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Title: Ionization-Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds

The nanoscale confinement of noble gases at noncryogenic temperatures is crucial for many applications including noble gas separations, nuclear waste remediation, and the removal of radon. However, this process is extremely difficult primarily due to the weak trapping forces of the host matrices upon noble gas physisorption. The formation of 2D clathrate compounds, which result from trapping noble gas atoms (Ar, Kr, and Xe) inside nanocages of ultrathin silica and aluminosilicate crystalline nanoporous frameworks at 300 K, is reported. The formation of the 2D clathrate compounds is attributed to a novel activated physisorption mechanism, facilitated by ionization of noble gas atoms. Combined X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) studies provide evidence of an initial ionization process that significantly reduces the apparent trapping barrier. Noble gas ions become neutralized upon entering the cages, and their desorption requires unprecedentedly high temperatures, even in ultrahigh vacuum conditions. From 2D aluminosilicate films these temperatures are 348 K (Ar), 498 K (Kr), and 673 K (Xe). DFT calculations also predict that Rn can be trapped in 2D aluminosilicates with an even higher desorption temperature of 775 K. This work highlights a new ionization-facilitated trapping mechanism resulting in the thinnest family of clathratesmore » ever reported.« less
Authors:
 [1] ;  [2] ;  [2] ;  [1] ; ORCiD logo [1] ;  [3] ;  [4] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Stony Brook Univ., NY (United States). Materials Science and Chemical Engineering Dept.
  3. National Univ. of San Luis (Argentina). CONICET. Inst. of Applied Physics (INFAP); Univ. of Wisconsin, Milwaukee, WI (United States). Dept. of Chemistry
  4. Stony Brook Univ., NY (United States). Materials Science and Chemical Engineering Dept.
Publication Date:
Report Number(s):
BNL-211478-2019-JAAM
Journal ID: ISSN 1616-301X
Grant/Contract Number:
SC0012704; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Name: Advanced Functional Materials; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); BNL Laboratory Directed Research and Development (LDRD) Program
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 2D zeolites; activated physisorption; gas separation; noble gas clathrate; single atom trapping
OSTI Identifier:
1504404
Alternate Identifier(s):
OSTI ID: 1498167

Zhong, Jian-Qiang, Wang, Mengen, Akter, Nusnin, Kestell, John D., Niu, Tianchao, Boscoboinik, Alejandro M., Kim, Taejin, Stacchiola, Dario J., Wu, Qin, Lu, Deyu, and Boscoboinik, Jorge Anibal. Ionization-Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds. United States: N. p., Web. doi:10.1002/adfm.201806583.
Zhong, Jian-Qiang, Wang, Mengen, Akter, Nusnin, Kestell, John D., Niu, Tianchao, Boscoboinik, Alejandro M., Kim, Taejin, Stacchiola, Dario J., Wu, Qin, Lu, Deyu, & Boscoboinik, Jorge Anibal. Ionization-Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds. United States. doi:10.1002/adfm.201806583.
Zhong, Jian-Qiang, Wang, Mengen, Akter, Nusnin, Kestell, John D., Niu, Tianchao, Boscoboinik, Alejandro M., Kim, Taejin, Stacchiola, Dario J., Wu, Qin, Lu, Deyu, and Boscoboinik, Jorge Anibal. 2019. "Ionization-Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds". United States. doi:10.1002/adfm.201806583.
@article{osti_1504404,
title = {Ionization-Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds},
author = {Zhong, Jian-Qiang and Wang, Mengen and Akter, Nusnin and Kestell, John D. and Niu, Tianchao and Boscoboinik, Alejandro M. and Kim, Taejin and Stacchiola, Dario J. and Wu, Qin and Lu, Deyu and Boscoboinik, Jorge Anibal},
abstractNote = {The nanoscale confinement of noble gases at noncryogenic temperatures is crucial for many applications including noble gas separations, nuclear waste remediation, and the removal of radon. However, this process is extremely difficult primarily due to the weak trapping forces of the host matrices upon noble gas physisorption. The formation of 2D clathrate compounds, which result from trapping noble gas atoms (Ar, Kr, and Xe) inside nanocages of ultrathin silica and aluminosilicate crystalline nanoporous frameworks at 300 K, is reported. The formation of the 2D clathrate compounds is attributed to a novel activated physisorption mechanism, facilitated by ionization of noble gas atoms. Combined X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) studies provide evidence of an initial ionization process that significantly reduces the apparent trapping barrier. Noble gas ions become neutralized upon entering the cages, and their desorption requires unprecedentedly high temperatures, even in ultrahigh vacuum conditions. From 2D aluminosilicate films these temperatures are 348 K (Ar), 498 K (Kr), and 673 K (Xe). DFT calculations also predict that Rn can be trapped in 2D aluminosilicates with an even higher desorption temperature of 775 K. This work highlights a new ionization-facilitated trapping mechanism resulting in the thinnest family of clathrates ever reported.},
doi = {10.1002/adfm.201806583},
journal = {Advanced Functional Materials},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {3}
}

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