Abstract
Grain boundaries separate crystallites in solids and influence material properties, as widely documented for bulk materials. In nanomaterials, however, investigations of grain boundaries are very challenging and just beginning. Here, we report the systematic mapping of the role of grain boundaries in the hydrogenation phase transformation in individual Pd nanoparticles. Employing multichannel single-particle plasmonic nanospectroscopy, we observe large variation in particle-specific hydride-formation pressure, which is absent in hydride decomposition. Transmission Kikuchi diffraction suggests direct correlation between length and type of grain boundaries and hydride-formation pressure. This correlation is consistent with tensile lattice strain induced by hydrogen localized near grain boundaries as the dominant factor controlling the phase transition during hydrogen absorption. In contrast, such correlation is absent for hydride decomposition, suggesting a different phase-transition pathway. In a wider context, our experimental setup represents a powerful platform to unravel microstructure–function correlations at the individual-nanoparticle level.
Highlights
Grain boundaries separate crystallites in solids and influence material properties, as widely documented for bulk materials
Grain boundaries are expected to be of significant importance due to the relative abundance of grain boundary sites compared to bulk materials with larger grains[16, 23,24,25,26,27]
We employ a multichannel variant of plasmonic nanospectroscopy[20], which enables measurements of the individual response from up to 10 nanoparticles simultaneously, during both hydrogen absorption and desorption, and combine it with transmission electron microscopy (TEM) and transmission Kikuchi diffraction (TKD)[28]
Summary
Grain boundaries separate crystallites in solids and influence material properties, as widely documented for bulk materials. 12 and 13) of optical single particle p-C isotherms from data sets 1 and 2, together with corresponding TEM images and TKD grain orientation maps.
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