Kavli Affiliate: David T. Limmer
| First 5 Authors: Daewon Lee, Sam Oaks-Leaf, Sophia B. Betzler, Yifeng Shi, Siyu Zhou
| Summary:
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.
| Search Query: ArXiv Query: search_query=au:”David T. Limmer”&id_list=&start=0&max_results=3