Induced Migration of CO2 from Hydrate Cages to Amorphous Solid Water under Ultrahigh Vacuum and Cryogenic Conditions
Restricted migration of reactive species limits chemical transformations within interstellar and cometary ices. We report the migration of CO2 from clathrate hydrate (CH) cages to amorphous solid water (ASW) in the presence of tetrahydrofuran (THF) under ultrahigh vacuum (UHV) and cryogenic conditio...
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Published in | The journal of physical chemistry letters Vol. 14; no. 11; pp. 2823 - 2829 |
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Main Authors | , , , , , , , , |
Format | Journal Article |
Language | English |
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American Chemical Society
23.03.2023
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Abstract | Restricted migration of reactive species limits chemical transformations within interstellar and cometary ices. We report the migration of CO2 from clathrate hydrate (CH) cages to amorphous solid water (ASW) in the presence of tetrahydrofuran (THF) under ultrahigh vacuum (UHV) and cryogenic conditions. Thermal annealing of sequentially deposited CO2 and H2O ice, CO2@H2O, to 90 K resulted in the partitioning of CO2 in 512 and 51262 CH cages (CO2@512, CO2@51262). However, upon preparing a composite ice film composed of CO2@512, CO2@51262 and THF distributed in the water matrix at 90 K, and annealing the mixture for 6 h at 130 K produced mixed CO2–THF CH, where THF occupied the 51264 cages (THF@51264) exclusively while CO2 in 51262 cages (CO2@51262) got transferred to the ASW matrix and CO2 in the 512 cages (CO2@512) remained as is. This cage–matrix exchange may create a more conducive environment for chemical transformations in interstellar environments. |
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AbstractList | Restricted migration of reactive species limits chemical transformations within interstellar and cometary ices. We report the migration of CO2 from clathrate hydrate (CH) cages to amorphous solid water (ASW) in the presence of tetrahydrofuran (THF) under ultrahigh vacuum (UHV) and cryogenic conditions. Thermal annealing of sequentially deposited CO2 and H2O ice, CO2@H2O, to 90 K resulted in the partitioning of CO2 in 512 and 51262 CH cages (CO2@512, CO2@51262). However, upon preparing a composite ice film composed of CO2@512, CO2@51262 and THF distributed in the water matrix at 90 K, and annealing the mixture for 6 h at 130 K produced mixed CO2–THF CH, where THF occupied the 51264 cages (THF@51264) exclusively while CO2 in 51262 cages (CO2@51262) got transferred to the ASW matrix and CO2 in the 512 cages (CO2@512) remained as is. This cage–matrix exchange may create a more conducive environment for chemical transformations in interstellar environments. |
Author | Kumar, Rajnish Malla, Bijesh K. Chowdhury, Soham Vishwakarma, Gaurav Reddy, Sandeep K. Reddy, K. S. S. V. Prasad Yamijala, Sharma S. R. K. C. Pradeep, Thalappil Ghosh, Jyotirmoy |
AuthorAffiliation | Department of Chemistry International Centre for Clean Water Centre for Computational and Data Science Department of Chemical Engineering Centre for Atomistic Modelling and Materials Design, Centre for Quantum Information, Communication, and Computing, and Centre for Molecular Materials and Functions IIT Madras Research Park DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry |
AuthorAffiliation_xml | – name: International Centre for Clean Water – name: Department of Chemical Engineering – name: IIT Madras Research Park – name: Department of Chemistry – name: Centre for Atomistic Modelling and Materials Design, Centre for Quantum Information, Communication, and Computing, and Centre for Molecular Materials and Functions – name: DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry – name: Centre for Computational and Data Science |
Author_xml | – sequence: 1 givenname: Gaurav surname: Vishwakarma fullname: Vishwakarma, Gaurav organization: DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry – sequence: 2 givenname: Bijesh K. surname: Malla fullname: Malla, Bijesh K. organization: DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry – sequence: 3 givenname: K. S. S. V. Prasad surname: Reddy fullname: Reddy, K. S. S. V. Prasad organization: Department of Chemistry – sequence: 4 givenname: Jyotirmoy surname: Ghosh fullname: Ghosh, Jyotirmoy organization: Department of Chemistry – sequence: 5 givenname: Soham surname: Chowdhury fullname: Chowdhury, Soham organization: DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence (TUE), Department of Chemistry – sequence: 6 givenname: Sharma S. R. K. C. orcidid: 0000-0003-1773-9226 surname: Yamijala fullname: Yamijala, Sharma S. R. K. C. organization: Centre for Atomistic Modelling and Materials Design, Centre for Quantum Information, Communication, and Computing, and Centre for Molecular Materials and Functions – sequence: 7 givenname: Sandeep K. orcidid: 0000-0002-1458-6853 surname: Reddy fullname: Reddy, Sandeep K. email: skreddy@iitkgp.ac.in organization: Centre for Computational and Data Science – sequence: 8 givenname: Rajnish orcidid: 0000-0002-4172-2638 surname: Kumar fullname: Kumar, Rajnish email: rajnish@iitm.ac.in organization: IIT Madras Research Park – sequence: 9 givenname: Thalappil orcidid: 0000-0003-3174-534X surname: Pradeep fullname: Pradeep, Thalappil email: pradeep@iitm.ac.in organization: IIT Madras Research Park |
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Title | Induced Migration of CO2 from Hydrate Cages to Amorphous Solid Water under Ultrahigh Vacuum and Cryogenic Conditions |
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