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Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy

Lee, Daewon [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0009000038757963)·Oaks-Leaf, Sam [University of California, Berkeley, CA (United States)] (ORCID:0000000326180380)·Betzler, Sophia B. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Shi, Yifeng [Georgia Institute of Technology, Atlanta, GA (United States)]·Zhou, Siyu [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000159590541)·Ophus, Colin [Stanford University, CA (United States)]·Wang, Lin-Wang [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000170612692)·Asta, Mark [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)]·Xia, Younan [Georgia Institute of Technology, Atlanta, GA (United States); Emory University, Atlanta, GA (United States)] (ORCID:0000000324317048)·Limmer, David T. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)] (ORCID:0000000227660688)·Zheng, Haimei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000338134170)
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Abstract

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. By utilizing liquid-phase transmission electron microscopy (TEM), we study hydrogen (de)intercalation in palladium nanocrystals as a model system and have achieved unprecedented atomic-resolution imaging of hydrogen intercalation wave dynamics. 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. Systematic image analysis uncovers the atomic evolution of the hydrogen intercalation wave, transitioning from nonplanar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate that the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. In conclusion, unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.

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Lee, Daewon [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0009000038757963), Oaks-Leaf, Sam [University of California, Berkeley, CA (United States)] (ORCID:0000000326180380), Betzler, Sophia B. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Shi, Yifeng [Georgia Institute of Technology, Atlanta, GA (United States)], Zhou, Siyu [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000159590541), Ophus, Colin [Stanford University, CA (United States)], Wang, Lin-Wang [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000170612692), Asta, Mark [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Xia, Younan [Georgia Institute of Technology, Atlanta, GA (United States); Emory University, Atlanta, GA (United States)] (ORCID:0000000324317048), Limmer, David T. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)] (ORCID:0000000227660688), Zheng, Haimei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000338134170). 2026-06-22. Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy. https://doi.org/10.1021/jacs.6c03937

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