Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study
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,...
Published in: | ACS Sustainable Chemistry & Engineering |
---|---|
Main Authors: | , , |
Other Authors: | , , , , , , , |
Format: | Article in Journal/Newspaper |
Language: | English |
Published: |
HAL CCSD
2022
|
Subjects: | |
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 |
id |
ftccsdartic:oai:HAL:hal-03725298v1 |
---|---|
record_format |
openpolar |
spelling |
ftccsdartic:oai:HAL:hal-03725298v1 2023-12-10T09:50:40+01:00 Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study Omran, Ahmed Nesterenko, Nikolay Valtchev, Valentin 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) 2022-06-20 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 en eng HAL CCSD American Chemical Society info:eu-repo/semantics/altIdentifier/doi/10.1021/acssuschemeng.2c01742 hal-03725298 https://hal.science/hal-03725298 https://hal.science/hal-03725298/document https://hal.science/hal-03725298/file/manuscript.pdf doi:10.1021/acssuschemeng.2c01742 info:eu-repo/semantics/OpenAccess EISSN: 2168-0485 ACS Sustainable Chemistry & Engineering https://hal.science/hal-03725298 ACS Sustainable Chemistry & Engineering, 2022, 10 (24), pp.8002-8010. ⟨10.1021/acssuschemeng.2c01742⟩ 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 info:eu-repo/semantics/article Journal articles 2022 ftccsdartic https://doi.org/10.1021/acssuschemeng.2c01742 2023-11-12T00:10:09Z 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. Article in Journal/Newspaper Methane hydrate Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) ACS Sustainable Chemistry & Engineering 10 24 8002 8010 |
institution |
Open Polar |
collection |
Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
op_collection_id |
ftccsdartic |
language |
English |
topic |
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 |
spellingShingle |
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 Omran, Ahmed Nesterenko, Nikolay Valtchev, Valentin Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
topic_facet |
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 |
description |
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. |
author2 |
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 |
author |
Omran, Ahmed Nesterenko, Nikolay Valtchev, Valentin |
author_facet |
Omran, Ahmed Nesterenko, Nikolay Valtchev, Valentin |
author_sort |
Omran, Ahmed |
title |
Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
title_short |
Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
title_full |
Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
title_fullStr |
Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
title_full_unstemmed |
Revealing Zeolites Active Sites Role as Kinetic Hydrate Promoters: Combined Computational and Experimental Study |
title_sort |
revealing zeolites active sites role as kinetic hydrate promoters: combined computational and experimental study |
publisher |
HAL CCSD |
publishDate |
2022 |
url |
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 |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
EISSN: 2168-0485 ACS Sustainable Chemistry & Engineering https://hal.science/hal-03725298 ACS Sustainable Chemistry & Engineering, 2022, 10 (24), pp.8002-8010. ⟨10.1021/acssuschemeng.2c01742⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1021/acssuschemeng.2c01742 hal-03725298 https://hal.science/hal-03725298 https://hal.science/hal-03725298/document https://hal.science/hal-03725298/file/manuscript.pdf doi:10.1021/acssuschemeng.2c01742 |
op_rights |
info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.1021/acssuschemeng.2c01742 |
container_title |
ACS Sustainable Chemistry & Engineering |
container_volume |
10 |
container_issue |
24 |
container_start_page |
8002 |
op_container_end_page |
8010 |
_version_ |
1784895887017771008 |