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Title: Confinement of Iodine Molecules into Triple-Helical Chains within Robust Metal–Organic Frameworks

Abstract

During nuclear waste disposal process, radioactive iodine as a fission product can be released. The widespread implementation of sustainable nuclear energy thus requires the development of efficient iodine stores that have simultaneously high capacity, stability and more importantly, storage density (and hence minimized system volume). Here, we report high I2 adsorption in a series of robust porous metal–organic materials, MFM-300(M) (M = Al, Sc, Fe, In). MFM-300(Sc) exhibits fully reversible I2 uptake of 1.54 g g–1, and its structure remains completely unperturbed upon inclusion/removal of I2. Direct observation and quantification of the adsorption, binding domains and dynamics of guest I2 molecules within these hosts have been achieved using XPS, TGA-MS, high resolution synchrotron X-ray diffraction, pair distribution function analysis, Raman, terahertz and neutron spectroscopy, coupled with density functional theory modeling. These complementary techniques reveal a comprehensive understanding of the host–I2 and I2–I2 binding interactions at a molecular level. The initial binding site of I2 in MFM-300(Sc), I2I, is located near the bridging hydroxyl group of the [ScO4(OH)2] moiety [I2I···H–O = 2.263(9) Å] with an occupancy of 0.268. I2II is located interstitially between two phenyl rings of neighboring ligand molecules [I2II···phenyl ring = 3.378(9) and 4.228(5) Å]. I2II is 4.565(2) Åmore » from the hydroxyl group with an occupancy of 0.208. Significantly, at high I2 loading an unprecedented self-aggregation of I2 molecules into triple-helical chains within the confined nanovoids has been observed at crystallographic resolution, leading to a highly efficient packing of I2 molecules with an exceptional I2 storage density of 3.08 g cm–3 in MFM-300(Sc).« less

Authors:
 [1];  [2];  [1];  [2];  [3]; ORCiD logo [4];  [1];  [5];  [5];  [5];  [6];  [6];  [2]; ORCiD logo [4];  [1];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Manchester (United Kingdom). School of Chemistry
  2. Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab., ISIS Facility
  3. Univ. of Manchester (United Kingdom). School of Chemistry; Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences (Russia)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). The Chemical and Engineering Materials Division (CEMD), Neutron Sciences Directorate
  5. Harwell Science Campus, Oxford (United Kingdom). Diamond Light Source
  6. European Synchrotron Radiation Facility, Grenoble (France)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1422565
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 45; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhang, Xinran, da Silva, Ivan, Godfrey, Harry G. W., Callear, Samantha K., Sapchenko, Sergey A., Cheng, Yongqiang, Vitórica-Yrezábal, Inigo, Frogley, Mark D., Cinque, Gianfelice, Tang, Chiu C., Giacobbe, Carlotta, Dejoie, Catherine, Rudić, Svemir, Ramirez-Cuesta, Anibal J., Denecke, Melissa A., Yang, Sihai, and Schröder, Martin. Confinement of Iodine Molecules into Triple-Helical Chains within Robust Metal–Organic Frameworks. United States: N. p., 2017. Web. doi:10.1021/jacs.7b08748.
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Zhang, Xinran, da Silva, Ivan, Godfrey, Harry G. W., Callear, Samantha K., Sapchenko, Sergey A., Cheng, Yongqiang, Vitórica-Yrezábal, Inigo, Frogley, Mark D., Cinque, Gianfelice, Tang, Chiu C., Giacobbe, Carlotta, Dejoie, Catherine, Rudić, Svemir, Ramirez-Cuesta, Anibal J., Denecke, Melissa A., Yang, Sihai, & Schröder, Martin. Confinement of Iodine Molecules into Triple-Helical Chains within Robust Metal–Organic Frameworks. United States. https://doi.org/10.1021/jacs.7b08748
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Zhang, Xinran, da Silva, Ivan, Godfrey, Harry G. W., Callear, Samantha K., Sapchenko, Sergey A., Cheng, Yongqiang, Vitórica-Yrezábal, Inigo, Frogley, Mark D., Cinque, Gianfelice, Tang, Chiu C., Giacobbe, Carlotta, Dejoie, Catherine, Rudić, Svemir, Ramirez-Cuesta, Anibal J., Denecke, Melissa A., Yang, Sihai, and Schröder, Martin. Wed . "Confinement of Iodine Molecules into Triple-Helical Chains within Robust Metal–Organic Frameworks". United States. https://doi.org/10.1021/jacs.7b08748. https://www.osti.gov/servlets/purl/1422565.
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@article{osti_1422565,
title = {Confinement of Iodine Molecules into Triple-Helical Chains within Robust Metal–Organic Frameworks},
author = {Zhang, Xinran and da Silva, Ivan and Godfrey, Harry G. W. and Callear, Samantha K. and Sapchenko, Sergey A. and Cheng, Yongqiang and Vitórica-Yrezábal, Inigo and Frogley, Mark D. and Cinque, Gianfelice and Tang, Chiu C. and Giacobbe, Carlotta and Dejoie, Catherine and Rudić, Svemir and Ramirez-Cuesta, Anibal J. and Denecke, Melissa A. and Yang, Sihai and Schröder, Martin},
abstractNote = {During nuclear waste disposal process, radioactive iodine as a fission product can be released. The widespread implementation of sustainable nuclear energy thus requires the development of efficient iodine stores that have simultaneously high capacity, stability and more importantly, storage density (and hence minimized system volume). Here, we report high I2 adsorption in a series of robust porous metal–organic materials, MFM-300(M) (M = Al, Sc, Fe, In). MFM-300(Sc) exhibits fully reversible I2 uptake of 1.54 g g–1, and its structure remains completely unperturbed upon inclusion/removal of I2. Direct observation and quantification of the adsorption, binding domains and dynamics of guest I2 molecules within these hosts have been achieved using XPS, TGA-MS, high resolution synchrotron X-ray diffraction, pair distribution function analysis, Raman, terahertz and neutron spectroscopy, coupled with density functional theory modeling. These complementary techniques reveal a comprehensive understanding of the host–I2 and I2–I2 binding interactions at a molecular level. The initial binding site of I2 in MFM-300(Sc), I2I, is located near the bridging hydroxyl group of the [ScO4(OH)2] moiety [I2I···H–O = 2.263(9) Å] with an occupancy of 0.268. I2II is located interstitially between two phenyl rings of neighboring ligand molecules [I2II···phenyl ring = 3.378(9) and 4.228(5) Å]. I2II is 4.565(2) Å from the hydroxyl group with an occupancy of 0.208. Significantly, at high I2 loading an unprecedented self-aggregation of I2 molecules into triple-helical chains within the confined nanovoids has been observed at crystallographic resolution, leading to a highly efficient packing of I2 molecules with an exceptional I2 storage density of 3.08 g cm–3 in MFM-300(Sc).},
doi = {10.1021/jacs.7b08748},
journal = {Journal of the American Chemical Society},
number = 45,
volume = 139,
place = {United States},
year = {Wed Oct 11 00:00:00 EDT 2017},
month = {Wed Oct 11 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/jacs.7b08748
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Figures / Tables:

Figure 1 Figure 1: (a) TGA-MS data for bare and I2-loaded MFM-300(Sc); (b) TGA plots and I2 adsorption capacities of MFM-300(M) (M = Al, In, Fe). (c) Amount of I2 adsorption in MFM-300(Sc) as a function of time.
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