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Title: Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles

Abstract

Many energy storage materials undergo large volume changes during charging and discharging. The resulting stresses often lead to defect formation in the bulk, but less so in nanosized systems. Here, we capture in real time the mechanism of one such transformation—the hydrogenation of single-crystalline palladium nanocubes from 15 to 80 nm—to better understand the reason for this durability. First, using environmental scanning transmission electron microscopy, we monitor the hydrogen absorption process in real time with 3 nm resolution. Then, using dark-field imaging, we structurally examine the reaction intermediates with 1 nm resolution. The reaction proceeds through nucleation and growth of the new phase in corners of the nanocubes. As the hydrogenated phase propagates across the particles, portions of the lattice misorient by 1.5%, diminishing crystal quality. Once transformed, all the particles explored return to a pristine state. As a result, the nanoparticles’ ability to remove crystallographic imperfections renders them more durable than their bulk counterparts.

Authors:
 [1];  [1];  [2];  [1];  [1];  [3]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); DIFFER - Dutch Institute for Fundamental Energy Research, Eindhoven (The Netherlands)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1347444
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; materials chemistry; materials for energy and catalysis; nanoscale materials; transmission electron microscopy

Citation Formats

Narayan, Tarun C., Hayee, Fariah, Baldi, Andrea, Koh, Ai Leen, Sinclair, Robert, and Dionne, Jennifer A. Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles. United States: N. p., 2017. Web. doi:10.1038/ncomms14020.
Narayan, Tarun C., Hayee, Fariah, Baldi, Andrea, Koh, Ai Leen, Sinclair, Robert, & Dionne, Jennifer A. Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles. United States. doi:10.1038/ncomms14020.
Narayan, Tarun C., Hayee, Fariah, Baldi, Andrea, Koh, Ai Leen, Sinclair, Robert, and Dionne, Jennifer A. Mon . "Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles". United States. doi:10.1038/ncomms14020. https://www.osti.gov/servlets/purl/1347444.
@article{osti_1347444,
title = {Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles},
author = {Narayan, Tarun C. and Hayee, Fariah and Baldi, Andrea and Koh, Ai Leen and Sinclair, Robert and Dionne, Jennifer A.},
abstractNote = {Many energy storage materials undergo large volume changes during charging and discharging. The resulting stresses often lead to defect formation in the bulk, but less so in nanosized systems. Here, we capture in real time the mechanism of one such transformation—the hydrogenation of single-crystalline palladium nanocubes from 15 to 80 nm—to better understand the reason for this durability. First, using environmental scanning transmission electron microscopy, we monitor the hydrogen absorption process in real time with 3 nm resolution. Then, using dark-field imaging, we structurally examine the reaction intermediates with 1 nm resolution. The reaction proceeds through nucleation and growth of the new phase in corners of the nanocubes. As the hydrogenated phase propagates across the particles, portions of the lattice misorient by 1.5%, diminishing crystal quality. Once transformed, all the particles explored return to a pristine state. As a result, the nanoparticles’ ability to remove crystallographic imperfections renders them more durable than their bulk counterparts.},
doi = {10.1038/ncomms14020},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Mon Jan 16 00:00:00 EST 2017},
month = {Mon Jan 16 00:00:00 EST 2017}
}

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Cited by: 7 works
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