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Characterization Study of CO2, CH4, and CO2/CH4 Hydroquinone Clathrates Formed by Gas–Solid Reaction

Coupan, Romuald and Péré, Eve and Dicharry, Christophe and Plantier, Frédéric and Diaz, Joseph and Khoukh, Abdel and Allouche, Joachim and Labat, Stephane and Pellerin, Virginie and Grenet, Jean-Paul and Sotiropoulos, Jean-Marc and Senechal, Pascale and Guerton, Fabrice and Moonen, Peter and Torré, Jean-Philippe Characterization Study of CO2, CH4, and CO2/CH4 Hydroquinone Clathrates Formed by Gas–Solid Reaction. (2017) Journal of Physical Chemistry C, 121 (41). 22883-22894. ISSN 1932-7447

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Official URL: https://doi.org/10.1021/acs.jpcc.7b07378

Abstract

Hydroquinone (HQ) is known to form organic clathrates with some gaseous species such as CO2 and CH4. This work presents spectroscopic data, surface and internal morphologies, gas storage capacities, guest release temperatures, and structural transition temperatures for HQ clathrates obtained from pure CO2, pure CH4, and an equimolar CO2/CH4 mixture. All analyses are performed on clathrates formed by direct gas–solid reaction after 1 month’s reaction at ambient temperature conditions and under a pressure of 3.0 MPa. A collection of spectroscopic data (Raman, FT-IR, and 13C NMR) is presented, and the results confirm total conversion of the native HQ (α-HQ) into HQ clathrates (β-HQ) at the end of the reaction. Optical microscopy and SEM analyses reveal morphology changes after the enclathration reaction, such as the presence of surface asperities. Gas porosimetry measurements show that HQ clathrates and native HQ are neither micro- nor mesoporous materials. However, as highlighted by TEM analyses and X-ray tomography, α- and β-HQ contain unsuspected macroscopic voids and channels, which create a macroporosity inside the crystals that decreases due to the enclathration reaction. TGA and in situ Raman spectroscopy give the guest release temperatures as well as the structural transition temperatures from β-HQ to α-HQ. The gas storage capacity of the clathrates is also quantified by means of different types of gravimetric analyses (mass balance and TGA). After having been formed under pressure, the characterized clathrates exhibit exceptional metastability: the gases remain in the clathrate structure at ambient conditions over time scales of more than 1 month. Consequently, HQ gas clathrates display very interesting properties for gas storage and sequestration applications.

Item Type:Article
HAL Id:hal-01679472
Audience (journal):International peer-reviewed journal
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Institution:French research institutions > Centre National de la Recherche Scientifique - CNRS (FRANCE)
Other partners > Total (FRANCE)
Other partners > Université de Pau et des Pays de l'Adour - UPPA (FRANCE)
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Deposited On:15 Feb 2019 13:08

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