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Title: High-pressure phase transition of alkali metal–transition metal deuteride Li2PdD2

Abstract

A combined theoretical and experimental study of lithium palladium deuteride (Li2PdD2) subjected to pressures up to 50 GPa reveals one structural phase transition near 10 GPa, detected by synchrotron powder x-ray diffraction, and metadynamics simulations. We report the ambient-pressure tetragonal phase of Li2PdD2 transforms into a monoclinic $C2/m$ phase that is distinct from all known structures of alkali metal–transition metal hydrides/deuterides. The structure of the high-pressure phase was characterized using ab initio computational techniques and from refinement of the powder x-ray diffraction data. In the high-pressure phase, the PdD2 complexes lose molecular integrity and are fused to extended [PdD2] chains. The discovered phase transition and new structure are relevant to the possible hydrogen storage application of Li2PdD2 and alkali metal–transition metal hydrides in general.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [7]
  1. Univ. of Saskatchewan, Saskatoon, SK (Canada); Canadian Light Source, Inc., Saskatoon, SK (Canada)
  2. Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.; Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.; Chinese Academy of Sciences (CAS), Heifei (China)
  4. Univ. of Saskatchewan, Saskatoon, SK (Canada)
  5. Jilin Univ., Changchun (China)
  6. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  7. Naval Research Lab. (NRL), Washington, DC (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
Natural Sciences and Engineering Research Council of Canada (NSERC); Defense Advanced Research Projects Agency (DARPA); Chinese Academy of Sciences (CAS); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; US Department of the Navy, Office of Naval Research (ONR)
OSTI Identifier:
1368302
Alternate Identifier(s):
OSTI ID: 1364186
Grant/Contract Number:  
AC52-07NA27344; FG02-94ER14466; AC02-06CH1357; W31P4Q1310005; W31P4Q1210008; 2011T2J20; EAR-0622171; DMR-1231586; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 23; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yao, Yansun, Stavrou, Elissaios, Goncharov, Alexander F., Majumdar, Arnab, Wang, Hui, Prakapenka, Vitali B., Epshteyn, Albert, and Purdy, Andrew P. High-pressure phase transition of alkali metal–transition metal deuteride Li2PdD2. United States: N. p., 2017. Web. doi:10.1063/1.4986245.
Yao, Yansun, Stavrou, Elissaios, Goncharov, Alexander F., Majumdar, Arnab, Wang, Hui, Prakapenka, Vitali B., Epshteyn, Albert, & Purdy, Andrew P. High-pressure phase transition of alkali metal–transition metal deuteride Li2PdD2. United States. doi:10.1063/1.4986245.
Yao, Yansun, Stavrou, Elissaios, Goncharov, Alexander F., Majumdar, Arnab, Wang, Hui, Prakapenka, Vitali B., Epshteyn, Albert, and Purdy, Andrew P. Mon . "High-pressure phase transition of alkali metal–transition metal deuteride Li2PdD2". United States. doi:10.1063/1.4986245. https://www.osti.gov/servlets/purl/1368302.
@article{osti_1368302,
title = {High-pressure phase transition of alkali metal–transition metal deuteride Li2PdD2},
author = {Yao, Yansun and Stavrou, Elissaios and Goncharov, Alexander F. and Majumdar, Arnab and Wang, Hui and Prakapenka, Vitali B. and Epshteyn, Albert and Purdy, Andrew P.},
abstractNote = {A combined theoretical and experimental study of lithium palladium deuteride (Li2PdD2) subjected to pressures up to 50 GPa reveals one structural phase transition near 10 GPa, detected by synchrotron powder x-ray diffraction, and metadynamics simulations. We report the ambient-pressure tetragonal phase of Li2PdD2 transforms into a monoclinic $C2/m$ phase that is distinct from all known structures of alkali metal–transition metal hydrides/deuterides. The structure of the high-pressure phase was characterized using ab initio computational techniques and from refinement of the powder x-ray diffraction data. In the high-pressure phase, the PdD2 complexes lose molecular integrity and are fused to extended [PdD2]∞ chains. The discovered phase transition and new structure are relevant to the possible hydrogen storage application of Li2PdD2 and alkali metal–transition metal hydrides in general.},
doi = {10.1063/1.4986245},
journal = {Journal of Chemical Physics},
number = 23,
volume = 146,
place = {United States},
year = {2017},
month = {6}
}

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