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• W2783154581 abstract "This thesis explores novel adsorbents for separation of three different types of gas mixtures found in liquified natural gas processes (a) CO2 from CH4 and N2, (b) CH4 from N2, and (c) helium from N2 and CH4. These separations represent challenging operations in natural gas processing because the conventional technologies to remove CO2 such as amine absorption units, reject N2 and recovery helium by cryogenic distillation are capital and energy intensive. Cyclic adsorption processes such as pressure swing adsorption (PSA) have potential as alternative technologies to reduce equipment costs and improve energy efficiency in liquified natural gas (LNG) production facilities, especially for small-scale plants. However, there are several challenges related to the development of adsorbents required to advance PSA technologies for natural gas processing. These include the development of adsorbents with excellent selectivity, low-pressure drops, and low production costs. Chapters 4 and 5 of the thesis report novel carbon foam monoliths that have several potential advantages such as lower pressure drops, better heat transfer properties, lower void fractions and higher mechanical strength in fixed-bed adsorption processes over pellets or granular adsorbents. In Chapter 4 I report pitch-derived carbon foam monoliths, and in this chapter I investigated the effects of using coal as a filler particle and the amount of potassium hydroxide on the stability of tar pitch during the foaming process, the product’s density, and the micropore structure. These pitch-derived carbon monoliths featured an open-cell structure and a well-developed microporosity that presented a BET specific surface area of 1044 m2.g-1. At 298 K and pressures close to 3500 kPa the adsorption capacities of the carbon monolith prepared with 50 %wt coal to pitch were 7.398 mmol.g-1 CO2, 5.049 mmol.g-1 CH4, and 3.516 mmol.g-1 N2. The second type of carbon foam developed in this thesis was a monolithic carbon foam with an open cellular structure that was synthesized from banana peel using a soft-template method with zinc nitrate, furfural, and 2-aminophenol (Chapter 5). I extended the experimental methods to investigate the effects of (a) carbonization temperature and (b) post-carbonization CO2 activation to enhance the microporosity of the carbon foams as adsorbents for CO2 capture. The CO2-activated carbon foams featured BET surface areas up to 1426 m2.g-1. The effect of surface chemistry and N-containing functional groups on the CO2 uptake was also investigated and it was showed that both nitrogen functional groups and microporosity are critical parameters in equilibrium CO2 absorption of the carbon foams. To evaluate the potential of these carbon foams as adsorbents for gas separation, the adsorption capacity of the carbon foams for CO2 and N2 were measured by a gravimetric sorption. At 298 K and pressures of 3990 kPa, the carbon foam synthesized at 1273 K in CO2 adsorbed 9.21 mmol.g-1 of CO2 and 3.29 mmol.g-1 of N2. Although the synthesized carbon foams show promising CO2 adsorption capacity and reasonable CO2 selectivity over N2, the selectivity of these carbons for CO2/CH4 and CH4/N2 was not as high as selectivities reported for zeolitic imidazolate frameworks (ZIFs). The ZIF-7 is known to exhibit a gate opening phase change in the presence CO2, and this behavior is associated with ZIF-7’s flexible framework. Chapter 6 reports for the first time experimental measurements to show that CH4 can also induce a gate opening effect in ZIF-7. The step change in CH4 adsorption associated with gate opening was observed at a pressure of 1500 kPa in the isotherm measured at 303 K, and with this behavior, the IAST selectivity of ZIF-7 for CH4 from an equimolar CH4 + N2 mixture was more than 10. At 303 K the step in the CO2 isotherm was observed at approximately 100 kPa which provides an equilibrium selectivity of 24 for CO2 over CH4 and 101 for CO2 over N2. In Chapter 7, I investigated the adsorption of helium on narrow micropore adsorbents including a clinoptilolite-rich natural zeolite (Escott), zeolite 3A, zeolite 4A and a carbon molecular sieve (CMS 3K-172). The helium adsorption procedure extends the previous works by Gumma and Talu* to determine the impenetrable solid volume of the adsorbent, which in standard helium pycnometry is determined under the assumption that helium does not adsorb at room temperature. I measured helium adsorption capacities and the true specific impenetrable solid volumes of the adsorbents by a gravimetric method at pressures of (300 - 3500) kPa and temperatures in the range of (303 - 343) K. The results confirm helium adsorption on these solids is small, but not zero: equilibrium helium adsorption capacities measured at 3500 kPa and 303 K were 0.067 mmol.g-1 on Escott, 0.085 mmol.g -1 on 3A, 0.096 mmol.g-1 on 4A and 0.089 mmol.g-1 on 3K-172. The specific solid volumes determined by the Gumma and Talu method were 10 – 15 % larger than the specific solid volumes measured by standard helium pycnometry, and this error can result in uncertainties of 2.6 – 28 % in the equilibrium adsorption capacities of CO2 and N2 measured at high pressures. * Gumma, S.; Talu, O., Gibbs Dividing Surface and Helium Adsorption. Adsorption 2003, 9 (1), 17-28." @default.
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• W2783154581 date "2017-10-04" @default.
• W2783154581 modified "2023-09-24" @default.
• W2783154581 title "Novel adsorbents for natural gas separation and purification" @default.
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• W2783154581 doi "https://doi.org/10.14264/uql.2017.873" @default.
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