Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study

• Published in: ACS Sustainable Chemistry & Engineering
• Main Authors: Omran, Ahmed, Nesterenko, Nikolay, Valtchev, Valentin
• Other Authors: Université de Caen Normandie (UNICAEN), Normandie Université (NU), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Laboratoire catalyse et spectrochimie (LCS), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS), TotalEnergies OneTech Belgium, Centre National de la Recherche Scientifique (CNRS)
• Format: Article in Journal/Newspaper
• Language: English
• Published: HAL CCSD 2022
• Subjects: Zeolitic ice; Acidic zeolites; Kinetic hydrate promoters; DFT; Promotion mechanism; Methane hydrate; Nucleation sites; Energy storage; [CHIM]Chemical Sciences; [CHIM.GENI]Chemical Sciences/Chemical engineering; [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry; [SPI]Engineering Sciences [physics]; [SDE]Environmental Sciences
• Online Access: https://hal.science/hal-03725298; https://hal.science/hal-03725298/document; https://hal.science/hal-03725298/file/manuscript.pdf; https://doi.org/10.1021/acssuschemeng.2c01742

International audience Clathrate hydrates are emerging as a novel storage medium for safe and compact methane storage. However, their industrial-scale applicability is hindered by relatively lower gas uptake and sluggish formation kinetics. In this study, we have employed zeolites with acidic (H−Y, FAU-type) and basic (Na−X, FAU-type) surface properties as kinetic hydrate promoters (KHPs). The impact of physical parameters as pressure and the gas-to-liquid ratio has also been studied. In a combined experimental and computational study, we assessed the performance of the two types of zeolites in different concentrations and pressures for binary CH 4 −THF clathrate hydrate synthesis in a nonstirred configuration. The kinetic study results showed that the acidic zeolite (H−Y) exhibited superior performance over the basic one (Na−X), reaching its optimum at 0.5 wt % zeolite, which agreed well with the DFT calculations. The methane conversion reached 94.25% at this concentration and a relatively mild pressure (6 MP). The induction time and t 90 (time to reach 90% of final gas uptake) were reduced by 35% and 31%, respectively. Our results open the door for a better understanding of the role of acidic zeolites as possible environmental benign KHPs that can help the utilization of water as a medium for green energy storage and transportation.