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Proceedings of the National Academy of Sciences of the United States of America, volume 118, issue 46

Combining pressure and electrochemistry to synthesize superhydrides

Guan Pin Wen 1
Hemley R. J. 2, 3
2
 
Department of Physics, University of Illinois Chicago, Chicago, IL 60607;
3
 
Department of Chemistry, University of Illinois Chicago, Chicago, IL 60607;
Publication typeJournal Article
Publication date2021-11-09
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor11.1
ISSN00278424, 10916490
Multidisciplinary
Abstract
Significance Superhydrides are a materials system where near–room-temperature superconductivity has been achieved but only at very high (megabar) pressures. This work proposes an approach that combines pressure and electrochemistry to stabilize superhydrides at moderate pressures. Through a computational study of the palladium–hydrogen system, we construct electrochemical phase diagrams and show that electrochemically synthesizing superhydrides may be possible when combined with moderate pressures. We generalize this to other binary metal superhydrides of interest for superconductivity, including La, Y, and Mg hydrides. Recently, superhydrides have been computationally identified and subsequently synthesized with a variety of metals at very high pressures. In this work, we evaluate the possibility of synthesizing superhydrides by uniquely combining electrochemistry and applied pressure. We perform computational searches using density functional theory and particle swarm optimization calculations over a broad range of pressures and electrode potentials. Using a thermodynamic analysis, we construct pressure–potential phase diagrams and provide an alternate synthesis concept, pressure–potential (P2), to access phases having high hydrogen content. Palladium–hydrogen is a widely studied material system with the highest hydride phase being Pd3H4. Most strikingly for this system, at potentials above hydrogen evolution and ∼ 300 MPa pressure, we find the possibility to make palladium superhydrides (e.g., PdH10). We predict the generalizability of this approach for La-H, Y-H, and Mg-H with 10- to 100-fold reduction in required pressure for stabilizing phases. In addition, the P2 strategy allows stabilizing additional phases that cannot be done purely by either pressure or potential and is a general approach that is likely to work for synthesizing other hydrides at modest pressures.

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GOST Copy
Guan P. W. et al. Combining pressure and electrochemistry to synthesize superhydrides // Proceedings of the National Academy of Sciences of the United States of America. 2021. Vol. 118. No. 46.
GOST all authors (up to 50) Copy
Guan P. W., Hemley R. J., Viswanathan V. Combining pressure and electrochemistry to synthesize superhydrides // Proceedings of the National Academy of Sciences of the United States of America. 2021. Vol. 118. No. 46.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1073/pnas.2110470118
UR - https://doi.org/10.1073%2Fpnas.2110470118
TI - Combining pressure and electrochemistry to synthesize superhydrides
T2 - Proceedings of the National Academy of Sciences of the United States of America
AU - Guan, Pin Wen
AU - Hemley, R. J.
AU - Viswanathan, Venkatasubramanian
PY - 2021
DA - 2021/11/09 00:00:00
PB - Proceedings of the National Academy of Sciences (PNAS)
IS - 46
VL - 118
PMID - 34753821
SN - 0027-8424
SN - 1091-6490
ER -
BibTex
Cite this
BibTex Copy
@article{2021_Guan,
author = {Pin Wen Guan and R. J. Hemley and Venkatasubramanian Viswanathan},
title = {Combining pressure and electrochemistry to synthesize superhydrides},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
year = {2021},
volume = {118},
publisher = {Proceedings of the National Academy of Sciences (PNAS)},
month = {nov},
url = {https://doi.org/10.1073%2Fpnas.2110470118},
number = {46},
doi = {10.1073/pnas.2110470118}
}
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