Selectivity and CO 2 capture efficiency in CO 2 -N 2 clathrate hydrates investigated by in-situ Raman spectroscopy

Chazallon, Bertrand; Pirim, Claire

doi:10.1016/j.cej.2018.01.116

Cited by 72 publications

(32 citation statements)

References 66 publications

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“…Thus, no CO 2 -rich liquid phase is possible to form since the CO 2 composition of our gas mixtures is always low enough and the temperatures high enough. Moreover, a very recent study based on Raman spectroscopic measurements highlighted that a CO 2 -N 2 gas mixture needs to contain a minimum of 98 mol-% N 2 to coexist with a structure II gas hydrate [39]. Thus, all gas hydrates are considered as structure I gas hydrate when the CO 2 -N 2 -CH 4 gas mixture was used.…”

Section: Phase Equilibrium Of Mixed Gas Hydratesmentioning

confidence: 99%

Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH4, CO2 and N2: Phase Equilibrium in the Presence of Excess Water and Gas Exchange

et al. 2018

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This article presents gas hydrate experimental measurements for mixtures containing methane (CH 4 ), carbon dioxide (CO 2 ) and nitrogen (N 2 ) with the aim to better understand the impact of water (H 2 O) on the phase equilibrium. Some of these phase equilibrium experiments were carried out with a very high water-to-gas ratio that shifts the gas hydrate dissociation points to higher pressures. This is due to the significantly different solubilities of the different guest molecules in liquid H 2 O. A second experiment focused on CH 4 -CO 2 exchange between the hydrate and the vapor phases at moderate pressures. The results show a high retention of CO 2 in the gas hydrate phase with small pressure variations within the first hours. However, for our system containing 10.2 g of H 2 O full conversion of the CH 4 hydrate grains to CO 2 hydrate is estimated to require 40 days. This delay is attributed to the shrinking core effect, where initially an outer layer of CO 2 -rich hydrate is formed that effectively slows down the further gas exchange between the vapor phase and the inner core of the CH 4 -rich hydrate grain.

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Section: Phase Equilibrium Of Mixed Gas Hydratesmentioning

confidence: 99%

Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH4, CO2 and N2: Phase Equilibrium in the Presence of Excess Water and Gas Exchange

et al. 2018

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“…The molecular sizes of CO2 and N2 are different, so CO2 form typical structure I (sI) hydrates, and N2 form typical structure II (sII) hydrates. The Raman shifts of pure CO2 hydrates occur at about 1276.6 and 1381.1 cm −1 , whereas the Raman shift of N2 is about 2324.5 cm −1 [30]. For hydrates with multicomponent guest molecules, a different hydrate structure can form, and the Raman displacement will be correspondingly affected.…”

Section: Resultsmentioning

confidence: 99%

Experimental Investigation of the Hydrate-Based Gas Separation of Synthetic Flue Gas with 5A Zeolite

et al. 2020

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Coal combustion flue gas contains CO2, a greenhouse gas and driver of climate change. Therefore, CO2 separation and removal is necessary. Fortunately, 5A zeolites are highly porous and can be used as a CO2 adsorbent. In addition, they act as nuclei for hydrate formation. In this work, a composite technology, based on the physical adsorption of CO2 by 5A zeolite and hydrate-based gas separation, was used to separate CO2/N2 gas mixtures. The influence of water content, temperature, pressure, and particle size on gas adsorption and CO2 separation was studied, revealing that the CO2 separation ability of zeolite particles sized 150–180 μm was better than that of those sized 380–830 μm at 271.2 K and 273.2 K. When the zeolite particles were 150–180 μm (type-B zeolite) with a water content of 35.3%, the gas consumption per mole of water (ngas/nH2O ) reached the maximum, 0.048, and the CO2 separation ratio reached 14.30%. The CO2 molar concentration in the remaining gas phase (xCO2gas) was lowest at 271.2 K in the type-B zeolite system with a water content of 47.62%. Raman analysis revealed that CO2 preferentially occupied the small hydrate cages and there was a competitive relationship between N2 and CO2.

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“…To examine the selectivity of the CO 2 over N 2 , CO 2 /(CO 2 + N 2 ) ratio with time after pressure set is presented in Fig. 2f showing a decrease with time, indicating stronger selectivity of the CO 2 over N 2 in all the experiments owing to relatively higher 27,28 stability of CO 2 than N 2 at the hydrate phase. This shows relatively higher occupancy of large cavities than small cavities.…”

Section: Resultsmentioning

confidence: 99%

An Experimental Investigation on the Kinetics of Integrated Methane Recovery and CO2 Sequestration by Injection of Flue Gas into Permafrost Methane Hydrate Reservoirs

Hassanpouryouzband

Yang

Okwananke

et al. 2019

Sci Rep

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Large hydrate reservoirs in the Arctic regions could provide great potentials for recovery of methane and geological storage of CO2. In this study, injection of flue gas into permafrost gas hydrates reservoirs has been studied in order to evaluate its use in energy recovery and CO2 sequestration based on the premise that it could significantly lower costs relative to other technologies available today. We have carried out a series of real-time scale experiments under realistic conditions at temperatures between 261.2 and 284.2 K and at optimum pressures defined in our previous work, in order to characterize the kinetics of the process and evaluate efficiency. Results show that the kinetics of methane release from methane hydrate and CO2 extracted from flue gas strongly depend on hydrate reservoir temperatures. The experiment at 261.2 K yielded a capture of 81.9% CO2 present in the injected flue gas, and an increase in the CH4 concentration in the gas phase up to 60.7 mol%, 93.3 mol%, and 98.2 mol% at optimum pressures, after depressurizing the system to dissociate CH4 hydrate and after depressurizing the system to CO2 hydrate dissociation point, respectively. This is significantly better than the maximum efficiency reported in the literature for both CO2 sequestration and methane recovery using flue gas injection, demonstrating the economic feasibility of direct injection flue gas into hydrate reservoirs in permafrost for methane recovery and geological capture and storage of CO2. Finally, the thermal stability of stored CO2 was investigated by heating the system and it is concluded that presence of N2 in the injection gas provides another safety factor for the stored CO2 in case of temperature change.

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Selectivity and CO 2 capture efficiency in CO 2 -N 2 clathrate hydrates investigated by in-situ Raman spectroscopy

Cited by 72 publications

References 66 publications

Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH4, CO2 and N2: Phase Equilibrium in the Presence of Excess Water and Gas Exchange

Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH4, CO2 and N2: Phase Equilibrium in the Presence of Excess Water and Gas Exchange

Experimental Investigation of the Hydrate-Based Gas Separation of Synthetic Flue Gas with 5A Zeolite

An Experimental Investigation on the Kinetics of Integrated Methane Recovery and CO2 Sequestration by Injection of Flue Gas into Permafrost Methane Hydrate Reservoirs

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