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Capturing Hydrate Formation Processes in Tetrahydrofuran/Water Mixtures with Temperature Resolved In Situ Synchrotron X‑ray Diffraction and Infrared Spectroscopy

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Title: Capturing Hydrate Formation Processes in Tetrahydrofuran/Water Mixtures with Temperature Resolved In Situ Synchrotron X‑ray Diffraction and Infrared Spectroscopy
Authors: Robert P. C. Bauer, Danny Rodriguez, Santanu Pathak, John S. Tse
Publication Year: 2025
Subject Terms: Biophysics, Ecology, Cancer, Inorganic Chemistry, Environmental Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, work provides atomic, situ synchrotron x, disordered diffraction pattern, different temperature regimes, deposited sample showed, infrared spectroscopy understanding, crystalline thf persisted, clathrate hydrate formation, infrared spectroscopy, thf segregated, temperature resolved, ray diffraction, new crystalline, deposited cryogenically, clathrate hydrate, upon heating, ultrahigh vacuum, system ’, range orders, onset crystallization, observed prior, molecular rearrangements, low temperatures
Description: Understanding the mechanisms behind clathrate hydrate formation is of both practical and fundamental interest. Here, we report the formation of a clathrate hydrate from a tetrahydrofuran (THF)–water mixture of “ideal” stoichiometry, deposited cryogenically in ultrahigh vacuum and studied with in situ synchrotron X-ray diffraction and infrared spectroscopy on slightly deuterated water samples. The experiments provide complementary information on the evolution of the system’s local and long-range orders. They revealed distinctive structural transformations in different temperature regimes. The as-deposited sample showed a disordered diffraction pattern. Upon heating, THF segregated and crystallized, while solid water remained amorphous. Crystalline THF persisted until 110 K, then it melted and interacted with water to form type II clathrate without ice contamination. No new crystalline or amorphous phases were observed prior to the onset crystallization of the hydrate. This work provides atomic-level insight into molecular rearrangements during clathrate hydrate formation, highlighting molecular mobility even at low temperatures.
Document Type: article in journal/newspaper
Language: unknown
Relation: https://figshare.com/articles/journal_contribution/Capturing_Hydrate_Formation_Processes_in_Tetrahydrofuran_Water_Mixtures_with_Temperature_Resolved_In_Situ_Synchrotron_X_ray_Diffraction_and_Infrared_Spectroscopy/29072528
DOI: 10.1021/acs.jpclett.5c00576.s001
Availability: https://doi.org/10.1021/acs.jpclett.5c00576.s001
https://figshare.com/articles/journal_contribution/Capturing_Hydrate_Formation_Processes_in_Tetrahydrofuran_Water_Mixtures_with_Temperature_Resolved_In_Situ_Synchrotron_X_ray_Diffraction_and_Infrared_Spectroscopy/29072528
Rights: CC BY-NC 4.0
Accession Number: edsbas.744B2A5C
Database: BASE
Description
Abstract:Understanding the mechanisms behind clathrate hydrate formation is of both practical and fundamental interest. Here, we report the formation of a clathrate hydrate from a tetrahydrofuran (THF)–water mixture of “ideal” stoichiometry, deposited cryogenically in ultrahigh vacuum and studied with in situ synchrotron X-ray diffraction and infrared spectroscopy on slightly deuterated water samples. The experiments provide complementary information on the evolution of the system’s local and long-range orders. They revealed distinctive structural transformations in different temperature regimes. The as-deposited sample showed a disordered diffraction pattern. Upon heating, THF segregated and crystallized, while solid water remained amorphous. Crystalline THF persisted until 110 K, then it melted and interacted with water to form type II clathrate without ice contamination. No new crystalline or amorphous phases were observed prior to the onset crystallization of the hydrate. This work provides atomic-level insight into molecular rearrangements during clathrate hydrate formation, highlighting molecular mobility even at low temperatures.
DOI:10.1021/acs.jpclett.5c00576.s001