All-Inorganic Open-Framework Chalcogenides, A3Ga5S9·xH2O (A = Rb and Cs), Exhibiting Ultrafast Uranyl Remediation and Illustrating a Novel Post-Synthetic Preparation of Open-Framework Oxychalcogenides
Abstract
Fast and effective uranyl sequestration is of interest to the nuclear industry. Recently layered chalcogenide materials have demonstrated fast, selective, and efficient sorption properties towards uranyl cations and the development and investigation of new types of chalcogenide materials continues to be of interest and represents an intriguing option for uranyl remediation. Three new all-inorganic A3Ga5S9·xH2O (A = Rb, Rb/Cs, and Cs) open-framework chalcogenides were obtained via an in-situ alkali carbonate to alkali sulfide conversion process achieved under mild hydrothermal conditions. The structures of the all-inorganic open framework chalcogenides consist of a 2-fold interpenetrated diamond-like 3D framework containing pseudo-T3 [Ga10S20]10– supertetrahedra. 48% of the structural volume is occupied by A+ cations and water species, as established by single-crystal X-ray diffraction (SCXRD), infrared (IR) and energy-dispersive (EDS) spectroscopies. The dynamic nature of the A+ cations and water molecules within the pores was investigated via single crystal X-ray diffraction as well as by IR spectroscopy monitored H2O to D2O exchange experiments. Framework stability was probed with post-synthetic treatment of A3Ga5S9·xH2O (A = Rb and Cs) samples in acidic solutions that resulted in the formation of the oxysulfide (A/H)3Ga5S9–yOy·xH2O (A = Rb and Cs; y = 0–1), as shown by SCXRD and IR. Ion-exchangemore »
- Publication Date:
- Research Org.:
- Univ. of South Carolina, Columbia, SC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1905732
- Grant/Contract Number:
- SC0018739
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 18; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cations; Chalcogenides; Chemical structure; Crystal structure; Uranium
Citation Formats
Berseneva, Anna A., Aziziha, Mina, Schorne-Pinto, Juliano, Besmann, Theodore M., and zur Loye, Hans-Conrad. All-Inorganic Open-Framework Chalcogenides, A3Ga5S9·xH2O (A = Rb and Cs), Exhibiting Ultrafast Uranyl Remediation and Illustrating a Novel Post-Synthetic Preparation of Open-Framework Oxychalcogenides. United States: N. p., 2022.
Web. doi:10.1021/acs.chemmater.2c02059.
Berseneva, Anna A., Aziziha, Mina, Schorne-Pinto, Juliano, Besmann, Theodore M., & zur Loye, Hans-Conrad. All-Inorganic Open-Framework Chalcogenides, A3Ga5S9·xH2O (A = Rb and Cs), Exhibiting Ultrafast Uranyl Remediation and Illustrating a Novel Post-Synthetic Preparation of Open-Framework Oxychalcogenides. United States. https://doi.org/10.1021/acs.chemmater.2c02059
Berseneva, Anna A., Aziziha, Mina, Schorne-Pinto, Juliano, Besmann, Theodore M., and zur Loye, Hans-Conrad. Thu .
"All-Inorganic Open-Framework Chalcogenides, A3Ga5S9·xH2O (A = Rb and Cs), Exhibiting Ultrafast Uranyl Remediation and Illustrating a Novel Post-Synthetic Preparation of Open-Framework Oxychalcogenides". United States. https://doi.org/10.1021/acs.chemmater.2c02059. https://www.osti.gov/servlets/purl/1905732.
@article{osti_1905732,
title = {All-Inorganic Open-Framework Chalcogenides, A3Ga5S9·xH2O (A = Rb and Cs), Exhibiting Ultrafast Uranyl Remediation and Illustrating a Novel Post-Synthetic Preparation of Open-Framework Oxychalcogenides},
author = {Berseneva, Anna A. and Aziziha, Mina and Schorne-Pinto, Juliano and Besmann, Theodore M. and zur Loye, Hans-Conrad},
abstractNote = {Fast and effective uranyl sequestration is of interest to the nuclear industry. Recently layered chalcogenide materials have demonstrated fast, selective, and efficient sorption properties towards uranyl cations and the development and investigation of new types of chalcogenide materials continues to be of interest and represents an intriguing option for uranyl remediation. Three new all-inorganic A3Ga5S9·xH2O (A = Rb, Rb/Cs, and Cs) open-framework chalcogenides were obtained via an in-situ alkali carbonate to alkali sulfide conversion process achieved under mild hydrothermal conditions. The structures of the all-inorganic open framework chalcogenides consist of a 2-fold interpenetrated diamond-like 3D framework containing pseudo-T3 [Ga10S20]10– supertetrahedra. 48% of the structural volume is occupied by A+ cations and water species, as established by single-crystal X-ray diffraction (SCXRD), infrared (IR) and energy-dispersive (EDS) spectroscopies. The dynamic nature of the A+ cations and water molecules within the pores was investigated via single crystal X-ray diffraction as well as by IR spectroscopy monitored H2O to D2O exchange experiments. Framework stability was probed with post-synthetic treatment of A3Ga5S9·xH2O (A = Rb and Cs) samples in acidic solutions that resulted in the formation of the oxysulfide (A/H)3Ga5S9–yOy·xH2O (A = Rb and Cs; y = 0–1), as shown by SCXRD and IR. Ion-exchange studies on A3Ga5S9·xH2O (A = Rb and Cs) samples were carried out utilizing a uranyl acetate solution. The presence of the UO22+ species in the ion-exchanged product was supported by IR and EDS spectroscopies. Batch method ion-exchange experiments on Cs3Ga5S9·xH2O powder demonstrated fast kinetics with 95% uranyl removal from the uranyl acetate solution during the first minute, a maximum uranyl uptake capacity of 15mg/g, and the subsequent elution of uranyl species with KCl solution. Furthermore, the porous and dynamic nature of the A3Ga5S9·xH2O framework coupled with effective UO22+···S2– bonding interactions makes it a good potential sorbent for uranyl remediation from aqueous media.},
doi = {10.1021/acs.chemmater.2c02059},
journal = {Chemistry of Materials},
number = 18,
volume = 34,
place = {United States},
year = {Thu Sep 08 00:00:00 EDT 2022},
month = {Thu Sep 08 00:00:00 EDT 2022}
}
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