni/DOBDC and Mg/DOBDC, are promising adsorbents for carbon dioxide capture from flue gas due to their high CO(2) capacities at subatmospheric pressures. However, stability is a critical issue for their application. In this paper, the stabilities of Ni/DOBDC and Mg/DOBDC are investigated. Effects of steam conditioning, simulated flue gas conditioning, and long-term storage on CO(2) adsorption capacities are considered. Results show that Ni/DOBDC can maintain its CO(2) capacity after steam conditioning and long-term storage, whereas Mg/DOBDC does not. Nitrogen isotherms for Mg/DOBDC show a drop in surface area after steaming, corresponding to the decrease in CO(2) adsorption, which may be caused by a reduction of unsaturated metal centers in its structure. Conditioning with dry simulated flue gas at room temperature only slightly affects CO(2) adsorption in Ni/DOBDC. However, introducing water vapor into the simulated flue gas further reduces the CO(2) capacity of Ni/DOBDC.

Carbon dioxide adsorption over DIPA functionalized MCM-41 and SBA-15 molecular sieves

The capture of carbon dioxide was carried out using MCM-41 and SBA-15 as adsorbents. These mesoporous materials were synthesized by the hydrothermal method, and subsequently functionalized with the di-iso-propylamine (DIPA). Then, they were characterized by XRD, BET, and TG/DTG. The X-ray diffraction patterns of the synthesized samples showed the characteristic peaks of MCM-41 and SBA-15, indicating that the structures of these materials were obtained. The functionalized samples presented a decrease of the intensities of these peaks, suggesting a decreasing in the structural organization of the material; however, the mesoporous structure was preserved. For the adsorption capacity measurements, the materials were previously saturated with carbon dioxide at 75 °C, and then desorbed in a thermobalance in the temperature range of 25–900 °C, under helium atmosphere. Desorption tests showed that the functionalized MCM-41 presented a weight loss of 7.5 wt%, against 5.9 wt% for SBA-15. The obtained values indicate that these nanostructured materials can be used as adsorbent for carbon dioxide capture.

Adsorption of carbon dioxide using polyethyleneimine modified silica gel

To find an ideal adsorbent for carbon dioxide capture, a new polyethyleneimine modified silica gel material was synthesized with a simple procedure. Three silica gel materials with various particle sizes (15, 25 and 40–63 μm) were prepared and functionalized with polyethyleneimine. The carbon dioxide adsorption amounts of modified silica gel and non-modified silica gel were calculated using a mass balance equation at three different temperatures (298.15, 308.15 and 318.15 K), respectively, and the influence of gas pressure and particle size on adsorption was discussed. Experimental data showed that the carbon dioxide adsorption capacity of modified silica gel was better than non-modified silica gel, and the adsorption capacity gradually decreased with increasing particle size. The smaller particle size (15 μm) PEI modified silica gel had the largest adsorption capacity, at 298.15 K, and the adsorption amounts of various particle sizes of PEI-silica better fit the Langmuir isotherm model.

Preparation and adsorption properties of polyethylenimine containing fibrous adsorbent for carbon dioxide capture

AbstractWe successfully prepared a novel fibrous adsorbent for carbon dioxide (CO2) capture by coating polyethylenimine (PEI) on a glass fiber matrix, using epoxy resin (EP) as crosslinking agent. The physicochemical properties of the fibrous adsorbents were characterized in terms of Fourier transform infrared spectrometry and thermogravimetric analysis. Factors that affected the adsorption capacity of the fibrous adsorbent were studied, including the crosslinking agent dosage, coating weight, moisture, adsorption temperature, and CO2 concentration of the simulated flue gas. The experimental results indicate that the properly crosslinked fibrous adsorbent had a high thermal stability at about 280°C. With a PEI/EP ratio of 10:1, a maximum adsorption capacity of 276.96 mg of CO2/g of PEI was obtained at 30°C. Moisture had a promoting influence on the adsorption of CO2 from flue gas. The CO2 adsorption capacity of the fibrous adsorbent in the presence of moisture could be 19 times higher than that in dry conditions. The fibrous adsorbent could be completely regenerated at 120°C. The CO2 adsorption capacity of the regenerated fibrous adsorbent was almost the same as that of the fresh adsorbent. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008