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Uncovering the intrinsic size dependence of hydriding phase transformations in nanocrystals
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Uncovering the intrinsic size dependence of hydriding phase transformations in nanocrystals
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Journal Article
Uncovering the intrinsic size dependence of hydriding phase transformations in nanocrystals
2013
Overview
A quantitative understanding of nanocrystal phase transformations would enable more efficient energy conversion and catalysis, but has been hindered by difficulties in directly monitoring well-characterized nanoscale systems in reactive environments. We present a new
in situ
luminescence-based probe enabling direct quantification of nanocrystal phase transformations, applied here to the hydriding transformation of palladium nanocrystals. Our approach reveals the intrinsic kinetics and thermodynamics of nanocrystal phase transformations, eliminating complications of substrate strain, ligand effects and external signal transducers. Clear size-dependent trends emerge in nanocrystals long accepted to be bulk-like in behaviour. Statistical mechanical simulations show these trends to be a consequence of nanoconfinement of a thermally driven, first-order phase transition: near the phase boundary, critical nuclei of the new phase are comparable in size to the nanocrystal itself. Transformation rates are then unavoidably governed by nanocrystal dimensions. Our results provide a general framework for understanding how nanoconfinement fundamentally impacts broad classes of thermally driven solid-state phase transformations relevant to hydrogen storage, catalysis, batteries and fuel cells.
Although quantitative understanding of nanocrystal phase transformations is important for efficient energy conversion and catalysis, difficulties in directly monitoring nanoscale systems in reactive environments remain. Direct quantification of hydriding transformations in palladium nanocrystals now clearly reveals that the transformation rates are governed by nanocrystal dimensions.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
