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Title: Avalanching strain dynamics during the hydriding phase transformation in individual palladium nanoparticles

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms10092· OSTI ID:1339269
 [1];  [2];  [3];  [2];  [2];  [4];  [4];  [4];  [3];  [2];  [4]
  1. Univ. of California, San Diego, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Univ. of Melbourne (Australia)
  4. Univ. of California, San Diego, CA (United States)

Phase transitions in reactive environments are crucially important in energy and information storage, catalysis and sensors. Nanostructuring active particles can yield faster charging/discharging kinetics, increased lifespan and record catalytic activities. However, establishing the causal link between structure and function is challenging for nanoparticles, as ensemble measurements convolve intrinsic single-particle properties with sample diversity. Here we study the hydriding phase transformation in individual palladium nanocubes in situ using coherent X-ray diffractive imaging. The phase transformation dynamics, which involve the nucleation and propagation of a hydrogen-rich region, are dependent on absolute time (aging) and involve intermittent dynamics (avalanching). A hydrogen-rich surface layer dominates the crystal strain in the hydrogen-poor phase, while strain inversion occurs at the cube corners in the hydrogen-rich phase. A three-dimensional phase-field model is used to interpret the experimental results. Our experimental and theoretical approach provides a general framework for designing and optimizing phase transformations for single nanocrystals in reactive environments.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1339269
Alternate ID(s):
OSTI ID: 1253608; OSTI ID: 1352829
Journal Information:
Nature Communications, Vol. 6; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 73 works
Citation information provided by
Web of Science

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Grain boundary mediated hydriding phase transformations in individual polycrystalline metal nanoparticles journal October 2017
Identifying Defects with Guided Algorithms in Bragg Coherent Diffractive Imaging journal August 2017
An Analytical Bond Order Potential for Mg−H Systems journal January 2019
Thermodynamic stability of driven open systems and control of phase separation by electro-autocatalysis journal January 2017
Facets and vertices regulate hydrogen uptake and release in palladium nanocrystals journal March 2019
Rational strain engineering in delafossite oxides for highly efficient hydrogen evolution catalysis in acidic media journal December 2019
Real-time coherent diffraction inversion using deep generative networks journal November 2018
Atomic-scale selectivity of hydrogen for storage sites in Pd nanoparticles at atmospheric pressure journal January 2019
Thermodynamic Stability of Driven Open Systems and Control of Phase Separation by Electro-autocatalysis text January 2017
Realization of an H 2 /CO dual-gas sensor using CoPd magnetic structures journal October 2018
Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales journal August 2017
Enhancing Electrocatalytic Water Splitting by Strain Engineering journal February 2019
Real-time coherent diffraction inversion using deep generative networks text January 2018
The self-healing of defects induced by the hydriding phase transformation in palladium nanoparticles journal November 2017
Bragg coherent diffractive imaging of single-grain defect dynamics in polycrystalline films journal May 2017
In situ structural evolution of single particle model catalysts under ambient pressure reaction conditions journal January 2019
Active site localization of methane oxidation on Pt nanocrystals journal August 2018