Development of carbon-based adsorbent for separation of impurities such as siloxane and ammonia from land-fill gas

Land-fill gas or bio-gas is composed of large portion of methane and carbon dioxide, and small amount of impurities such as nitrogen, oxygen, hydrogen sulfide, siloxane and ammonia. These gases can be used as a gas-fuel after upgrading treatment. For the application of the land-fill gas and bio-gas as a fuel, we developed highly-performing carbon-based adsorbent which can separate siloxane and ammonia residue from these gases. It was quite necessary to consider the chemical properties of siloxane and ammonia for development of suitable adsorbent of each component. The siloxane can be polymerized in acidic or basic condition to form bulkier species which causes adsorbent deactivation and difficult regeneration. The ammonia gas is well known as basic molecules which have strong affinity to acidic species. In these reasons, we prepared neutral carbon materials by various methods for siloxane adsorption. In addition, we developed carbon-based basic ammonia-adsorbent by simple methods such as the chemical treatment of commercial activated carbon or the impregnation of organic molecules into the activated carbon. And then, adsorption-desorption isotherms and breakthrough curve of siloxane and ammonia were measured for thus synthesized adsorbents. Detail results for synthesis and the adsorption measurement of the studied adsorbents will be presented in the conference

Adsorptive removal of CO2 from CO2-CH4 mixture using cation-exchanged zeolites

Raw natural gas and landfill gas contains methane as its major component, but it also contains considerable amounts of contaminants such as CO2 and H2S (i.e. acid gases) that can cause corrosion and fouling of the pipeline and equipment during transportation and liquefaction. Amine-based CO2 gas removal processes have been employed in the gas industry, but these processes have disadvantages including high regeneration energy requirements and inefficiencies; these issues have not been adequately solved to date. Currently, adsorptive acid gas removal technologies have received significant interest because of the simplicity of adsorbent regeneration by thermal or pressure variation1). Numerous micro- and mesoporous adsorbents including zeolites [2-3], titanosilicates[4], activated carbons[5-6], metal-organic-framework (MOF) [7], and silica-alumina materials[8-9] were studied for this type of application. However, the CO2/CH4 selectivity of the aforementioned adsorbents was not high enough for commercial applications.In this study, different cation-exchanged zeolites were synthesized, physicochemically characterized, and evaluated for adsorptive removal of CO2 from CO2-CH4 mixtures. The adsorption isotherms of CO2 and CH4 in the pressure and temperature ranges 0 − 3MPa and 10 – 40 oC, respectively, for different cation-exchanged zeolites were measured and compared. The ideal-adsorbed solution theory (IAST) was employed for the estimation of CO2/CH4 selectivity for the different cation-exchanged zeolites. References 1) D. Aaron, C. Tsouris, Separ. Sci. Technol. 2005, 40, 321–348 2) J. Collins, US Patent No. 3,751,878. 1973. 3) M. W. Seery, US Patent No. 5,938,819. 1999 4) W. B. Dolan, M.J. Mitariten, US Patent No. 6,610,124 B1. 2003 5) A. Kapoor, R.T. Yang, Chem. Eng. Sci. 1989, 44, 1723–1733 6) A. Jayaraman, Chiao, A. S.; Padin, J.; Yang, R. T.; Munson, C. L., Separ. Sci. Technol. 2002 37, 2505–2528 7) L. Hamon, E. Jolimaitre, G. Pringruber , Ind. Eng. Chem. Res. 2010, 49, 7497-7503 8) W.B. Dolan, M.J. Mitariten, US patent No. 2003/0047071, 2003 9) G. Bellussi, P. Broccia, A. Carati, R. Millini, P. Pollesel, C. Rizzo, M. Tagliabue, Micropor. Mesopor. Mat., 2011, 146, 134–14

High catalytic performance of surfactant-directed nanocrystalline zeolites for liquid-phase Friedel-Crafts alkylation of benzene due to external surfaces

Beta zeolite is known as an efficient catalyst for Friedel-Crafts alkylation. In liquid phase reactions, however, beta zeolite catalyst is often deactivated rapidly. We discovered that the maximum possible catalytic turnovers in benzene alkylation with benzyl alcohol could be increased by six times by using a beta zeolite with a nanosponge-like morphology, in comparison to bulk beta zeolites. The nanomorphic zeolite was obtained using a hydrothermal synthesis method which uses multiammonium surfactants as a meso-micro hierarchical structure-directing agent. The origins of the high catalytic performance were investigated by measuring the catalytic conversions after selectively poisoning acid sites located on external surfaces and in internal micropores selectively. The result indicated that the high catalytic performance was due to the alkylation reactions occurring on external surfaces. External active sites were able to perform the catalytic function even after active sites inside the zeolite micropores were deactivated. Similar results were obtained with other nanomorphic zeolites such as MFI nanosheets, MTW nanosponge and MRE nanosponge. © 2013 Elsevier Ltd. All rights reserved.134361sciescopu

MFI zeolite nanosponges possessing uniform mesopores generated by bulk crystal seeding in the hierarchical surfactant-directed synthesis

The synthesis of a mesoporous material with uniform mesopore diameters and crystalline MFI zeolite walls has been achieved, simply by seeding the multiammonium surfactant-directed synthesis with bulk zeolite crystals. The bulk seeds disappeared in the final product. As a result of seeding, the mesoporous zeolites could be generated rapidly even at high Al content. © the Partner Organisations 2014.133361sciescopu

Characterization of the Surface Acidity of MFI Zeolite Nanosheets by 31P NMR of Adsorbed Phosphine Oxides and Catalytic Cracking of Decalin

MFI zeolite nanosheets tailored to 2.5-nm thickness were synthesized using a surfactant-type zeolite structure-directing agent, [C22H45−N+(CH3)2−C6H12−N+(CH3)2−C6H13](Br−)2. The zeolite nanosheets possessed Brønsted acid sites on their external surfaces as well as in the internal micropore walls. The acid strength and concentration was characterized by the 31P NMR signals of the adsorbed trimethylphosphine oxide and tributylphosphine oxide. The 31P NMR investigation identified three types of Brønsted acid sites with different strengths on external surfaces; there were four types inside the micropores. A linear correlation has been established between the number of the external strongest acid sites and the catalytic activity in decalin cracking for the MFI zeolite catalysts investigated in this work.174781sciescopu

Physical Separation of Contaminated Soil Using a Washing Ejector Based on Hydrodynamic Cavitation

A washing ejector is a pre-treatment technology used to remediate contaminated soil by separating fine particles. The washing ejector developed in this study is a device that utilizes fast liquid jets to disperse soil aggregates by cavitation flow. The cavitation phenomenon is affected by the Bernoulli principle, and the liquid pressure decreases with the increase in kinetic energy. The cavitating flow of the fluid through the Ventrui nozzle can remove surface functional groups and discrete particles. The main methodology involves the removal of small particles bound to coarse particles and the dispersion of soil aggregates. Particle collisions occur on the surface soil, such as the metal phase that is weakly bound to silicate minerals. It was observed that the dispersed soil affected the binding of toxic heavy metals and the mineralogical characteristics of the soil. The quantity of oxides, organic matter, and clay minerals affected the properties of the soil. An almost 40–60% removal efficiency of total metals (As, Zn, and Pb) was obtained from the contaminated soils. After treatment by a washing ejector, the volume of fine particles was reduced by 28–47%. When the contaminants are associated with particulates, separation using a washing ejector can be more effective. Therefore, physical separation improves the removal efficiency of heavy metals from soil aggregates

Mesopore wall-catalyzed Friedel-Crafts acylation of bulky aromatic compounds in MFI zeolite nanosponge

We investigated the effects of mesopore generation in a MFI zeolite when used as a catalyst in liquid-phaseFriedel.Crafts acylation reactions of bulky aromatic compounds. For this investigation, we obtained anMFI zeolite with nanosponge morphology, following a seed-assisted hydrothermal synthesis route usingC22H45.N+(CH3)2.C6H12.N+(CH3)2.C6H13. The zeolite nanosponge exhibited a narrow distribution ofmesopore diameters centered at 4 nm, in which the mesopores were built with a disordered networkof 2.5-nm thick MFI zeolite layers. This zeolite exhibited high catalytic performance in various acylationreactions, compared with bulk MFI zeolites, beta zeolite and mesoporous materials composed of amor-phous aluminosilicates. The high catalytic performance corresponded to the strong Bronsted acid sitesexisting on the mesopore walls. © 2014 Elsevier B.V. All rights reserved111111sciescopu

Exploring Mass Transfer in Mesoporous Zeolites by NMR Diffusometry

With the advent of mesoporous zeolites, the exploration of their transport properties has become a task of primary importance for the auspicious application of such materials in separation technology and heterogeneous catalysis. After reviewing the potential of the pulsed field gradient method of NMR (PFG NMR) for this purpose in general, in a case study using a specially prepared mesoporous zeolite NaCaA as a host system and propane as a guest molecule, examples of the attainable information are provided

Remediation of Toxic Heavy Metal Contaminated Soil by Combining a Washing Ejector Based on Hydrodynamic Cavitation and Soil Washing Process

Based on the features of hydrodynamic cavitation, in this study, we developed a washing ejector that utilizes a high-pressure water jet. The cavitating flow was utilized to remove fine particles from contaminated soil. The volume of the contaminants and total metal concentration could be correlated to the fine-particle distribution in the contaminated soil. These particles can combine with a variety of pollutants. In this study, physical separation and soil washing as a two-step soil remediation strategy were performed to remediate contaminated soils from the smelter. A washing ejector was employed for physical separation, whereas phosphoric acid was used as the washing agent. The particles containing toxic heavy metals were composed of metal phase encapsulated in phyllosilicates, and metal phase weakly bound to phyllosilicate surfaces. The washing ejector involves the removal of fine particles bound to coarse particles and the dispersion of soil aggregates. From these results we determined that physical separation using a washing ejector was effective for the treatment of contaminated soil. Phosphoric acid (H3PO4) was effective in extracting arsenic from contaminated soil in which arsenic was associated with amorphous iron oxides. Thus, the obtained results can provide useful information and technical support for field soil washing for the remediation of soil contaminated by toxic heavy metals through emissions from the mining and ore processing industries