High-pressure synthesis and thermodynamic stability of PdH1±ε up to 8 GPa
Abstract
Palladium hydride alloys are superconductors and hydrogen storage materials. One synthesis route is compression of Pd to high pressure in a hydrogen-rich environment. Here we report the evolution of the unit cell volume of PdHx synthesized by compressing Pd in a pure H2 medium to pressures from 0.2 to 8 GPa in a diamond anvil cell at room temperature. The volume of the face-centered cubic unit cell changes nonmonotonically with pressure, increasing upon compression from 0.2 to 1 GPa and decreasing upon compression from 1 to 8 GPa. Volume is reversible upon decompression and is independent of whether the sample was heated to 600 K at low pressure (P<2 GPa). The x-ray diffraction data show no evidence for a phase transition between 0.2 and 8 GPa. The volume maximum at 1 GPa must be caused by progressive hydrogenation from 0 to 1 GPa. Assuming a pressure-volume-composition equation of state derived from previously published data, the [H]:[Pd] ratio in this study increases to a maximum value of x=1±0.02 at 2±0.5 GPa and remains stable upon further compression to and from 8 GPa. These results add to a mounting body of evidence that Pd H1±ε is in thermodynamic equilibrium with pure H2more »
- Authors:
-
[1];
[4];
- Carnegie Inst. of Washington, Washington, DC (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- International Inst. for Hydrogen Materials Research (i2-HMR), Bourgoin Jallieu (France)
- Bhabha Atomic Research Center (India)
- Univ. of Illinois, Chicago, IL (United States)
- Publication Date:
- Research Org.:
- Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1766801
- Alternate Identifier(s):
- OSTI ID: 1768059
- Grant/Contract Number:
- NA0003975; AC02-06CH11357; SC0001057; NA0003858; NA0001974
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 103; Journal Issue: 2; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Composition; Crystal structure; Pressure effects; Superconductivity; Superconductors
Citation Formats
Geballe, Zachary M., Somayazulu, Maddury, Armanet, Nicolas, Mishra, Ajay K., Ahart, Muhtar, and Hemley, Russell J. High-pressure synthesis and thermodynamic stability of PdH1±ε up to 8 GPa. United States: N. p., 2021.
Web. doi:10.1103/physrevb.103.024515.
Geballe, Zachary M., Somayazulu, Maddury, Armanet, Nicolas, Mishra, Ajay K., Ahart, Muhtar, & Hemley, Russell J. High-pressure synthesis and thermodynamic stability of PdH1±ε up to 8 GPa. United States. https://doi.org/10.1103/physrevb.103.024515
Geballe, Zachary M., Somayazulu, Maddury, Armanet, Nicolas, Mishra, Ajay K., Ahart, Muhtar, and Hemley, Russell J. Tue .
"High-pressure synthesis and thermodynamic stability of PdH1±ε up to 8 GPa". United States. https://doi.org/10.1103/physrevb.103.024515. https://www.osti.gov/servlets/purl/1766801.
@article{osti_1766801,
title = {High-pressure synthesis and thermodynamic stability of PdH1±ε up to 8 GPa},
author = {Geballe, Zachary M. and Somayazulu, Maddury and Armanet, Nicolas and Mishra, Ajay K. and Ahart, Muhtar and Hemley, Russell J.},
abstractNote = {Palladium hydride alloys are superconductors and hydrogen storage materials. One synthesis route is compression of Pd to high pressure in a hydrogen-rich environment. Here we report the evolution of the unit cell volume of PdHx synthesized by compressing Pd in a pure H2 medium to pressures from 0.2 to 8 GPa in a diamond anvil cell at room temperature. The volume of the face-centered cubic unit cell changes nonmonotonically with pressure, increasing upon compression from 0.2 to 1 GPa and decreasing upon compression from 1 to 8 GPa. Volume is reversible upon decompression and is independent of whether the sample was heated to 600 K at low pressure (P<2 GPa). The x-ray diffraction data show no evidence for a phase transition between 0.2 and 8 GPa. The volume maximum at 1 GPa must be caused by progressive hydrogenation from 0 to 1 GPa. Assuming a pressure-volume-composition equation of state derived from previously published data, the [H]:[Pd] ratio in this study increases to a maximum value of x=1±0.02 at 2±0.5 GPa and remains stable upon further compression to and from 8 GPa. These results add to a mounting body of evidence that Pd H1±ε is in thermodynamic equilibrium with pure H2 at room temperature from 2 GPa to at least 8 GPa. The simplest interpretation is that H atoms occupy all octahedral sites and no tetrahedral sites in face-centered cubic PdH 1.0.},
doi = {10.1103/physrevb.103.024515},
journal = {Physical Review B},
number = 2,
volume = 103,
place = {United States},
year = {Tue Jan 19 00:00:00 EST 2021},
month = {Tue Jan 19 00:00:00 EST 2021}
}
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