Atomic evolution of hydrogen intercalation wave dynamics in palladium nanocrystals

Fuente: arXiv
Saved in:
Bibliographic Details
Main Authors: Lee, Daewon, Oaks-Leaf, Sam, Betzler, Sophia B., Shi, Yifeng, Zhou, Siyu, Ophus, Colin, Wang, Lin-Wang, Asta, Mark, Xia, Younan, Limmer, David T., Zheng, Haimei
Format: Preprint
Published: 2024
Subjects:
Online Access:
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1866915021143932928
author Lee, Daewon
Oaks-Leaf, Sam
Betzler, Sophia B.
Shi, Yifeng
Zhou, Siyu
Ophus, Colin
Wang, Lin-Wang
Asta, Mark
Xia, Younan
Limmer, David T.
Zheng, Haimei
author_facet Lee, Daewon
Oaks-Leaf, Sam
Betzler, Sophia B.
Shi, Yifeng
Zhou, Siyu
Ophus, Colin
Wang, Lin-Wang
Asta, Mark
Xia, Younan
Limmer, David T.
Zheng, Haimei
contents Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. We study hydrogen (de)intercalation in palladium nanocrystals as a model system and achieve atomic-resolution imaging of hydrogen intercalation wave dynamics by utilizing liquid-phase transmission electron microscopy. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ~60 nm down to ~10 nm. We uncover the atomic evolution of hydrogen intercalation wave transitioning from non-planar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. Unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.
format Preprint
id arxiv_https___arxiv_org_abs_2404_02416
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Atomic evolution of hydrogen intercalation wave dynamics in palladium nanocrystals
Lee, Daewon
Oaks-Leaf, Sam
Betzler, Sophia B.
Shi, Yifeng
Zhou, Siyu
Ophus, Colin
Wang, Lin-Wang
Asta, Mark
Xia, Younan
Limmer, David T.
Zheng, Haimei
Statistical Mechanics
Materials Science
Chemical Physics
Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. We study hydrogen (de)intercalation in palladium nanocrystals as a model system and achieve atomic-resolution imaging of hydrogen intercalation wave dynamics by utilizing liquid-phase transmission electron microscopy. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ~60 nm down to ~10 nm. We uncover the atomic evolution of hydrogen intercalation wave transitioning from non-planar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. Unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.
title Atomic evolution of hydrogen intercalation wave dynamics in palladium nanocrystals
topic Statistical Mechanics
Materials Science
Chemical Physics
url https://arxiv.org/abs/2404.02416