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Title: Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations

Abstract

In this work, a combined analytical method of NEXAFS measurement and DFT-calculation was employed for the evaluation of Cs states in clay minerals. The measured Cs M 4,5 NEXAFS spectra of Cs halides were analyzed using the DFT-calculations in order to establish the analytical methods. The NEXAFS spectra of the Cs halides were well reproduced by incorporating the core-hole strength. The Cs M 4,5 NEXAFS spectrum of the clay minerals was well reproduced by the DFT-calculations including the major transitions and tail structures with the established method. Further evaluation of this spectrum by charge density analysis suggested that these major transitions and the tail structures likely reflect the bonding state and the local environment around the Cs atoms. Comparison of electronic states of Cs in the clay mineral with those in the Cs halides by DFT-calculations has shown that the interaction between Cs and the nearest-neighbor atom is largest in the clay mineral, which differs from those of Cs halides. This happened due to the energy level of Cs-5s and 5p, which was closer to that of O-2s and 2p than the s and p orbitals of other alkali metal and alkali earth metal elements.

Authors:
 [1];  [2];  [1];  [3];  [4]; ORCiD logo [3];  [3];  [3]; ORCiD logo [1];  [1]
  1. Japan Atomic Energy Agency (JAEA), Tokai-mura, Naka-gun, Ibaraki-ken (Japan)
  2. Japan Atomic Energy Agency (JAEA), Sayo, Hyogo (Japan)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1508065
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics and Chemistry of Solids
Additional Journal Information:
Journal Volume: 127; Journal Issue: C; Journal ID: ISSN 0022-3697
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cesium; NEXAFS; Clay mineral; DFT calculation; Electronic state

Citation Formats

Suzuki, Chikashi, Yaita, Tsuyoshi, Suzuki, Shinichi, Pacold, Joseph, Altman, Alison B., Minasian, Stefan G., Tyliszczak, Tolek, Shuh, David K., Yoshida, Hiroyuki, and Osaka, Masahiko. Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations. United States: N. p., 2018. Web. doi:10.1016/j.jpcs.2018.11.011.
Suzuki, Chikashi, Yaita, Tsuyoshi, Suzuki, Shinichi, Pacold, Joseph, Altman, Alison B., Minasian, Stefan G., Tyliszczak, Tolek, Shuh, David K., Yoshida, Hiroyuki, & Osaka, Masahiko. Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations. United States. doi:10.1016/j.jpcs.2018.11.011.
Suzuki, Chikashi, Yaita, Tsuyoshi, Suzuki, Shinichi, Pacold, Joseph, Altman, Alison B., Minasian, Stefan G., Tyliszczak, Tolek, Shuh, David K., Yoshida, Hiroyuki, and Osaka, Masahiko. Wed . "Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations". United States. doi:10.1016/j.jpcs.2018.11.011. https://www.osti.gov/servlets/purl/1508065.
@article{osti_1508065,
title = {Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations},
author = {Suzuki, Chikashi and Yaita, Tsuyoshi and Suzuki, Shinichi and Pacold, Joseph and Altman, Alison B. and Minasian, Stefan G. and Tyliszczak, Tolek and Shuh, David K. and Yoshida, Hiroyuki and Osaka, Masahiko},
abstractNote = {In this work, a combined analytical method of NEXAFS measurement and DFT-calculation was employed for the evaluation of Cs states in clay minerals. The measured Cs M4,5 NEXAFS spectra of Cs halides were analyzed using the DFT-calculations in order to establish the analytical methods. The NEXAFS spectra of the Cs halides were well reproduced by incorporating the core-hole strength. The Cs M4,5 NEXAFS spectrum of the clay minerals was well reproduced by the DFT-calculations including the major transitions and tail structures with the established method. Further evaluation of this spectrum by charge density analysis suggested that these major transitions and the tail structures likely reflect the bonding state and the local environment around the Cs atoms. Comparison of electronic states of Cs in the clay mineral with those in the Cs halides by DFT-calculations has shown that the interaction between Cs and the nearest-neighbor atom is largest in the clay mineral, which differs from those of Cs halides. This happened due to the energy level of Cs-5s and 5p, which was closer to that of O-2s and 2p than the s and p orbitals of other alkali metal and alkali earth metal elements.},
doi = {10.1016/j.jpcs.2018.11.011},
journal = {Journal of Physics and Chemistry of Solids},
number = C,
volume = 127,
place = {United States},
year = {2018},
month = {11}
}

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