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Water System: Rapid Methane Gas Storage in Hydrates Burla Sai Kiran, Kandadai Sowjanya, Pinnelli S.R

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Water System: Rapid Methane Gas Storage in Hydrates Burla Sai Kiran, Kandadai Sowjanya, Pinnelli S.R Experimental investigations on tetrahydrofuran – methane – water system: Rapid methane gas storage in hydrates Burla Sai Kiran, Kandadai Sowjanya, Pinnelli S.R. Prasad, Ji-Ho Yoon To cite this version: Burla Sai Kiran, Kandadai Sowjanya, Pinnelli S.R. Prasad, Ji-Ho Yoon. Experimental investigations on tetrahydrofuran – methane – water system: Rapid methane gas storage in hydrates. Oil & Gas Science and Technology - Revue d’IFP Energies nouvelles, Institut Français du Pétrole, 2019, 74, pp.12. 10.2516/ogst/2018092. hal-01981692 HAL Id: hal-01981692 https://hal.archives-ouvertes.fr/hal-01981692 Submitted on 15 Jan 2019 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Oil & Gas Science and Technology - Rev. IFP Energies nouvelles 74, 12 (2019) Available online at: Ó B.S. Kiran et al., published by IFP Energies nouvelles, 2019 ogst.ifpenergiesnouvelles.fr https://doi.org/10.2516/ogst/2018092 REGULAR ARTICLE Experimental investigations on tetrahydrofuran – methane – water system: Rapid methane gas storage in hydrates Burla Sai Kiran1, Kandadai Sowjanya1, Pinnelli S.R. Prasad1,*, and Ji-Ho Yoon2 1 Gas Hydrate Division, CSIR – National Geophysical Research Institute (CSIR-NGRI), Hyderabad 500007, Telangana, India 2 Department of Energy and Resources Engineering and Department of Convergence Study on the Ocean Science and Technology, Ocean Science and Technology (OST) School, Korea Maritime and Ocean University, Busan 606-791, Korea Received: 10 September 2018 / Accepted: 20 November 2018 Abstract. This study reports methane (CH4) gas storage capacity along with TetraHydroFuran (THF) as guest molecules in mixed hydrates. This process has been studied in two reactors of 100 and 400 mL capacity, having 4.5 and 7.5 cm internal diameter respectively, in non-stirred configuration. Experiments were conducted in each reactor at constant initial gas pressure (7.5 MPa) and by increasing the height of the solution from 1 to 8 cm, resulting in volume scale-up factor of 5. The total CH4 gas uptake (moles) passes through a maximum at around 50% volume of the reactor indicating a transition from gas-rich to solution rich conditions. Observed variations in gas uptake are within ±20% of the maximum, upon different solution volume from 35% to 70% of reactor’s volume. Another set of experiments were conducted keeping the amount of the solution con- stant and increasing gas pressure in the range of 0.5–11.0 MPa. The gas uptake increased upon an increase in the gas pressure, but this is at least 40% less compared to the theoretical estimate. The stirring of solution or addition of promoter (Sodium Dodecyl Sulfate, SDS) is also not effective in increasing the gas consumption. Kinetics of gas uptake, in both stirred and non-stirred conditions, are quicker and 90% of gas consumption occurs in an hour after the hydrate nucleation event. 1 Introduction The research on gas hydrates in earlier days remained purely as a scientific curiosity. Of late it has become a topic Clathrate hydrates are the ice-like crystalline solids, often of great importance because of multi-facet applications in found in low temperature and high-pressure regions, namely the energy sector, e.g., natural gas hydrates could be an in the certain arctic zone and oceanic sediments. The water energy source, large storage capacity could be utilised for molecules transform into porous ice in the presence of smal- gas storage and transportation, of course, depending on ler hydrocarbons such as methane, ethane, propane, etc., or structural stability issues. Also, the property is much useful carbon dioxide; or hydrogen sulphide; and vacant pore to sequester the greenhouse gas such as carbon-dioxide [2–7]. spaces are occupied by these guest molecules. At the molec- In particular, storage of Natural Gas (NG), where the ular level, a network of water molecules forms various poly- dominant constituent is methane, is practised by different hedral cages through hydrogen bonding, and the guest methods, such as Liquefaction (LNG) or Compressed molecules are encased in cages. There are five types of poly- (CNG) or Adsorption (ANG) on suitable adsorbents or hedral cages, commonly found in hydrates, in increasing size: via clathrate hydrates (Solidified Natural Gas, SNG). pentagonal dodecahedron (512-cage), dodecahedron (435663- LNG has a volumetric capacity of about 600 v/v and is a cage), tetrakaidecahedron (51262-cage), hexakaidecahedron very active mode to transport NG from source to market, (51264-cage), and icosahedron (51268-cage). Three common but not suitable for storage due to stringent temperature unit cells (sI, sII, and sH) of gas hydrates are known to form requirements and the continuous gas boiloff issues [8]. from a few types of cages depending largely on the size and CNG (~200 v/v at 20 MPa) as a mode of storage requires physical properties of the guest species. For example, the high pressure for both production and storage and its sI unit lattice consists of two 512-cages and six 51262-cages, inherent flammable/explosive nature, practically makes it and the sII unit lattice has sixteen 512-cages and eight hazardous for NG storage. In contrast, ANG requires 51264-cages. The sH hydrate comprises three different cages: adsorbing NG onto sorbents, like, activated carbon, Carbon three 512-cages, two 435663-cages, and one 51268-cage [1]. Nanotubes (CNTs), graphene, Metal-Organic Frameworks (MOFs), etc. [9–12]. Given the history of the development * Corresponding author: [email protected] of these materials for NG storage and known scale-up This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. 2 B.S. Kiran et al.: Oil & Gas Science and Technology - Rev. IFP Energies nouvelles 74, 12 (2019) issues, there is a need to demonstrate process development. Veluswamy et al. [38, 39] have conducted studies on storage Furthermore, some of them are highly sensitive to moisture capacity and gas uptake kinetics in CH4 +THF+H2O [13]. On the other hand, solid hydrates of natural gas system and have reported process scale-up using three (SNG) are stable at moderately high pressure (5 MPa) different reactors, namely, in small (dia: 1.3 cm), medium and 279 K. Under the assumption of complete cage occu- (dia: 5.1 cm) and large (dia: 10.2 cm) using 2, 53 and pancy (8 in sI and 16 small in sII) of methane gas, one unit 220 mL of aq-THF solution at comparable methane gas of SNG upon dissociation can release 182 and 109 units of pressure. However, such scale-up is deceptive as both methane gas at 293 K and 0.1 MPa from sI and sII struc- diameter and volume (height) of the solution vary. Our tures. Thereby, the storage of gas in the form of SNG is a motivation is to investigate the hydrate formation process handy solution. The larger cages (51264) of sII in mixed with different amounts of aq-THF solution and initial gas hydrates are often occupied by the large co-guest molecules pressure to understand the role of surface area, the volume such as TetraHydroFuran (THF), resulting in significant of solution (height) and driving force (at a fixed volume of reduction in the methane gas volumetric storage capacity. solution) as these are a relevant parameter in the gas storage However, the thermodynamic stability conditions are vastly process. different than methane hydrates in sI [14]. However, noticeable drawbacks are in the form of the sluggish formation kinetics and inefficient water to hydrate 2 Experimental method conversion. The hydrates largely form at the gas-water interface and thus increase the surface area and helps in Figure 1 shows the schematic experimental layout attaining higher hydrate conversion. The common methods employed in our study. We used two different SS-316 for increasing clathrate formation kinetics, for example, use cylindrical reactor vessels of volume 100 and 400 mL for of high pressures (driving force), vigorous mechanical mix- these experiments. Cold fluid (water + glycol mixture) ing, surfactants, or micron-sized ground/sieved ice particles, was circulated in the vessel with the help of AN CYRO- can be adopted in the laboratory environment [2, 15–17]. LTCCB-40 circulator, to maintain the temperature inside Also, the hydrates formed in a porous medium have shown it at the desired level. A platinum resistance thermometer rapid and efficient gas storage [18–22]. But the process of (Pt100) inserted into the vessel was used to measure tem- mixing of reactants continuously may be less cost-effective peratures within ±0.2 K. The thermometer is placed in a and impractical in real gas storage applications. thermowell, which was fixed closer to the bottom surface In the current study, we use THF, a well-known sII of the reactor vessel and therefore the measured tempera- hydrate former, in stirred and unstirred configurations and ture is always in liquid/hydrate phase. The pressure in investigate the formation of mixed methane/THF hydrates the vessel was measured with a WIKA pressure transducer by systematically varying aq-THF amount keeping initial (WIKA, type A-10 for pressure range 0–16 MPa) and this gas pressure at 7.5 MPa and also varying the initial methane sensor measures the variations in the vapour phase.
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